137
Magnetic Moment and Hyperfine Field Studies Using Gamma-Gamma Perturbed Angular Correlation DHARMENDRA KUMAR GUPTA M. Sc. (Aligarb) Thesis Submitted to the Aligarh Muslim University^ AHgarh in Partial Fulfilment For the Award ef Ph. D. Degree in PHYSICS 1972

Magnetic Moment and Hyperfine Field Studies Using … · making alloys from Metallurgy Department is also gratefully acknowledged. I am deeply indebted to Professor Rais Ahmed whose

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Magnetic Moment and Hyperfine Field Studies Using

Gamma-Gamma Perturbed Angular Correlation

DHARMENDRA KUMAR GUPTA M. Sc. (Aligarb)

Thesis Submitted to the Aligarh Muslim University^

AHgarh in Partial Fulfilment For the Award ef

Ph. D. Degree in

PHYSICS

1972

T1258

' ' DEC 1373

1 1

Cert i f ied that the work presented in t h i s

t h e s i s i s the or ig inal work and has heen ca r r i ed

out by me <,

i^l/vG4t Dharmendra Kumar Gupta

Research Officer Department of Physics

A.M.Uo, Aligarh

Ill

ACOOWLEDGE^EHTS

The work presented in this thesis was carried out at

the Central Nuclear Laboratories of the Indian Institute of

Technology, Kanpur (India) under the able guidance of

Dr. G« No Rao, Assistant Professor. I am deeply indebted

to him for introducing me to this field, for taking keen

interest in my work, for his valuable guidance and for

placing all facilities at my disposalo

I wish to thank Professor J.J. Huntzicker, Dr. T.M.

Srinivasan, Dr. G.K. Mehta, Dr. S. Mukerjee and group

co-workers, Dr. B.V.N. Rao, Dr.D.N. Sanwal, Dr. K.B. Lai,

Mr. A.K. Singhvi, Mr. C. Rangacharyulu and Mr. R. Singh for

the useful discussions and assistance during the completion

of this work. I am also grateful to Messrs B.K. Jain and

G.P. Mishra for technical help throughout this v/ork. The

help in computer programming from Mr. A.K. Chopra and in

making alloys from Metallurgy Department is also gratefully

acknowledged.

I am deeply indebted to Professor Rais Ahmed whose

encouragement and guidance have throughout been a source

of inspiration to me. I take this opportunity to thank

various of my well wishers and colleagues particularly

Dr. S. Pazal Mohammed, Dr. M.L. Sehgal and Dr. K. Rama Reddy

who helped me in the preparat ion of t h i s t h e s i s . I am also

thankful to my teachers namely Professor Mohdo Zi l lu r Rahman

Khan and Prof« D.G. Sarkar for t h e i r kind help and encouragement,

I g ra te fu l ly acknowledge the f inanc ia l as,'jist.ance from

N.B.S. Washington, D.C. (USA) under PL-480 Scheme ( H B S ( G ) 1 2 7 ) .

I also thank the o f f i c i a l s of I IT, Kanpur for providing me

the r e s i d e n t i a l f a c i l i t i e s and the a u t h o r i t i e s of t h i s

Univers i ty for grant ing me leave for the period I v/as in

I . I . T „ , Kanpur.

F ina l ly , I thank to Kr N. Ahmad for exce l len t typing

of the manuscript.

(DoK. Gupta)

V

LIST OE GONTSI TTS

Page

List of Tables vii

List of Figures viii

Abstract xii

I. INTRODUCTION 1

lie NUCLEAR STRUCTURE STUDIES - EXPERIMENTAL RESULTS 5

A. Study of the Time Resolution of the Delayed Coincidence Spectrometer Using Different Nuclear Radiation Detectors 5

l- Time resolution of Ge(Li) detector ' 6

2. Time resolution of scintillation detectors 7

Bo Lifetime Measurements 8

C« The Decay Scheme of ^^Rh 27

III. MAGNETIC MOMENT MEASUREMENTS 38

Ao Magnetic Mom.ent of 206-keV State in ^ ' Re 40

1. Source preparation 40

2. Experimental set-up 40

3. Deca.y scheme and gamma-rays 41

4.. Magnetic moment measurem-ent of 206~keV

level in - - 'Re 41

B. Magnetic Moment of 68-keV state in ^Sc 43

1c Source preparation 43 2. Decay scheme and gamma-rays 43 3= Magnetic moment measurement of 68-keV

l eve l in ^^Sc 43 Co Results and Discussion 45

VI

IV. HYPERFINE PIEID MEASUREBffiNTS _ 50

A. Origin of the Hyperfine Fields, Hyperfine Field Models and Systematics of the Hyperfine Fields 50

Bo The Hyperfine Field Measurements at 'Re Nuclei in Nickel Lattice at Room Temperature 63

1. Source preparation 63

2. Experimental set-up 63

3c Experimental results and analysis of the data 64

44 Ce The Hyperfine Field at Sc Nuclei in Iron lattice at Room Temperature 65

1. Source preparat ion 65 2. Experimental arrangement 65 3c Experimental results and analysis of

the data 66

D. Results and Discussion 68

REFERENCES 77

PUBLICATIONS 83

V l l

Table

LIST OP TABLES

1 Comparison of the present l i a l f - l i i e measurements v/ith ava i lab le published valueso

2 Comparison of the experimental t r a n s i t i o n p r o b a b i l i t i e s and matrix elements ¥ith""slngle p a r t i c l e estim,ates and theore t i ca l matrix elements due to Arima et a l .

99 3 Gamma-rays observed in the decay of 16.1 d Rli

and t h e i r r e l a t i v e i n t e n s i t i e s . 4 Summary of the Ge(Li)-Ge(Li) f a s t - s low-eo inc i -

dence measurements.

5 Summary of the Nal(Tl)-NaI(Tl) sum-coincidence measurements.

5 Comparison of the present magnetic moment measurements with avai lable published va lues .

7 Comparison of the present hyperfine f i e ld

measurements with ava i lab le published va lues .

V l l l

LIST OF FIGURES

Figure

1 Slock diagram of delaj 'ed coincidence spectrometer.

2 MCA channel calibration and TPHC linearity.

22

3 Prompt time spectrum of Na t;ource wi th g a t i n g s

around 72-keV and 480-keV. A l ead loaded p l a s t i c

s c i n t i l l a t o r f o r t h e 72-keV and a Nal (Tl ) c r y s t a l

fo r t h e 480-keV are used . —

4 Li fe t ime spectrum of 68-ke? s t a t e i n Sc.

75 5 L i f e t ime spectrum of 280-keV s t a t e i n As (hollow

22 do t s ) along v/ith prompt time spectrum of Na ( s o l i d do ts ) under the same energy gate s e t t i n g s .

99 6 L i fe t ime spectrum of 89-keV s t a t e i n Ru.

170 7 Li fe t ime spectrum of 84-keV s t a t e i n Yh.

1 Pii 8 Lifetime spectrum of 206-keV state in Re.

ITL 9 L i fe t ime spectrum of 124-keV s t a t e i n CSc

131 10 Lifetime spectrum of 134-ke'V state in Cs.

11 Lifetime spectrum of 81-keV state in -' •Cs.

197 12 Lifetime spectrum of 77-keV state in Au

(hollow dots) along with prompt time spectrum

22 of Na (solid dots) under the same energy gate

settings.

IX

Figure

13 Gamma-ray s i n g l e s spectrum of Kb. i n the .-:;nergy

reg ion 0-443 keV obta ined wi th a Ge(Li) d e t e c t o r

( l i v e t i m e 60 min) .

go

14 Gamma-ray s i n g l e s spectrum of Rh i n the energy

reg ion 443-1208 ke? with a Ge(Iii) d e t e c t o r

( l i v e t i m e 600 min) .

99

15 Gamma-ray s i n g l e s spectrum of Rh in~ttre energy

r eg ion 1208-1749 keV ob ta ined wi th a Ge(Li)

d e t e c t o r ( l i v e t i m e 1200 min ) .

99 16 Gamma-ray s i n g l e s spectrum of Pli i n t h e energy

r eg ion 1749-2059 keV ob ta ined wi th a &e(Li)

d e t e c t o r ( l i v e t i m e 1800 min) .

17 Block diagram of Ge(Li)-Ge(Li) sl 'ow-fast co inc idence

spec t rome te r .

18 The spectrum of y-^^ays in the r eg ion 0-511 keV

c o i n c i d e n t with the 322-ke7 y-vs^J' r ecorded wi th

a Ge( I i ) -Ge(L i ) f a s t - s l o w assembly^

19 The spectrum of y~rajs i n the region 0-941 keV

c o i n c i d e n t with the 353-keV y-raj r ecorded wi th

a Ge(Li)-Ge(Li) f a s t - s l o w assembly. 99

20 Level scheme of Ru. Dashed l i n e s shown a r e new t r a n s i t i o n s .

X

Figure

21 Arrangement of magnet and detectors.

22 Decay scheme of " 'W (24h) -^ " ' Re.

23 Time differential perturbed angular correlation

spectra of Re in an external magnetic field

of 7 KOeo

24 R(t) vs time t plotted for the TDPAC spectra of 1 R7

Re i n an e x t e r n a l magnetic f i e l d of 7 KOe.

25 The F o u r i e r t r ans fo rms of R( t ) for Re i n an

e x t e r n a l magnetic f i e l d of 7 KOe.

26 Decay scheme of ''"' Ti i^'^^k) —?• "^"^Sc.

27 Time d i f f e r e n t i a l p e r t u r b e d angu la r c o r r e l a t i o n

spectrum of Sc i n an e x t e r n a l magnet ic f i e l d

of 7 KOe.

28 R( t ) vs time t p l o t t e d for t h e TDPAC s p e c t r a of

44 Sc in an external magnetic field of 7 KOe.

29 The Fourier transforms of R(t) for Sc in an

internal magnetic field of 7 KOe.

30 Magnetic hyperfine fields at solute nuclei in

iron matrix plotted vs the atomic number Z of

the solute atom. Open circles indicate that

the sign of the field has not been directly

measured.

X I

Figure

31 Magnetic hyperfine f i e l d s a t solute nuc le i in

cobalt matrix p lo t ted vs the atomic number Z

of the solute atom. Open c i r c l e s indicate tha t

the s ign of the f ie ld has not been d i r e c t l y

measured.

32 Magnetic hyperfine f i e lds a t solute nucle i in

nickel matrix p lo t ted vs the atomic number Z

of the solute atom. Open c i r c l e s ind ica te t h a t

the sign of the f i e ld has not been d i r e c t l y

measured.

33 Calculated po la r iza t ion P. of the S-electrons

a t the impurity s i t e as a funct ion of the

valence Z. of the impurity atom. Curve ' a '

represents the estimate of Daniel and F r i e d e l ;

Carve ' b ' represents the estimate of Campbell.

j?cr i r on P, = 1, h

34 R(t) vs time t for the TDPAC spectra of • ' HeNi

in an external polarizing magnetic field of 2 KOe.

1 on 35 'fhe Fourier transforms of R(t) for ReNi in an

external polarizing magnetic field of 2 KOe.

36 R(t) vs time t for the TDPAC spectra of ^^ScPe

in an external polarizing magnetic field of 3 KOe,

37 'Ihe Fourier traiisforms of R(t) for ScFe in an

external polarising magnetic field of 3 KOe.

Xll

MAGNETIC MOMENT AND HYPERPINE FIELD STUDIES USII G

GAMMA-GAMMiii PERTURBED ANGULAR GORPJCLATION

ABSTRACT

Using time differential pertur'bed angular correlation

technique (TDPAC), the hyperfine fields on Sc in Pe_ and on

Re in Ni_ are measured. The hyperfine field on ScFe is

reported for the first time. Using th-e-same method^ the

44 magnetic moment of the 68-keV state in Sc and of the

1 Rl 206~keV state in Re are also measured^

Detailed studies on the time resolution of Ge(Li)

detectors and scintillation detectors were carried out.

44 75 99 I'l 1'5' The nuclear lifetimes in ^^Sc, '^Se, ^Ru, " Cs, " Cs,

1 70 1 Pil 1 Q7 Yb, Re and Au are also measured using the delayed

coincidence techniques. A new value for the lifetime in

131

Cs is reported. In most of the other cases the errors

in our measurements are considerably less compared to the

earlier reported values. The nuclear lifetime measurements 151 133 197

in Cs, Cs and Au fall under the category of l-forbidden transitions. The experimental Ml, E2 transition probabilities

obtained from the present measurements in the 1-forbidden

131 133 197 transitions in Cs, Cs and Au are compared with the

predictions of Arima et al. Por the remaining cases, the

experimental values are compared with the single particle

estimates.

Xlll

The detailed decay scheme studies in the de-excitation

99 of Ru are also reported. These studies are carried out

using Ge(Li) detectors, G-e(Li) detectors in coincidence,

Nal(Tl) detectors etc. The genetic relationships are estab­

lished from accurate intensity measurements and coincidence

studies. One nev/ gamma ray and four-n«4v cascade transitions

are establishedc

The existing hyperfine field models are discussed in

brief. The systematics of the variation of the dilute impu­

rity hyperfine fields in the host matrices of Fe, Ni, C£ are

studied. All the reported dilute hyperfine field values are

plotted against the atomic number of the solute for each

of the Pe, Ni, £0 matrices and some new trends are pointed

out, e.g.

(i) The hyperfine field H, „ is negative in 3d, 4d and 5d

impurities in all the three hosts F_e, _G£, Ni except in the

4d series for ^^Fe, ^^ZrFe and " ZrOo.

(ii) In iron host, the field increases gradually for Ru, Rh

and Pd and the maximum value is obtained for Pd. However,

the reverse trend is clearly seen for the same impurity

metals for the other host matrices of _C£ ind Ni.

(iii) In 5d impurities, the maximum value of hyperfine

field is obtained at Ir for all the three matrices.

(iv) In the case of 5p impurities, the field starts with

a small negative value and gradually increases to a maximum

XIV

value for I and falls off to zero.

(v) In 4f series the fields are negative for low 4f values

and then it changes from negative to a large positive value

and again from positive value to a large negative value.

The hyperiine fields for ScFe_, B.eNi are compared with

the models suggested by Shirley et al.; Camphell; Balahanov

et al.; and Stearns. It is found that none of these models

can successfully explain the measuradr-f4.elds in ScPe and

ReNi. The observed field in Se?e both in magnitude and

sign may be qualitatively explained by the conduction

electron polarization (GEP) and the core polarization (GP)

models suggested by Shirley. The field on Re in Ni may be

understood if we assume that conduction electron polariza­

tion and the overlap polarization (OP) are vectorially added

to give the final experimental value. The experimental

magnetic moments are compared with the prediction of the

existing nuclear models. The magnetic moment value of

206-keV level in Re is in fair agreement with the

theoretical value obtained from the modified Nilsson's

model proposed by De Boer et al. Attempts are made to

explain the experimentally measured magnetic moment for

68-keV state in Sc assuming the configurations for a

1 "^ proton and neutron groups as ( 7/0)7/0 ^^ • 7/? 7/?

respectively. But the value for magnetic, moment thus

XV

obtained is found larger by a factor->• 1.4 compared with

the experimental value. Therefore, the absence of any

definite knowledge of the configuration of 68-keV state

44 m Sc is the hind: ronce in interpreting the magnetic

moment of this state.

CHAPTER I

INTRODUCTION

Since the discovery of Samoilov et al. in 1959 that

diamagnetic gold nuclei dissolved in ferromagnetic iron experience

a large magnetic hyperfine field ('•>l MOe), the range and usefulness

of application of hyperfine fields has increased considerably. The

large magnetic fields seen by the impurity nuclei can be favourably

exploited to measure the magnetic dipole moments of the short

lived nuclear excited states of the impurity nuclei. The hyperfine

field measurements are also useful as sensitive probes for the

understanding of the Core and Conduction electron wave functions.

A formal solution of the problem of the impurities in

ferromagnetic hosts is quite complex and would involve the solu­

tion of a many body problem. However, the systematic variations

of the signs and magnitudes of the hyperfine fields as a function

of the electronic configurations of the impurity atoms (in

particular as a function of the atomic number Z) has provided us

the insight to understand the major mechanisms responsible for

the origin of these hyperfine fields. The large experimental

data currently available with literature enabled many workers

to suggest many models for the hyperfine fields. Because of

this reason, there has been considerable interest to measure

the magnetic hyperfine fields on magnetic and nonmagnetic

2)

impurities in ferromagnetic and paramagnetic hosts. As pointed

by Jaccarino, Walker and Wertheim (see page 51), the experimental

data with temperature variation of the hyperfine field on the

impurity can be used to detect the possibility of a localized

moment around the impurity., It has been our interest to measure

the hyperfine fields on dilute diamagnetic impurities in ferro­

magnetic hosts to have a better understanding of the mechanisms

involvedo

Many experimental techniques in principle can be used for

the hyperfine field measurements. These techniques may-iroadly

be divided into two categoriess a) stable nuclei are used (nuclear

magnetic resonance (NMR), electron spin resonance, nuclear

specific heats etc.), and b) radioactive nuclei are used~(pertur-

bed angular correlation, nuclear orientation, Mossbauer effect,

nuclear magnetic resonance/nuclear orientation ( M R / N O ) ) . In

this thesis, v/e have used the time differential perturbed angular

correlation techniques (TDPAC) for the hyperfine field measurements.

Normally WIR techniques give results of highest accuracy.

However, the recent improvements in the TDPAC techniques like the

Fourier transform of the auto-correlation function has made it

competetive with NMR accuracy. In addition, the TDPAC technique

has certain advantages when compared to the NMR in terms of its

higher sensitivity and wider applicability in terms of temperature

etc. The higher sensitivity of the PAC technique will be parti­

cularly helpful for the measurement of the dilute impurity

hyperfine fields because the impurity-impurity interactions

are negligible.

In the PAG technique of measuring the hyperfine fields

one observes the change in the angular correlation pattern of the

3

nuclear radiation when the intermediate state having a magnetic

dipole moment is perturbed "by the internal hyper fine fields o In

the ahsence of any external perturbations, the angular correla­

tion of the y-^ays could he expressed as a sum of a series of

legendre polynomials " <, V/hen the intermediate state is perturbed

by magnetic field, classically speaking, the dipole moment

processes around the applied field with Larmor frequency. The

larmor frequency and hence the internal hyperfine field could be

obtained from the observed change in the (y-y) angular correla­

tion pattern, if we know the magnetic dipole moment of the

nuclear state involved.

For the cases measured in this thesis, cubic hosts were

chosen so that the quadrupole effects are sm.all. In addition,

the impurities form solid solutions with the corresponding hosts.

All the experimental data available in the literature for the

impurity hyperfine fields have been plotted as a function of

the impurity atomic number for the host matrices of Fe_, _C£» Ni.

Similar plots for Fe host are already available in the literature

(see Chapter lY), From the studies of these systematics, we are

able to draw some nev/ trends which were not pointed out until

now such asi (i) The hyperfine field H, is negative in 3d, 4d

and 5d impurities in all the three hosts Fe, C_o, Ni except in

the 4d series for '- YFe, ' ZrFe and ZrCo. (ii) In iron host,

the field increases gradually for Ru, Rh and Pd and the maximum

value is obtained for Pd. Hov/ever, the reverse trend is clearly

seen for the same impurity metals for the other host matrices

of Oo and Ni„

The magnetic moments of some of the nuclear states are

also measured using the TDPAC technique., These values are

compared with the existing nuclear models.(see Chapter III).

99 The nuclear level structure of Ru is studied using

Ge(Li) detectors J Nal(Tl) sum-coincidence spectrometers and

G-e(Li) detectors in coincidence. These studies resulted in

99 an improved level schemxe of Ru„ The short nuclear lifetime

measurements in ^^Sc, ' Se, ^Ru, '^^^Cs, ^^^Cs, " Yh, " Re

197 and Au were also carried out. One new value for the 134--

keV state in Cs is reported. In other cases the existing

errors in the m.easurements are reduced. The experimental Ml,

E2 transition probabilities obtained from, the present measure­

ments in the 1-forbidden transitions are compared with the

predictions of Arima et al. Por the remaining cases;, tke

experimental values are compared with the single particle

estimates (see Chapter II). Detailed studies on the time

resolution of Ge(Li) detectors and scintillation detectors

were carried out.

CllPTSR II

NUGLBAR STRUCTURE STUDIES - EXPERIMENTAL RESULTS

Ao STUDY OE THE TIMS RESOLUTION OF THE DELAYED COINGIDENCE

SPECTROMETER USING DIFEER3NT NUCLEAR RADIATION DETECTORS

The time resolution of the spectrometer plays an

imp'ortaiit role in the measurements of lifetime, magnetic

moment and hyperfine fields. The "block diagram of the

electronics is shown in Eig. 1. Depending upon the parti­

cular case under investigation the comMnation of the

detectors among Nal(Tl), lead loaded plastic scintillator,

plastic scintillator and Ge(Li) detector is chosen. All

the scintillators used in the present experiments are

coupled with 56 AVP photomultiplier tubes. The fast pulses

from the detectors are amplified (particularly low energy

radiations) using EGi G 1 nsec DC amplifiers and then fed

into Past discriminators ORTEG model 417" The outputs are

fed into model 437A ORTEG time-to-pulse height converter

(TPHC). The TPHC is calibrated by recording prompt ^°Co

spectra and by observing the channel corresponding to the

centroid of this prompt spectrum for various values of

delay introduced in the 'stop' arm. This delay is varied

in the interested range by using the ORTEG model 425 delay

box (nsec region) or ORTEG model 42? delay amplifier (jisec

region). These delay sources are in turn calibrated with

standard techniques say for example using standard lengths

of 50i" (RG58A/U) cable which has delay of 5.06- nsec per meter.

5

o

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The introduction of delay gives rise to a shift of the

centroid of the prompt time spectrum^ It is found that a

plot of delay versus the centroid position (channel number)

was a straight line (shown in 'Fig,2) thus confirming the

linearity of the TPHC. A least squares fit to this straight

line (given in Fig. 2) gave the slope, or the calibration

of the spectrometer^ It was found that the linearity of

the system is better than O.lX-

1. Time resolution of Gre(Li) Detector

In the study of the time resolution of electronic

system, one 5.1 cm x 5.1 cm plastic scintillator coupled

with 56 AVP photomultiplier tube in start channel and a

Ge(Li) detector of 7 mm depletion depth and 6 sqcm effec­

tive area in the stop channel are used. A bias voltage of

+900 V is applied to Ge(Li) detector while -2000 V to the

P..M. tube. Here in place of fast discriminators Constant

Fraction Timing Discriminators ORTEC model 453 are used in

fast channels. In the Ge(Li), using veiy narrow window,

a wide range of energy is scanned and 'corresponding time

spectra are recorded. The FWHM is found to be varying from

2.9 nsec to 3.7 nsec and slope from 0,4 nsec to 2.8 nsec in

4) the energy range from 32-keV to 1830-keV '. This response

5-7) i s compared with the exis t ing l i t e r a t u r e ' for 100-keV

to 1330-keV region and found in good agreement. This study

gives the information about the l i m i t s of the system and i t

20 30 40 Delay in nsac

50

Fxa.2 MCA CiiANNiiL C.\L iBR Al'lON AND TPHC LiNEAiilTY /"usee RliGIONJ.

u c

a

Q

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I

0 <

0 01

0 0

0 GO

0 CD

0 ^

0 CM

jaqujnN puuDMO

7

is helpful in selecting the cases of magnetic moment and

hyperflne fields.

2. Time resolution of the scintillation detectors

Similar studies are made using 5.1 cm x 5.1 cm

Nal(Tl) scintillators in both the channels i.e. start and

stop respectively» Best timing conditions are achieved

when -1900 V is applied to the photomultiplier tube in

start channel and -2000 V to the photomultiplier tube in

stop channel. For carrying out the measurements on the

g

44

44 g - factor of 68-keV state in Sc and hyperfine field at

So nuclei in iron lattice, the time resolution of the

electronic system gating 78-keV gamma rays in start channel

and 68-keV gamma rays in stop channel is determined. The

values obtained for the FWHM and slope of the prompt spec-

22 trum using Na radioactive source are 15.0 nsec and 2.0

nsec respectivelyo In the g-factor measurement of 206-keV

1 87 state in Re, 480-keV gamma rays are gated in start channel

and 72-keV gamma rays in stop channel. Under these energy

gate settings the FWHM and slope of the prompt spectrum are

found to be 4.8 nsec and 0.5 nsec respectively. While in

1 87

the hyperfine field measurement at Re nuclei in nickel

matrix the Nal(Tl) is replaced by a 5.1 cm x 5.1 cm lead

loaded plastic scintillator for the detection of 72-keV

gamma rays in stop channel. Under these energy gatings

the FWHM and slope of the prompt spectrum are found to be

1.3 nsec and 0.24 nsec respectively. A sample of the prompt

time spectrum is shown in Pig. 3.

B. THE LIFETIME MEASUREMENTS^"^^^

Several half-lives of the excited states in various

44 99 nuclei are measured. All the sources except Ti and Rh

in the present measurements have been purchased from the

Atomic Energy Commission, Bombay (India). The dimension

of the sources used is taken very small so as to have

better true to chance ratio. The detectors are kept at

2% geometry and the source is at the centre of the detec­

tors. The final values of the lifetime reported in this

work are the statistical average of many runsc The least

squares fit of the coincidence data is done with the help

of an IBM 7044 computer.

(i) The half-life of the 68-keV state in ^^Sc : The 48.2 Y

44 activity of Ti decays through electron capture to the

excited levels in " Sc. The measurement of the half-life

is accomplished by observing the delayed coincidences

between 78- and 68-keV gamm.a rays. Since these gamma rays

cannot be resolved in Nal(Tl) detectors, the combined peak

is gated in both start and stop channels. Therefore, the

slope is obtained on both the arms of the time spectra.

The recorded time spectrum is shown in Pig. 4. The final

computed value of many runs for the half-life of the 68-keY

state is 155.5 + 2.0 nsec.

3x10'

c D O U

u c •o u c o u

10

FWHM = 1.3 nsec.

Slope /5i/2=0.2A

-

n sec. ^

10

20 Ch.No.

30 J

0 5 10 Time in n sec.(Arbitrary Zero)

F I G . 3 PROMPT TIME SPECTOUM OF ^^Na SaiRCE WITH GATINGS

ARCVND 7 2 - k e V AND URO-keV. A LEAD LOADED PI A3TIC

SCINTILLATOR FOR THE 7 2 - k e V AND A N a l ( T l ) CRYSTAL

FOR THE i^fiO-keV ARE USED.

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•i • t

• • •• • • .•

•• o CM

O o o CN

O o eg

o . o

CD t —

o _ o

<

o r O

(Nl

O

o *"

o - o

. CD

o - o

- U3

O - O

- <r

o - O ~ CNl

O L-

(i»

N

d •*-'

3 *

o

< J--

u U1

c

c

Ci)

E h-

H

<

•Ji

> 0

1

Cl:.,

c «p

i o y

t?? - j )

% H H y ( b ,—t

•-, r " .

- I -

I I I ' ' ' L

o o en

SINHOD BDNBQIONIOD

o

Our measured half-life value agrees very well with

the earlier measurements of Bergstrom et al. ' (153+1)

12) nsec, and Ristenen et al, ' (153+2) nsec and disagrees

13)

with the measurements of Kliver et al. ' (166+5) nsec

and Bandi et al. ' (192+40) nsec. Ristenen and Sunyar

concluded from their angular correlation data that 68-keV

transition is a mixture of Ml and E2. They also confirmed

that 68-keV level has spin, parity as 1+. The measured

half-life is employed to calculate the experimental transi­

tion prohabilities T (Ml)^^^ and 'T (E2) ^ from the following exp exp

relations, ^ (-)e.p - f r H ^ ^ exp - Ti (1 + a ^ -J (1 ^2)

2.

exp = T T T F T T ^ ^ (1 ^ 52) T (E2)_ = . ^ I'T' ^ X — ^ (2-1)

The values of branching ratio (R), mixing ratio (6 ) and

total internal conversion coefficient (a, ,) are taken from tot

"IP "I 7^

the existing literature ' , and thus on substituting the p

values of R, 6 and a, , in eqn. (2-1), the experimental transition probabilities obtained are,

T (E2) ^ 2,5 X 10^ soc~^ 'exp

T (Ml) - 2.0 X lo' sec"-"-^ 'exp

16) and the theoretical single particle estimates ' are

T (Ml)g . 7.7 X 10- ^ sec""

T (E2) - 4.0 X 10^ sec"- ^ ^sp

10

On comparison we find that the Ml part of the 68-keV gamma

-4 transition is retarded by a factor of .v4 x 10 and the E2

is enhanced hy a factor of--16 relative to the single parti­

cle estimates. It is in agreement with the earlier measure-

12) ments ' .

(ii) The half-life of the 280-keV state in '''As : The

75 half-life of the 280-keV state in '- As is determined by

75

using a Se (120d) source. The measurement of the half-

life is accomplished by observing the delayed coincidences

between 121-keV and 280-keV gamma rays. Here a lead loaded

plastic scintillator is used in stop channel for the detec­

tion of 280-keV gamma ray. Since the slope of the prompt

time spectrum under the same energy gate settings is of

the same order as the lifetime under study, the lifetime

of the excited state is determined by the centroid shift

method a,nd it is found to be Ti_ = 0.277 + 0.031 nsec. The

lifetime and prompt time spectra are given in Pig. 5.

The 280-keV transition has been identified as mixture

of electric quadrupole (E2) and magnetic-dipole (Ml) '.

The experimentally observed half-life is employed to calculate

the transition probabilities T (Ml) and T (E2) from the

eqn. (2-1),

The values of branching ratic (R) and mixing ratio p 2.5)

(6 ) are taken from the published literature ' obtained

with Coulomb excitation technique. The experimentally

in ••-•

c D o u u c C9

u C o (J

0 5 10 T ime i n n s e c (Arbitrary 2ero)

F I G . 5 LIFETIME SPECTRUM OF 2 8 0 - k o V STATE IN ^^Aa (HOLLOW 22

DOTS) A3.0NG WITH PROMPT TLME SPECTRUM OF Na {SOL.ID

DOTS) UNDER THE SAME .ENERGY GATE SETTINGS.

11

measured value of total internal conversion coefficient

(a, , ) by G-rigorev et al. ' is used to obtain the

experimental transition probabilities,

T (Ml) •-• 2 X 10^ sec"- ^ ' exp

T (E2) ^ 4 X 10^ sec"^ ^ 'exp '^

Theoretical single particle transition probabilities are

17) estimated from the known relations ' using statistical

factor as unity.

T (Ml) - 6.6 X 10 - sec"- ^ ^ sp

T (E2) . 4.9 X lo' sec""'-^ ' sp

On comparison one finds that E2 transitions are enhanced

by a factor--'8 and Ml transitions are retarded by a

-3 factor'-'3 x 10 as compared to the single particle estimates. Our results are in agreement with the earlier

, 18) workers '.

( i i i ) The h a l f - l i f e of the 89-keV in ^^Ru : The half-

l i f e of 89-keV" level in - - Ru i s measured by the delayed 99 coincidence method using Rh (16.1 d) source. One lead

loaded p l a s t i c s c i n t i l l a t o r (5 .1 cm x 5.1 cm) i s used in

the stop channel to accept 89-keV gamma rays and Nal(Tl)

c rys ta l of (5.1 cm x 5.1 cm) in the s t a r t channel to

accept gamma rays from 320-520 keV. The l i f e t ime spectrum

i s shown in Fig. 6. The f ina l computed value of many runs

for the h a l f - l i f e (T^) i s 20.5 + 0.1 nsec. 2 ~"

T—nr

rO CVJ

CO

m

T — I I I o O if) c

o in d CVJ

CT> CO

FT—I I U»L

• • • • • •

. • • • •

ro in ro

in

cc 0^

• •

CM

O 0 ^

O

O in

o ro

o O

o

o 1^

o in

o ro

U l U—J—I L I • ' » > • I 1 I I I ' • *' *

o 5r

o

o o

o GO

o VD

O sr

o k .

c N

>>

n • 4 -

<

u (^

r. N E

H-

r^

0 .

ic K

<t

C/5

> W !

CN

oc-& H

o

H O '-4 P4 f,0

W

r-r.

o CM

o ro Cvi

J- O

H

VO

S

s^unoo 3Duappu|03

12

The 89-keV gamma ray is a mixture of Ml and E2

19) multipolarities. Kistner ' from his Mossbauer studies

2

reported that the mixing ratio 5 =2.7+0.6. The

total internal conversion coefficient '^x.^x. of the 89-keV

transition is taken as 1.43 from the tables of Sliv and 20)

Band ' , The presently reported half-life is corrected

for internal conversion and transition probabilities T(M1)

and T (E2) are computed. It is found that the experimental

E2 transition probability T(E2) is enhanced by a factor

.•••25 and the Ml transition probability T (Ml) ie retaitVed by -5 a factor'- 8 x 10 when compared to the single particle

21) estimates. Moss and McDaniels '' from their experimental observations concluded that the lower excited states of 99 Ru are the result of a multiplet formed by a coupling of

the 2dc-/p neutron to the first 2+ state of the even core 98

of the neighbouring nucleus, Ru. However, recent work

22) of Kaindl et al. on the analysis of the quadrupole

99 polarization on isomer shift measurements in Ru using

Mossbauer technique ruled out the possibility of any such

coupling. This discrepancy can be removed with the help

of our lifetime measurements. The core-excitation model

proposed by Moss and McDaniels suggests that the B (E2)

values of such multiplets should be equal to the B (E2)

values of the even core. The B (E2) value is computed

from our presently measured and corrected value of the

lifetime of the E2-transition of the 89-keV gamma ray.

13

The experimental B (E2) value of the 2+ —^ 0 + transition

of Ru is taken from the work of Stelson et al.' . The

ratio of these two quantities ^^Ru B (E2)/^ Ru B (E2) is

found to be 1.4, which is nearly unity. This indicates

that the conclusion drawn by Moss and McDaniels that the

99 lower excited states in Ru are the result of a multiplet

98 formed by a coupling of the neighbouring nucleus, Ru

seems to be valid.

(iv) The half-life of the 84-keV state in '''''Yb : The

170 half-life of the 84-keV level in lb is determined by

170 using a Tm (130 d) source. The measurement of the

lifetime is accomplished by observing the delayed coinci­

dences between 84-keV gamma rays and 886-keV p-rays. Here

tv/o plastic scintillators 5.1 cm x 5.1 cm are used in both

the channels. The plastic scintillator used in stop channel

for the detection of 84-keV gamma rays is mounted in an

aluminium can of sufficient thickness ( 400 mg/cm ) so as

to absorb p-rays. The lifetime spectiiim is shown in Fig. 7»

The final statistically computed value of many runs for the

half-life (T^) of the state is = 1.62 + 0.02 nsec.

The 84-keV transition is from 2 + to 0+ states and

24) i s a pure E2 t ransi t ion . The experimental t ransi t ion probabili ty i s calculated from our measured ha l f - l i f e value

20) using theoretical total internal conversion coefficient

«tot = •^^-

2x10"

1000

c O

u

c

^ 100 u c o u

10

• * T =1.62t0.02 ns«c

to

•I J

. • I "

Ch. No. 20 30

_ j . j _ 40 .

u 1 1 r 0 10 20 30 40 50 60 70

Time in nsec(Arbitrary-zero)

170 FIG. 7 LIFETIME SPECTRUM OF 84-keV STATE IN Yb

14

T (E2) ~ 5.6 X lo' sec"- ^ ' exp

The single particle estimate for E2 transition is-3.0 x

10^ sec"^ where E = 0.08423 MeY. Y

It can be seen from the above data that the experi­

mental transition rate is faster than the single particle

estimates "by a factor' -'1S9. This much of enhancement is

commonly observed in deformed region for E2 transitions 25)

within rotational band for even-even nuclei . The theory of rotational motion can be applied in-this case also since

170 Yb lies in the strongly deformed region.

1 R7 (v) The half-life measurement of 206-keY level in Re :

1 ft7

The 24 h a c t i v i t y of W decays through the p-decay to the 1 R7

excited states in 'Re. The measurement of the half-life

is carried out by observing the delayed coincidences between

48C-keV and 72-keV gamma rays. Here two Nal(Tl) scintil­

lators 5.1 cm X 5.1 cm are used in both channels. The time

spectrum obtained is given in Pig. 3. The same experiment

is also perfoOTied by keeping a lead loaded plastic scintil­

lator in place of Nal(Tl) in stop channel for the detection

of 72-keV gamma rays. The final computed value of many runs

for the half-life (Ti_) of 206-keV state is 555-3 + 1.7 nsec.

The 72-keV gamma ray from the de-excitation of the

206-keY state in 'Re is known to be a pure El transition ' .

Our measured half-life value gives the experimental transition

probability,

'OJ

M ^ » ioo

r" '^3 H

• ^

i K

;p:

a •^

31

.-• ^

M

^ t X* o <;

j > H r-M

00 _^ ^ 0

H

I ^ _ . D

O n

^ i - ^

> •n 2?

o •n »<

N f ) O

x _ ^

"^J

en

en o

00 O O

o

CD O O

"«s3

(Jl

o

00

o o

_ A

o (J) o

>

o o

CD O

o o

- 1 ^

CD cn O

_ i k

00 o o

1.

~o ^ PO

o

_ >

o

o

_ 0 0

o

_ 4 ,

-o o

- ro o

-it^ o

o

- 0 0

o

ro -o o

fO - rv:»

O

NJ - ^ o

Coincidence Counts

-TT-TTTJ-"(Ji

1—I—rr

1 N)

%

1

/

, 1 ,„J 'l I I I 1,

1 +

u (/I

o

1 1 1 1 1 1 1 1 J 1

•15

T (El)^^^-- 6.77 X 10^ sec"^

The value of total Internal conversion coefficient is taken

20) from the table of Sliv and Band '. The single particle

12 -1 estimate for the El transitioii is~1.7 x 10 sec . One

finds from these values, the El hindrance factor is -

4 X 10"'^. The 72-keV transition is from the band K=9/2

to the band E=5/2 with A K = 2. This transition is a K -

forbidden transition and the El-hindrance factor for such

-A -7 transitions is known to vary from 10 to 10 or even less.

Our conclusions are in agreem.ent with the results by

27) Perdrisat ^ ' . An empirical law has been proposed by

Rusinov^ ' connecting the hindrance factor to the degree

of K-forbiddeness. He gave log H = 2 ( A K - L ) , v/here H

is the observed hindrance and I the transition multipolarity,

This law is roughly compatible with K-forbidden El transi­

tions measured in odd and even -A nuclei. An attempt to

evaluate the hindrance of K-forbidden El transitions has

29) also been presented by Rouchanine jad -^' , He used a method

of projecting the Nilsson eigen functions on the eigen-

states of the total angular momentum.

(vi) The nuclear life-time measurements in 1-forbidden

transitions in Cs, Cs and Au :

(a) The half-life of the 124- and 134-keV states in ^^^^^ •

1'51 The 14d activity of •" Ba decays through the electron

131 capture to the excited states in Cs. The half-life

16

of 124-keV state is determined "by observing delayed coinci­

dences between 496-keir'and 124-keV gamma rays. This delgiyed

coincidence spectrum is obtained with Nal(Tl) scintillator

on the stop side (gated at 118-keV with a window of.'• '•30-keV)

and the Ge(li) detector on the start side (gated at 495-keV

with a window of 6-keV). The final computed value for the •

half-life (T^) = 3.80 + 0.01 nsec. While the lifetime of

134-keV state is determined from the delayed coincidence

spectrum obtained with the Nal(Tl) scilrfcillator on the stop

side (gated at 128-keV with a window of'--30 keV) and the

Ge(Li) detector on the start side (gated at 493-keY with

a window of 6-keV). The final computed value of the half-

life (Ti) of the 134-keV level is = 8.1 + 0.1 nsec. These

half-life values a-re obtained after the subtraction of the

slope due to electronics obtained with prompt spectra of

22

Na weak source having the same statistical accuracy and

under the same energy settings. The lifetime spectra

corresponding to 124-keV and 134-keV levels are shown in

Pigs. 9 and 10 respectively. (b) The half-life of the 81-keV state in ^^^Cs : The half-

133 life of the 81-keV state of Cs is determined by using 133 -^^Ba (7.2 I) source. The measurement of the half-life

is accomplished by observing the delayed coincidences

between 556-keV and 81-keV gamma rays» Here two 5.1 cm x

5.1 cm Nal(Tl) scintillators are used in both the channels.

io^

i2|10 § ! O i O I <^ i J= i

"O i

El 5! 10'

10 0

^ '

20 l _

-L

?2 ' ' 2 ' (V,.3/J -

V>. T, =(3.80i0.01)ns

\ " .

40 _ j

V

620

496

\(\''/2)-^-^

V5,;

•124

131 Cs

• •

•••

»• • • • • • ~

Ch. No. 60

I . 80 . t

100 120

10 15 20 25 30 35 40

Time in nsec (Arbitrary zero)

140

45

FIG. 9 LIFETIME SPECTRUM OF 124.keV STATE IN ^ ' ' ^Cs .

"1—r •'I I I I I M i l l — r

i

-t -( t - —1

4- ( p o

Is: IC

t- •• .h -H

& O

V Cj

--^

6 tl 00

II

Cv(

1 - ^

•s < ;

• » • ,y . . • • •

• • •

• •5

. • • . , : •

. . ^

• ; • •

, ^

y

• » . . • « •

V

X_J L. 1 I 1-J L _ _ L , li.. O

m O

04

T 22

o ID

O

o CM

O

2 O

o

o • o

o

o oo

. o

C9 c c a x: o

o 00

o CD

O

o

O

_o

o

N

o o ±:

"CD J 3

i n Ci» 0)

c

C9

(V) f—

O "CM

r\

H

>

A. I

o

-J

J

O

s^unoo 2DU3ppuio3

17

The same spectrum is also obtained with a Nal(Tl) crystal

for ':hc detection of 356-keV gamma rays and a lead loaded

plastic scintillator (5.1 cm x 5.1 cm) for 81-keV gamma

rays. I'he plastic scintillator is mounted in an aluminium

can of sufficient thickness (- 400 mg/cm ) so as to ahsorh

p-rays. The time spectrum is shown in Pig. 11. The final

statistically computed value of the half-life (Tj ) of the

81-keV state is 6o36 +_ 0.03 nsec.

(c) The half-life of the 77-keV state in ^^^Au ; The 65h

1Q7 activity of Hg decays through electron capture to the

197 excited states in Au. Two 5.1 cm x 5.1 cm lead loaded

plastic scintillators are used for this measurement. The

half-life measurement is done hy observing the coincidences

between 68-keY X-rays and 77-keV gamma rays. Since these

cannot be resolved in the plastic scintillators the combined

peak around 70-keV is gated in both the channels. For

obtaining the lifetime of the 77-keV state the contribution

to the slope from the electronics is subtracted with the

22

help of the prompt spectrum of Na having the same statis­

tical accuracy obtained under the same energy settings. The

final computed value for the half-life (Ti) of the excited

state is 1.84 + 0.02 nsec. The lifetime spectrum alongwith

prompt spectrum is given in Fig. 12. The experimental

transition probabilities T (Ml)^„^ and T (E2)^^^ have been Gxp exp

obtained from the observed half-life (Tj ) using the values 2

>

>5'

CM

to

CO

in

c O

d +1

5 o

a o-(>4

- . 0

tn u

u

c CO O 6 +1

CD

: • ^ • '

/

CM

+ + ^ CM in to .V

. .«•

o o rr CM-

o CD

o •CO

V ' . /

/

o. 00

o CD"

O

j , . i .1,1 I M I I I L 1 1 1 ( 1 L _ _ L

o CM

„o

n:

0 CD

0 I f)

0

0 CO

0 i _

C9 N

a 1 -

xi I -

< ^ — » •

u CJ

c

£ 0 £

I—

ti)

y rn

> Of •?

CO

k y^-'

Si •A:

53i

1 Hi

co «s

sj,uno3 aDuappujoo

c D o u tJ o c

C ' o o

10~

10^ =t

10 3i B t t f

IQ

o • » o

o

o

0 o o

o '

00 o •

<? (f

o o

o <h

00° 0

"<p

o o

oo o

• •

— 00

• * *

o

ooo

t/2*

3/2^

Hg(65h)

197,

77 KeV (1.8 4 t0.02)nsL_

0

Au

o •

o

CO o

Lifetime of the 77 KeV 197

X Stole in Au = (1.84 t0.02)n sec-

-4i

Na Promt spectrum

^

• • • o o

o o

oo o

o o o

• • i

. . • •

h40 80 Ch. No.

o o o o

o oo

o o

120 160 J

T AO 10

F * l . 12

10 20 30i Time in nsec (Arbitrary zero)

50

197 LIFETIME SPliXJTRUM OF 77 -k«V STAfE IN "^'Au (HOLLOW DOTS) -22-

ALONG WITH PROMPT TIME SPECTRUM^ OF • N» (SOLID DOTS)

UNDER THK SAME ENERGY GATE SETTINGS.

n

of tt-f. +> & and R in the eqn. (2-1) while the single

particle transition prohabilities T (Ml) and T (E2)

are those which have been calculated with the help of the

17) ' 2 laiown relations ' . The values of mixing ratio (6 ) are those which have "been reported in literature as a result

50-33) of angular correlation of polarisation measurements '.

The values of total internal conversion coefficient (a, ,) tot

32 34-) are taken either from the experimental measurements'^ ^ ^^' 20) or from the extrapolation of Sliv. and_^and's table ' ,

The value of branching ratio (R) is taken as 0.75 in the

133 33) 131 197 case ^^Cs -^ and for - Cs and Au as unity. Before

discussing the results of transition probabilities v/e will

discuss in brief the 1-forbidden Ml transitions.

35)

l-?'orbidden Ml transitions : According to strict

single particle model, the Ml transitions between states

of different angular momenta are forbidden. The calculation

of the transition probability for such 1-forbidden Ml transi­

tions requires modified assum.ptions about nuclear v/ave func­

tions. The radiative transition probability for a magnetic

dipole radiation '\ (Ml) may be expressed in terms of nuclear 35)

matrix element by the relation ',

r . mc

= 0.419 X lO-"- \'^ tp-Ty sec"- (2-2)

//here E is measured in MeV and I,, is the angular momentum

^ 2 of the initial state. The square of matrix element7'A is

19

"* ,'

Where V \i is the summation of the magnetic moment operators

35") of each nucleon in the nucleus. Arima et al. ' have

derived the simple expressions for the calculations of

matrix olemont of 1-forbidden Ml transitions on the basis

of configurational mixingj and are written as:

Ao For like core (L) transitions i.e. when odd particle

changes its state,

i f ^ (I.) I^ (0) -^ if (0) i f 1 (I^)

The matrix element is given hy:

™ - ^ ( I + l)($T^ +1) J ^ Lgd.^i^^i)]

X (gg - g- ) X Fj (2-4)

where (g^-gn) is 4.585 n.m. for an odd proton nucleus and

-3.826 n.m. for an odd neutron nucleus» The Fj which has

the meaning of the unfavoured factor, takes into account

of the'contribution due to all the possible models of

excitation as given below:

1. P (when I-, , Ip are two different mixing states but

having same orbital angular momenta 1-, )

, V 1(1 I.;I I /(/ E) _ n-^ i21^+l-n^) 1^ (1- +1) J s 1 2 1 1

^LI^ - ^LI^ = (21^+1) (2I2+I) "21"^: 'i y _y

^ g(-V^)i(i-Li2;iiV

(-A.E)

(2-5)

20

n-| , Hp denote the even number of particles in I-, and Ip

mixing states respectively.

The values in the curly "bracket in (2-5) must be

chosen in such a way that the even numbers of nucleons in

the orbits I-, and Ip are like or unlike nucleons with those

in the outer most orbit I.. The value of g is 0.834 for

the effect of proton excitation on the odd neutron transi­

tion. The interactions between nucleons are assumed to be

attractive and the attractive force inutile triple state is

assumed to be stronger than the single state of the two

nucleons in the ratio; V = 1.5 ]v j . I is a Slater

integral for a delta function interaction:

(2-6)'

The product of the singlet strength and the integral I has

the form

?gl (I^lg; I^I^) = - C2 F (I^Ig; Iilf)/2A (2-7)

A is the mass of the nucleus and Cp is a constant taken to

be equal to 250 MeV for harmonic oscillator wave function.

P is a non-dimensional constant which does not depend on A

35) but depend's on the shape of the wave function '^.

2. J'TTJ (when the mixing s ta te I-, coincidences with I^)

^11. = ^LII = 2 1 ^ ^ ll^+l ^s^ ^4' ^i^f) (- -h ) (2-8)

21

3. ^TTTT (when the mixing state lo coincidences with I.)

(2I.-1-P) l.(l.-i-l) ^^^2 . . . / 1

(2-9) •

^Liii^ - iiii^ = (2ij_-i)"" ' XIIT|-TT * s^^^'^'^i^f^ V T E .

B* For unlike core (U) transitions i.e. when the even

particle changes its state I?"- (I ) l| (O) -^ I^ (O) I^"^ (I^)

The matrix element is given hy:

TT r Pq il/2 l. (lf+l) 1/2 U = 2i._+l)(2I -H)J ^2(l.+l^+lJ^ (Ss-Sl) U

(2-10)

The contribution due to the first mode of excitation i.e.

P .j is given hy the same formula as the corresponding F-|.-|-,

while the contrihution due to other two modes are calculated

"by the follov/ing expressions,

q - 2 2 •'"f • f"'"-'-

^uii^ = uii^ = 2TpT ' s ^^f' i f "^ipT: ^2-^^^ and

21 +1-P 1^(1 +1 ) 2

UIII^ ~ ^UIII^ ~ 21^-1 21T+I s^ ^^i' ^i^'f^

(2-12)

The above expressions hold good only for the same case when

the angular moments of the initial and final configuration

are I. = 1 . - -J- and I„ = 1^ + -h. However, for the other case

in which 1. = 1 . + •§• and I^ = l.p - •§•, we need only exchange

the role of initial and final states i.e. I^, 1^, q should

be replaced by I., 1., p and vice versa in the above formulae.

All the measured lifetimes are tabulated in Table 1

along with the recent values of half-life reported in

literature. We observe that our measured half-life values

22

fairly agree with the previous measurements except in the

case of 154-ke? level in ' Os. V/e claim our results to

be more accurate compared to the previous measure-

ments^^'^^'^^'^'^?. They ' - ^ selected the K-capture

131 X-rays of Ba in one of the channels which do not feed

151 directly the 154-keV level in Cso Hence in their

measurements they had assumed that there exist no other

lifetimes which would interfere with the lifetime measure­

ments of 134-keV state Besides this,the statistical

uncertainties in their measurements seem to be largeo

Our measurement is a direct one, in which the 486-keV

y-ray in the start channel is precisely selected with

the help of a G-e(Li) detector. It directly feeds to

134-keV state and a Nal(Tl) detector is used for the

detection of 154-keY y-raj. Table 2 summarizes the

results of the measurements on the transition probabi­

lities and matrix elements of 1-forbidden Ml transitions

131 l^^ 197 in - Cs, Cs and ' Au along with the theoretical

single particle transition probabilities and matrix

elements due to Arima et alo

It is evident from Table 2 that the magnetic

131 dipole transitions from the excited states of Cs,

133 197

Cs and - 'Au are in general retarded by a large factor

because of the 1-forbiddeness. The E2 transitions on the

other hand are enhanced. The enhancement may be expres­

sed in terms of an increase in the effective proton charge

25

from the closed shell of protons at 50 and 80. Pechrxer

51) et al. ' from their angular correlation data predicted

151 the 124-keV transition in ^ Cs to be pure E2-transition,

The analysis of the results (Table 2) indicate

that the large retardation factor observed for the

1-forbidden Ml transitions cannot be explained by the

simple single particle picture in which the transition

takes place from one pure state to another pure state.

But the comparison of the experimental matrix elements

with those calculated from Arima's theory shows that such

a picture yield theoretical values in reasonable agree­

ment with the experimental values. The configurations

which give the best agreement with the experimental

values have been considered.

24

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27

C. THE DECAY SCHEME OF ^^Rh^^

(i) Source preparation and cheiDical separation : The source

was obtained in solid form from the Oak Ridge National Labo­

ratory (ORNL), U.S A.. According to the given specifications,

the enriched target material (99.9 ./ ) was enclosed in an

aluminium capsule and was bombarded with the proton beam of qq

the ORNL Cyclotron^ The 16.1 d - Rh activity was produced

by means of a (p,n) reaction.

Chemical separations are carried out to separate the

rhodium activity from the impurities, particularly aluminium.

The method used for it is a:s follows; The target material

is dissolved in aqua regia, then repeatedly evaporated to

dryness after adding a few drops of cone. HCl each time

and then final residue is dissolved in distilled water.

Milligram quantities of Rh in the form of chloride solotion

is added and rhodium activity is precipitated by adding

aluminium foils to the solution. The ppt. is centrifuged

and washed a fevv' times with distilled v-/ater»

All the measurements reported here are carried out

with the chemically separated source.

(ii) Single spectra, Q-amma ray energies and relative

intensities : The single spectra are recorded in different

energy regions with the help of a Ge(Li) detector of deple-

tion depth 7 mm with sensitive area 6 cm (given in Figs.

13-16). The energy resolution (FWHM) for 7 mm detector

28

was 2.8keV. The dynode pulse is amplified with the linear

amplifier ORTEC model 410. All the singles spectra are

recorded with the help of Packard 400-Channels Analyser.

Figo 13 gives the y-rajs observed in the energy range of

0-442 keV. We have found no evidence for the existence

of the 119.4-keV Y"-2?ay which was reported hy Moss and

21) McDanicls . The spectra recorded with the impurity

source showed the existence of a well defined photopeak

at 119.4 keV. This shows that the 119.4-keV y-T&j does

not "belong to the decay of Rh. Tne rest of the y-rays

in this region, hov/ever, agree well with the earlier work

21) of Moss and McDaniels . The y-raj spectrum in the energy

range 440-1200 keY is given in Fig. 14. In addition to

21)

the y- ays reported earlier ^ we have observed an addi­

tional Y~ a-y at an energy of 910.8-keY. This is found to

decay with the 16.1 d half-life. The peak at 778.1-keV QQ

does not belong to the decay of 16.1 d - Rh. In Pig. 15

we have plotted the y-raj spectrum in the energy range

1200-1750-keV. Pig. 16 gives the y-Tsy spectrum in the

high-energy region (>1960-keV). The y-^ays observed by

us in the singles essentially confirm the results reported

by Moss and McDaniels except for minor variations. The - , . . . . . . . 241. 57n 203TT 22„

energy calibration is done using Am, Co, Hg, Na,

Cs, Mn, Co and Y standard sources, providing y-rays

with energies in the region 60-1850 keV. The energies of

E z "5 c c a D

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Channal Number

F i a . 16 GAMMA-RAY SINGLES SPIKIRUM Of ^%h IN THE

ENERGY REGION 17^9-2059 keV OBTAINED WITH

A G«(Li) DETECTOR (LIVETIMi iSCft) MIN) .

29

the Y-3 ays observed by us in the 16.1 d decay of - Rh

are listed .in Table 3. The energies of the y-vfi.js a.

obtained from our energy clibration are very close to

the values reported by Moss and McDaniels. Therefore,

we have adopted their energy values except in the case 99 of the 1295-keV level in Ru. The starred peaks in

99 Figs. 13-16 do not belong to the 16.1 d decay of Rh;

the origin of these lines has not been explicitly

determinedo

The full-energy peak efficiency of the detector

used for recording the singles spectra is experimentally

determined ,using standard sources giving energies in the

range of interest, at a fixed geometry. The same geometry

is maintained throughout the single's studies. The area qq

under the photo-peaks of the y- rays of - Rh are determined

after subtracting the background and are used for the

evaluation of the relative intensities. The relative

intensities obtained by us are listed in Table 3 along

21) v/ith the values reported by Moss and McDaniels ^ and

Antoneva et al. . The intensities reported by us are

relative y-ray and no attempt are made to correct data

for internal conversion.

(iii) Goincldence Spectra

(a) Ge(Li)-G-e(Ll) slow-fast coincidences : Two Ge(Li)

detectors of depletion depths 7 mm and 5 mm with sensitive

30

2 areas of 6 cm each a re used for the slow-fast coincidence

s tud ies . The energy reso lu t ion (FWHM) for the 7 mm and

5 mm de tec tors were 2.8-keV and 3.5-keV respec t ive ly

1'57 for the 662-keV y-Tajs of CSo The "block diagram of

the associated e lec t ron ics i s given in Pig. 17• l he

resolving time ( 2 T ) of the f a s t coincidence c i r c u i t used

in the Ge(Ii)-Ge(Li) fas t -s low coincidence spectrom-eter

was 40 nsec while that of the slow coincidence c i r c u i t

was 2 (isec.

The coincidence spectra are recorded with gates

accepting the peaks at energies 322„4- and 353«0-keV.

The widths of the gate settings used are m.ainly to

include the photo-peaks of the y-Tscys of interest.. The

results are summarized in Table 4. The coincidence

spectruffx obtained with the gate at 322.4-keV is shown

in Pig. 18. The peaks observed in Pig» 18 at 175.2-, 322.4-

and 353.0-keV have probably resulted from coincidence with

the compton part of the annihilation radiation present

under the gate setting of 322.4-keV. The 295.7-keV y-ray

observed in coincidence with 322.4-keV y-^ay is due to a

transition leading from the level at 618.0-keV going to

the level at 322.4-keV. The peak at 511-keV is due to

the coincidences between the 322.4-keV y-va.j and the

511-key annihilation radiation feeding the level at

322o4-keV. No evidence for the existence of the 119.4

keV y-raj reported by Moss and McDaniels is seen in Pig.18.

5 i^ l < </) X > j O -J 1 < ' O Z = o < , <

UJ

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^^

o

y o y n H

?»: H

-• o

( Sr O

>

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H

J a

t^

CI

0*119

0-Gse • .

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31

The y-Vd,j which are observed in coincidence with

353.0-keV y-raj are shown, in Pig. 19.' The'SVidefte^'lor•-

the existence of coincidences between 553.0-keV y-xduj

and 89.4--, 175.6-, 941.5-keV y-rays is clearly seen. The

peak at 511-keV is due to the annihilation radiation. The

broad hump around 340-keV is due to the compton edge of

the 511-keV radiation.

(b) NaT(Tl)-Nal(Tl) sum-coincidence m-easurements : The

sum-coincidence spectrometer consisted of two 5.1 cm x

5.1 cm Nal(Tl) scintillators coupled to 56 AVP photo-

multipliers. The energy resolution (FWHM) for these two

detectors was 9-10% for the 662-keV y-rays of "'' ' Cs. The

linear signals from the two detectors are summed and

operated in a slow-fast coincidence modes. The resol­

ving time (2T:) of the fast coincidence circuit was 30 nsec

coincidence spectra are reported by fixing the gates at

energies of 575-, 618-, 734-, 850-, 897-, 941-, 1000- and

1295-keV. The sum-coincidence experiments are carried out

for establishing the existence of the cascade transitions.

99 99

The 16.1 d Rh decays to the excited levels in Ru

through Ec and p decay. The intense sum-coincidence

peaks at 511-keV that are obtained in the spectra are

mostly due to the coincidence*between the intense 511-

keV annihilation radiation feeding the levels and the

compton part of the following y-rays. The results are

summarized in Table 5.

o o CO

6)

E 3 2

"5 c c a x: u

g

H

H O « H o o >

CO

s i

f - <<ll

I O f o H S Qi

S H

Z H

en >H

< OS

1

V ^

s p ^

' * * < '

S • *

g w > a in S i i <m *2 ««

ii*

0* to

o

S (M

o o ^ s^unoo aDuappupo 2 c i

32

(iv) Results and discussion for establishing the decay

Bchome of ^Rh : The level scheme suggested "by Moss and

MdDaniels with some modifications which are warranted by

our experimental results is reproduced in Fig, 20. Our

investigations essentially support the decay scheme sug­

gested by Moss and McDaniels except for the following

results:

(a) Our coincidence data gave no evidence for the

presence of a 119.4-keV y- ray. The fact that we

have observed an intense 119.4-keV y-Ta.j in the

singles spectrum of the chemically separated

impurity led.us to conclude that the 119.4-keV QQ

y-ray does not belong to the decay of 16.1 d Rh.

(b) The existence of a 232-keV transition from the

322- to 89-keV level was reported by Moss and

McDaniels. Though we did observe a small peak at

232-keV in the Ge(Li)-Ge(Li) slow-fast coincidence

spectrum with the gate at 89.4-keV, we cannot

explain the sum-coincidence spectra obtained with

the sum-coincidence gate at 850-ke7 unless we keep

the 232-keV transition between the 850- and 618-keV

levels,

(c) Moss and McDaniels suggested that the 264-keV tran­

sition is between the 1662-and 897-keV levels. Our

sum-coincidence data warrants that it should be

vQ n o» CO O CO

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1662

.1532.9 1505.1

1382.9

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99

FIG. 20 LEVW. SCHEME OF ^^Ru . DASHED LINES SHOWN ARE THE NEW TOANSITIONS.

33

between 1381- and 618-keV levels. However, our

results do not rule out the possibility that there

could be one more 764-keV transition between 1662-

and 897-keV levels,

(d) The sum-coincidence spectrum with the gate at

1000-keV energy gave evidence for a new transition

of 911-keV energy. This transition is probably

from the 1000- to 89-keV level;;—A y-raj with

911-keV energy was also observed in the singles

spectra recorded with Ge(Li) spectrometer.

(e) The sum-coincidence spectrum recorded with the

gate setting at 1295-keV energy gave evidence for

a new transition of 295-keT energy from 1295- to

1000-keV level.

TABLE 3

Gamma-rays observed in the decay of 16.1 d

99 Rii and t h e i r r e l a t i v e i n t e n s i t i e s

34

Energy (E ) in keV ''

89.36

'119 .4

175.2

232.4

295.7

322.4

553.0

442.8

486,5

Annihi la t ion

527.7

575.2

618.0

734.2

763.9

306.6

850.3

897.2

910.8

941.5

Relative y

Moss et a l ,

76

0.13

5.8 ,

1.3

2 .1

16.5

81.3

4.3

1.5

rad ia t ion

100

0.6

10.0

0.8

1.0

3.5

0.6

1.7

-

3.8

-ray

21) •

I n t e n s i t i e s ( I )

Anton'eva e t a l . '

100 + 10

< 2

4.5 f - i . O

1.5 + 0.5

3.5 + 0.5

18 + 2

100 + 10

4.5 + 0 .5

1.5 + 0.5

100

0.8 + 0 .2

11 + 1

0.9 + 0.2

-

3.6 + 0 .5

41 1.7 + 0.2

-

3.3 + 0.5

Present

56.3

-

3.8

0.72

2.6

9 .1

78.3

5.4

0.89

100

0.47

11.9

0.61

0.88

3.5

1.1

2 .1

0.13

3.4

Table 3 (Contd.)

35

Energy (E ) in keV '

1000.2

1061.2

1089.4

1208.3

1295.2

1323.9

1382.9

1442.1

1484.3

1505.1

1532.9

1572.4

1618.0

1662.1

1749.1

1970.3

2058.6

Relative y-vaj

21) Moss et al. ^

1.7

0.4

0.8

0.4

0.9

0.4

0.4

0.2

0.4

0.2

1.4

0.58

0.6

0.15

0.15

0.4

0.08

intensities

Antoneva ei

2.0 + 0.

0.6 + 0.

41

4 0.8

1.0 ± 0.

4 0.5

%0.4

<50.4

<0.4

<0.4

1.9 + 0.

0.7 + 0.

^< 0.6

< 0.4

< 0.4

< 0.4

-

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2

2

3

4

2

p-r*p op-n-f X i- \^ iD\^li.\J

2.0

0.55

1.0

0.66

0.72

0.66

0.29

0.34

0.14

0.1

1.3

1.3

0.9

0.23

0.6

0.21

0.43

21 The values reported earlier by Moss and McLaniels ' and Antoneva et al, ' are also given.

•36

TABLE 4

Summary of the Ge(Li)-Ge(Li) fast-slow

coincidence measurements

y-ray Energy E (keV) Y~ a-y i^ coincidence with E

322.4 295.7

353.0 89.4,175.2, 941.5

37

TABLE 5.

Summary of the Nal(Tl)-NaI(Tl)

sum-coincidence measurements

Sum-coincidence gate energy (keV) Cascades observed

575 5 7 5 ^ ^ 89 0

618 (a) 618 ^ 89 0

(b) 618 ^ ^ 522 ^ 0

(c) 618 i ^ 443 ^ 0

734 734 ^^^0

'850 (a) 850 - ^ ^ 618 ^ ^ 0

(b) 850 ^ 0

897 897 ^ ^ 89 0

941 941 ^ ^ ^ 175

1000 1000 ii^ 89 ^ 0

1295 (a) 1295 ^ ^ 1000 i ^ ^ 0

(b) 1383 ^ ^ 443 ^ 89

(c) 1383 ^ ^ 618 ^ 89

CHAPTER III

MAGNETIC MOMENT MEASUREMENTS

Recently the techniques of measuring magnetic dipole

moments of nuclear excited states with short lifetimes

have developed to the extent where they can provide,a

significant addition to our knowledge about the magnetic

properties of nuclei. Already the experimental work done

has proved to he of major significance in testing the

well developed theories, and one can no doubt expect

that the additional results in other areas now being

obtained will also play a significant role in under­

standing other aspects of nuclear structure and nuclear

magnetism. The magnetic moment measurements are carried

out with the help of the time differential (y-y) perturbed

angular correlation technique (TDPAC). This technique

yields directly the interaction strength independent of

any knowledge of the nuclear lifetime of the excited

state. This method also gives information on the environ­

mental conditions of the source, i.e. the time dependent

perturbation effects, relaxation processes, etc. The dif-

ferential method has an upper limit, it can also be used

if the resolving time of the coincidence arrangement is

considerably smaller than the lifetime of the excited

state under consideration. Since the number of oscil­

lations obtained in the measurements with TDPAC technique

38

59-

is quite large, therefore, the Larmor frequency can be

determined very accurately using Fourier transformation

technique. Hence the''value of the magnetic moment obtained

with this method will be more accurate as compared to other

techniques.

The angular correlation and Mbssbauer methods of

determining electromagnetic moment of excited nuclear

states are based on the static interaction between

external field and the nuclear moments. "ffinTB, these

methods give results which are independent of any assump­

tion concerning the origin of these moments and are,

therefore, classified as model-independent or spectro­

scopic methods. It is possible to establish relationships

between the static electromagnetic moments and dynamical

properties of nuclear states v;ith some degree of confidence.

It is thus feasible to obtain reasonably reliable values

of the electromagnetic moments of excited states by observing

the properties of transitions between nuclear states. The

results on nuclear moments obtained in this manner are

obviously model dependent. The magnetic properties of

deformed nuclei (in this thesis we are presenting a case

of Re which belongs to the deformed region) are of

interest both liecause they represent another group of

nuclei whose structure is thought to be reasonably well

understood, and also because there is a considerable amount •

of experimental data available.

40

The measurements on lifetimes together with the

measurements on magnetic moments should he very valuable

for the understanding of the structure of the particular

nuclear excited level.

A. MAGNETIC MOMENT OF 206-lceV STATS IN " j' Re n- ' ^ :# ^

1. Source preparation : The g factor measurement of

the 206-key level is carried out with the source in the

solution form as sodium tungstate. The source is procured

from the Department of Atomic Energy, Bomhay (India).

2, Experimental set-up i A smaller, C-frame iron core

electrom.agnet, capable of producing a maximum field of

7 kOe over a 1 cm gap with a 1 cm diameter of pole piece,

is used. The stability of the magnetic field is 1 7 for

a typical run of 7 days. The field of the magnet is

measured either by a-Hall probe (Bell model 240) or by a

rotating coil gaussmeter (New Rochelle, model PM). These

instruments arc calibrated using proton resonance. Thus,

errors in fields are due principally to inhomogeneities

and drift.

There are two basic types of shielding material -

medium permeability (NETIC) material for medium attenuation

(which will withstand high magnetic fields) and high

permeability (Co-NETIC) or high attenuation shielding

material (which will saturate at lower fields). Multiple

41

layers of Co-netic and Netic material, separated by non­

magnetic spacers, are used for shielding the photomulti-

plier tubes. For maximum shielding of the phot omultipliers

these layers of Co-netic and Netic material are extended

well beyond the face of the photomultiplier tubes. The

effect of the field is checked in single y-^ay spectra

and prompt time spectra as well.

In the magnetic moment measuremen±£_the two detectors

are kept at an angle of 135° to each other in a plane

perpendicular to the external polarizing field (as shown

in Fig. 21).

3. Decay scheme and gamma rays : In Fig. 22 the decay

scheme of W pertinent to our studies is given . The

(480-72) keV gamma cascade is used for the magnetic moment

1 Pii micasurement of the 72-keV state in Re.

4. Magnetic moment m^easurement of 206-keV state ; Two

5.1 cm X 5.1 cm Kal(Tl) scintillation detectors coupled

to 56 AVP photoff/dltipliers are used for the detection of

480-72 keV cascade. The fast pulses from the photom.ultiplier

tube in the stop channel are amplified using EG&LG- 1 nsec DC

amplifier. The outputs of the ORTEC fast discriminators

are fed into a model 437 ORTEC time-to-pulse height converter.

The source of appropriate strength is put in very smiall bulb

provided at one end of the pyrex glass capillary tube. This

source is placed at the centre of the pole pieces of the

J,

L,

T. in mec.

COUNTER

STOP CHANNEL

COUNTER I

START CHANNEL

MAGNET

F I G . 21 ABRANaEMl!3<JT OF MAGNET AND DETECTORS

u

C

CM

U

c in ir» tr)

tn Q.

II JN 'CM

to m to o

en en II

> ^

* o o H °o i: <r C

o •

o N . o

;

-;;

c 2 f*

(*>—• r»^^

*—N

00 > "* - 6 to ^ CM * - '

O X

ac GO

x: CO CM

M

s bi

CO

42

magnet. The experiment is carried out at 7«00 KOe and a

iDackard 400 channel analyzer is used tc record the time

spectra. The ratio,

p^ + '\ - C!(9,t,H- -) - C(6,t,H-v) /_ \ ^ "'' - c(e,t;Hi) + 0(9,t,Hi) ^5-1)

3 exp (-A t) Ag Sin (2c^t) ^^^

" 2 + exp (->.2t; t Ag ' H = 0

is obtained for each time channel.

Here G(9,t,H4/) and C(9,t,Ht) are coincidence c'ounts in

the same time channel for field down and field up respec-

tively and A - relaxation constant, u. ^ = -—.- is

the larmor frequency of a nucleus in the magnetic field

I-I. The time spectrum with field on is given in Pig. 23.

Pig. 24 shows the measured expression R as a function of

52) time t . The s i n e , cosine and a b s o l u t e t r ans fo rms ' defined by

A (c...) =. "> R( t ) Sin (27itc^t)

B (L5) - ' >R( t ) Cos (27lu:^t)

F M - WWnrWW) (3-2) a re p l o t t e d in F i g . 25 .

The va lue of the Larmor frequency i s ob ta ined from the

a b s o l u t e t ransform P(co) which i s independent of p h a s e .

The va lue of the double Larmor frequency i s = 1 2 , 1 + 0.2

MHz. The measured Larmor frequency i s r e l a t e d through

the r e l a t i o n ,

.o1

^ in-•^ 10 D O U

u c

u

#

10 b

' • • • • • • • • w t ^

' • ^ • • . . ^ . . M ^ ^ ^ • • • •^ • •MM.!^

••••*«^«> • • ^ - — - - ^ A . , ,-f-H,. ^ • M M M ^ , ,

Source

^ :

• • • •*•• • •%••( •••••^••^.••.••, •s* •%•.•«,

••^•^H.,„

10 20 AO _ L _

Ch. No. 60 80 _L ±

too J

120 J

uo _I

16Qi

100 200 300 AOO 500 600 700 800 900

Time in nscc(arbitrary zero)

FIGj. 23 TIME DIFFERENTIAL PERTURBED ANGULAR CORRELATION SPECTRA OF 187 Re IN AN EXTERNAI. MAGNETIC FIELD OF 7 KOe.

o o H ft.

i

OJ' s

o o LfX

o o St

i

^

o o CO

c - « - •

9

5 z H

00 >•

<

e §. 0 . CO

o <

s s

Q

O

5i

« tt O > «

« I

^ CM s:: o ?:; $^ $5 • • • o o o o o o o

+ + • o ' I I rr

T7-TT

^

• • f

o . / f t :

X

/ •• •,

•••

•• •

c S d c J o o o d d o •f + I I I i

(/ jDJ)|qjv)apni!lduLJV

CM CM

O CM

00

CD * "

CM

O ' ^

CO

CO

<

N X 2 c

3

§

g 9

PC4

•P

&< o «5

2 o ^

^

e H

8 p

9 O

t -

fa o Q sJ H fo o H

<3

2 9i

CM

^

6 H E>A

R

43

^-L = - iS ^5-3)

Where (j. is the nuclear magneton and H , is the externally

applied magnetic field. After applying the diamagnetic

correction, the final measured value for g-factor is

= + 1.12 + 0„03o Since the spin of the 206-keV level

is 9/2 ^ and the value of the magnetic moment_4i_of the

state is = (+5.04 + O.I4) nm.

B. MAGNETIC MOMENT OF 68-keV STATE LN ' " Sc

1„ Source preparation : The Ti source is obtained in

solution form as chloride from Nuclear Science and Engineerirg

Corporation (NSEG), USA and is used as such for carrying out

the experiment for the magnetic moment measurement.

2. Decay scheme and gamma rays : In Eig. 26 the decay

44 12) scheme of Ti pertinent to our studies is given . The (72-68)-keY gammia cascade is used to carry out the magnetic

44 m.oment experiment of 68-keV state in Sc.

3. , Magnetic moment measurement of 68-keV state : Two

5ol cm X 5.1 cm Nal(Tl) scintillators coupled to 56 AVP

photomultiplier tubes are used for the detection of (78-

68)-keV cascade. The fast pulses from the photomultipliers

are amplified using EG tG- 1 nsec DC amplifiers. The outputs

are processed through the ORTEC fast discriminators and

time-to-pulse height converter. The source of proper

strength is put in a very small bulb provided at one end

o ^

flO II t^ J=

N — '

rf"-^

^ o w ' ^ o ( O II

'-^ > i::! w o 3<^ ' I T

II ® u to _ S f c ^

fc

£

r)

sr

.8 ^.

C«J

^ o U) II £S,

u eg

c in tn M

«-C4

^ » -

13

44

of the pyrex glass capillary tute. This source is placed

at the centre of the pole pieces of the magnet. This

experiment is also carried out at 7.00 KOe, applied per­

pendicular to the plcine of the detectors, and a Packard

400 charjiel analyzer is used to record the data. The

application of magnetic field produces oscillations on

the time spectrum with the sign of the moduilation depending

upon the direction of the applied field (see Fig. 27)__. With

the field up and field down the spectra have modulations

of opposite phase. The ratio,

^ ^ ^ ~ G (9,t,H,0 + C (9,t,Hf)

3A2 Sin 2«^t

where 0 (9,t,Hi) and 0 (9,t,Ht) have the usual meaning

as explained earlier since the intermediate state has a

12)

spin 1, therefore, the A^ term, is zero ' . Fig. 28 shows

the plot of the measured expression R as a function of

time t. No attenuation of R is seen upto some [isec.

Using the expressions given in relation (3-2), the Fourier

transforms of the data are plotted in Fig. 29. The Larmor

frequency is obtained from the absolute transform F (-o)

which is independent of phase (^). Thus the value of the

double Larmor frequency is = 3.65 + 0.05 MHz. Using the

relation (3-3) the value of the g-factor is calculated.

After applying diamagnetic correction the value obtained

a u

SB

o a

< H

OS p

•J - X

S

<? 0 H «

* J-

ft i

H (3

o

^

' O O o R fa

1 1 1 1 1 r

' ' I > t * I ' t t

8 S 5 9 o S 8 o o o o o o + • * ^ I I I

cr

o e . Ck O

Q

si

m o > w

4*

« O

00

••J '•. T — r - * T

3 CD

:'? •••••• / • - . „ ,

.1 , • • ^ ^

• • • • i

••. \ .••

J L X iK 1 L I , I

CD

ID

N CD «^

: 2

<D

CO

« • • . • ^ • • . o o o o o o o o o • • 4 • • I I I

•<r: If) o o

I I

o

(AJDijiqJV) apn^iiduiv

4>

m

9 Wl O 3; ui

a M

S h

45

f o r the g - f a c t o r i s = + 0.345 + 0 . 0 0 ? . Since the sp in IP)

of the oS-keV s t a t e to "be 1 % the magnetic moment

(J, of t he 68-keV s t a t e i s (+ 0.345 + OoOO?) nm.

C RESULTS AND DrsCUSSION

Our measured r e s u l t s a re t a b u l a t e d in Tahle 6 along

wi th the o the r a v a i l a b l e exper imenta l v a l u e s i n the l i t e r a ­

t u r e f o r comparison. The 206-keV exc i t ed s t a t e i n odd A

187 53)

deform.ed nucleous Re has been identified ' as a

Nilsson state- ' ' with the q_uantum numbers 9/2" (514+)

i.e. [I = I , K =-Ci.= |-, N=5, 1^2=1,A=4, and ^ =l].

Using the Differential perturbed angular correlation method Koicki et al. ' , Walter et al. ^ and Nigam and

51) Bhattacharya ^ obtained the values for g are 1.046 + 0.03,

1.11 + 0.03 and 1.04 + 0.04 respectively. Koicki et al.

made their measurement at two different fields 1720 and 5020

Oe. respectively while Walter et al. and Nigam-Bhattacharya

used external fields of 3150 and 3100 + 30 Oe. respectively.

In the present measurement, however, the external magnetic

field is 7000 + 70 Oe. Our measured g-factor is in fair

agreement with the previous measurem.onts (see Table 6).

Z • If rotational g-factor is taken as g-^ = - ^ =

0.407 and free proton spin g-factor g„ = 5.585,then using

the Nilsson's formula - a value of g = 1.32 is obtained,

which is considerably larger than the experimentally

measured g value. However, as suggested by De Boer and

46

55)

Rogers ' if the free nucleon spin g-factor is taken to

"be 0.6 g^, then a value of g = 1.08 is obtained and it

is in fair agreement with the experimentally determined

value of g. The sign of the g-factor is also determined

from the sign of the anisotropy and the sign of the first

oscillation (when the modulated time spectrum is carefully

extrapolated to zero time). From Table 6 we observe that our measured g-factor

A A

value for 68-keV s t a t e in Sc a lso agrees well with the

previously reported values for go If the l eve l s of Sc

are a l l derived from the same configuration for the

neutrons and protons , the magnetic moments of the l e v e l s

are given by:

. I-, ( 1+2) - I (I +1) V- = {-^1) (g^+gg) + (gi-g2^ 2 (I + 1)

where I is the total angular mom.entum, I-, and I^ are the

angular m.omenta and g-, and gp are the g-factors for the

proton and neutron groups respectively. If the angular

i< 4 momenta of the proton and neutron groups in '' Sc are

taken 7/2 ', the g-factors for all the energy levels

will be identical and will be given by g = -I (g-i+gp)-

Using Schmidt values for the odd neutron and odd proton,

a g-factor of + 0.55 is obtained. If the configurations

for a proton and a neutron groups are assumed to be

1 '5 " 7/2 7/2 ^^ " 7/2 7/2 respectively, a g-factor of

47

+ 0.50 is obtained. These values of g-factor do not

agree with the experimentally measured g-factor values

for various levels in So. This clearly indicates that

this simple model is not appropriate for Sc« The absence

of any definite knowledge of the configuration of 68-keV

44 state in Sc is an hindcrance in interpreting the g-factor

of this state.

It is interesting to note in Figs. 24 and 28 that f

no attenuation of the function R or of the differential

1 R7

angular correlation in a period of 0.7 (isec (in Re

measurement) and 0.4 jisec (in ' Sc measurement) is detected.

Nevertheless, for sources in liquid form, this attenuation

must always be present (even though too small to detect

during the nuclear lifetime)due to the interaction between

the nuclear quadrupole moment and the fluctuating electric

field gradients produced by neighbouring atoms. From

Figs. 24 and 28 a limit may be set for the exponential

attenuation factor or relaxation constant X > 4 x 10

sec" andX'^ 2 y: 10 sec" respectively for 'Re and be .

The Fourier transform of the R(t) function is

essentially the NMR line having a Lorentzian shape. In

Azi the case of Sc magnetic moment measurement, the

observed width (F¥HM)--9 x 10 eV is about twice the

48

natural width = 4.4 x 10 - eV. In tlie 'Re magnetic

moment measurement the observed width (PWHM)~15 x 10 _Q

eV compared to the natura,! width of ~ 1.25 x 10 eV.

The large observed width may probably be due to the

quadrupole interactions etc.

49

TABLE 6

Comparison of the p r e s e n t magnetic moment measurements

wi th a v a i l a b l e pub l i shed v a l u e s

M,^-i^ „ Level Ex te rna l f i e l d .P 4. D -P--Nucleus jc^g^) app l i ed (KOo) g - f a c t o r References

^^'^Re 206 1.72 1.046+0.03 47

5.02

3.15 1.11 + 0.03 46

3.10 + 0.03 1.04 + 0.04 51

7.00 + 0.07 +1.12 j^ 0 .03 P r e s e n t mcasure-and

p,= +5.04+0.14 nm ment

^^Sc 68 5.560 + 0.011 +0.35 + 0.02 11

2.648 + 0.005

7.550 + 0.075 +0.342 + 0.006 12

7.00 + 0.07 +0.345 + 0.007 Present

"" measure-and

^= +0.345+0.007 nm ment

CHAPTER lY

T f P E R P I J J E P I E L P MEASURE^IEKTS

A iri a ORIGIN OF THE HYPERPINE PIELDS, HYPERPINE PIELP MODELS

AM) SY5TEMTIGS OP HYPERPIHE FIELDS

Hyperfine field determinations are often used as a

tool in the study of the magnetisui and magnetic matericils.

Hyperfine fields at impurities in ferromagnets can iDe

studied with respect to (a) variation with atomic numher

A (or'Z) for different im.purities in the same host ,

(h) variation with tem.perature , and (c) changes with

the impurity content '. The first case will give infor­

mation on spin polarization, transfer and overlap effects.

Prom (b) one can find out a possihle local m.ome2it behaviour,

whereas case (c) is used to study neighbour effects for

higher concentrations. Most of the experiments reported

in the literature have been carried out in iron and nickel

hosts. The interpretations of the measurements is then

relatively simple, since impurity atoms usually occupy

regular cubic sites. The general trends in the variation

of the magnetic hyperfine fields with impurity A (or Z)

are reasonably understood. The hyperfine fields are

discussed in terms of a semiempirical model by Shirley

et al. . In the Daniel-Friedel theory , we consider

the scattering of the electrons around the impurity which

50

51

results in a net spin polarization at the nucleus. This

model was further extended "by Campbell ^.

V/hen we measure the hyperfine fields on dilute

impurities we essentially sample the m.agnetization on the

impurity nuclei alone. These measurements need not strictly

confirm to the bulk magnetization measurements like suscep­

tibility etc. In fact, experimental measurements on the

temperature variations of the hyperfirte fields have clearly

showed these ef f ects " '.

The hyperfine field measurements as a function of

temperature on many dilute impurity atoms showed that the

magnetization at the impurity does not follow the host /'p^

magnetization curve. As suggested by Jaccarino ct al. '

in those cases there is a possibility for a localized

moment around the impurity atom. Similar experimental

studies are made by Rosenblum et al. ' and Pramila et al. '

also confirm the above conclusions. However, the hyperfine

fields as a function of temperature are found to follow the

bulk magnetization properties of the host ' '.

Till 1967, the most precise values have, in general,

been obtained by spin-echo magnetic resonance exploited

extensively by Eontani and Itoh ', though it should be

em.phasized that these measurements are probably on solutes

in domain.walls while other methods sample the entire bulk

material. This difference may account for the discrepancies

52

in H, r. reported from different techniques. The time-

differential perturbed angular correlation (TDPAC)

technique is a powerful tool for precision hyperfine

field measurements in ferromagnetic lattices. The TDPAC

technique has two important advantages OYBV other methods

such as nuclear magnetic resonance; the measurements can

be performed (i) at lov/ impurity ccricentrations, and (ii)

over a wide temperature range.

(i) Origin of hyperfine fields on impurities in ferromagnets 44

Before we start discussion on our measurements on Sc and T on

Re, we give a discussion of the observed solute hyperfine

fields in iron, cobalt and nickel latticeSo Taken individually

the solute fields are of little importance but their variation

with host magnetization and particularly v/ith solute atomic

number can lead to an understanding of their origins. The

origin of hyperfine interactions in ferromagnets is still

not well understood. However, further theoretical work on

the manybody problem may better our understanding of these

interactions. Here we shall try to define the 'hyperfine

field' and shall elaborate the mechanisms that can give

rise to these fields in ferromagnets. These mechanisms can

then be related to the electronic configurations of solute

and the solvent atoms.

In a ferromagnet the effective field experienced by

a nucleus may be defined as,

53.

H. „„ = H, J, + H ( i n a domain w a l l ) e f f h f jj ^

or

H ^^ = H, n + H-p + H - DM ( i n a domain) e i f Txi L 0 ^ •

Here H, ^ and H represent the hyperfine f i e ld and the

applied f i e l d , DM i s the demagnetizing f i e ld and H-j- i s

the Lorentz f ie ld (4n;/3 M) plus the f i e l d a r i s ing from . . - . .-—V

dipoles in Lorentz cavity. Hi and H-j- are found, in

general parallel (or antiparallel) even in domain walls.

In order to understand that hov/ the hyperfine fields in

57)

ferromagnetic metals a r i s e from hfs ; Shirley et a l , '

defined a Hamiltonian which i s appl icable to both a

ferromagnetic host metal and so lu te ,

= ^cf "2 ^-^x ' ^ ^ ^ ' S - YiHe -"^

+ 2 p Yj v.-"^- ^'1*1 + [?^L(L+l)-lc] "S-I

~ I I [(L.S)(L-I) + (L.I)(L^)] ^ J

In using and explaining this Hamiltonian we think of a

particular solute atom characterized by the quantum

numbers L, S, and I acted upon by all the other impurity

atoms in the lattice characterized by the crystal field

interaction (V ) ,• the exchange field (H ), and the

conduction electron polarisation (K ). The XI'S term

is the electronic spin-orbit interaction and the terms 67) in curly brackets represent the magnetic hfs interaction '

54

in operator equivalent notation . The L'l term represents

the interaction of the iilectronic orhital angular momentum with

the nuclear spin, the ."kS'I term, the polarisation and the

three terms in - the interaction of the electronic spin

with the nuclear spin. Here p is the Bchr magneton, and

<'r > is evaluated for open electronic shell (if any) of

72) _

the solutec The first three terms are the largest and must

he evaluated first to give the zero order wave functions.

Except for rare earth solutes j the /\ 1 • S is smaller than

the other two parts. The fourth term descrihes condactioh-

electron polarization, H . It is approximately proportional

to the lattice magnetization.

For the situation in which the spin - orhit coupling

is smaller than both the crystal field and the exchange

field, we can assume that the electronic orhital angular

m.om.entum is quenched by the crystal field. For cubic lat­

tices the Hamiltonian can be written as a sum of two parts,

where :,'\' -, = H ^, which determines the zero order v/ave 1 cf'

function and

Pi-^ = 2 p~Hg^ .^ - Yj H -"! - 2p Yi (^'^^ ^ "S-l

= 2 P H e x - S - Y^-tif

55

In the above equation the second term is in the form of

magnetic field interacting v/ith magnetic dipole. The

exchange term is the largest among the other terms

involved in hL. If it is considered that this is evaluated

first to give <'Sr7) , the expression for H, „ can he written

as scalar

\f = He + 2 < S^) H^

where H. = p k <r ; , the core polarization hyperfine

field arising from a single unpaired d-electrons. Accor-

69) ding "CO Shirley and tfestenbarger ' H = p >H where H

is the free atomic hyperfine field arising from atom in

ns state. This substitution is perm-issiblc because it

is expected that conduction band s-wave states resemble

the atomic functions near the nucleus. Thus the final

expression for the hyperfine field is''''',

hf ^ ns ^ S d

The first term on the right hand side is the conduction

electron polarization (CEP) contribution and the second

is the core polarization (CP) contribution, which arises

only in cases v/here there are unpaired magnetic electrons

(i.eo, open p,d shells). This equation should be valid

for all impurities in ferromagnets except for those with

incomplete f-subshells, because we assumed

56

£Q study the relative importance of the mechanisms

that produce hyperfine fields at solutes in ferromagnets,

it is useful to survey the fields reported in iron, cobalt,

79)

and nickel latcices. The earlier observation -^ that

solute fields vary smoothly with atomic nuEQber has been

very nicely confirmed for all the three host lattices. 71) A-i uptodate such compilation ' is displayed for all the

three lattices ¥e_, Co and M in Pigs. 30,31 and 32 respec­

tively. In the case of iron, cobalt, and nickel the

electrons involved in this exchange interaction are the

unpaired d-electrons, A reasonably good approximation

can be made that these d-electrons are localized on

individual atoms and the spontaneous magnetisation can

be considered to arise from the summation of all the

atomic moments. It is the same d-electrons which are

also responsible for the large magnetic hyperfine fields

at the nuclei of atoms in ferromagnets. In cubic ferro-

magnets these fields arise principally from the Fermi

contact interaction of s-electrons which have been

polarized by the d-electrons. The mechanism by which

this polarization results is not quantitatively under­

stood as yet, but the theoretical treatment given by

Freeman and Watson ' ' is encouraging. The exchange

interaction arises from purely electrostatic forces

as a result of the Pauli exclusion principle and is

$.8

w r

00 o o O O o

1 <J>

o o

1 to O o

^

te 8

a

8 4 ^

SJ a

S-" C/1

8-

en Q.

©^ 4^

CD. O

O O

en

g

m

I

o o ^^

^

6"

8-

N) XI

XI

a

1

ro«c in

3

I

o o 1_

I o o

o o • t

o o .. I

o o

0 3 * >

57

written most generally as,

;'4 =- 2 .T j . . t . •-!.

v/here J. . is the strength of the interaction and S. and

S. are electron spin operators. The summation is carried

out for all atoms i with all other atoms j ^ i. The

exchange interaction is not generally isotropic.

(ii) Hyperfine field models : The large magnetic hyper-

fine fields observed experimentally "aT the nuclei of

impurities dissolved in metallic iron, nickel and cobalt

can be explained 'tjj the following three existing models,

1. Conduction electron polarization (GEP)

2. Core polarization (CP)

3. Overlap polarization (OP)

1. Conduction electron polarization i The contribution

of the conduction electron polarisation to the hyperfine

field (Hp -rj) at the site of the nucleus is largely due to

the contact interaction of those conduction electrons that

have S-character with respect to the impurity atom. This

59) model was proposed by Daniel and Friedel \ In this

model the d moments (u, ) of the host atom.s are assumed

to act as an effective field on conduction electrons,

giving rise to a difference in energy of the conduction

electrons with spin up and spin down. Since the electrons

with spin up and spin down should fill the conduction band,

5?

therefore, a difference in their density is resulted. The

sign of the difference depends on the character of the

coupling between the 3d electrons and the conduction

electrons, which may be parallel or antiparallel.

The impurity nucleus is considered as a rectangular

potential well, having a depth Z.-Z, betv/een the impurity

atom and host atom (where Z. is the valence of the impurity

atom and Z is the valence of the host atom). The radius

of this potential well is defined as 'a' and is set by

certain assumed number of S-electrons per atom in the

conduction band. Due to their difference in energy in

conduction band both types of electrons will see a dif­

ferent potential at the impurity site. This means there

will be two wave functions, "4-' 1 and H'' •• This implies a ' s s ^

difference in density of both types of S-electrons at the

s i te of the nucleus, f'Nv(0M! ^ and K^(0)'^l ^. The result ing t o . ] ' S

net conduction electron polarization will be p| (0)t . ^~

1 (0)4 !• It may be positive or negative, depending

on which effect is stronger.

Daniel and Friedel assumed the conduction band to

contain one S-electron per host atom, and calculated this

polarization at the impurity site P. as a function of the

valence (see Fig. 33, curve a). They predicted the reversal

in sign of the hyperfine field at Z.~ + 3 and concluded that

the experimental results show that the host conduction electror

-no»-

F I G . 33 CALCULATED Ptl,ARIZATTON P OF T;^':. S-LlAvCTRONS

AT THE IMI^URITY SITE AS A FUNC ril?."' OF THE /ALENCi,

Z^ OF THE IMPURITY ATOM. CURVy'a'REPRESENTS THE

ESTIMATE OF DANIEl. AND FHIED£3. } Cri';Vi.;'b'REI^RESENTS

THE ESTIMATE OF CAMPBELL. FOR IROK r . = 1^ r

59

polarization is positive.

Tliis model is later on modified by Campbell ^ when

Daniel and Priedel model could not explain certain experi­

mental results of H, . (say for exam.ple Cu?e). In the

modified version of Daniel and Friedel model, Campbell

assumed that the conduction band is taken as a composite

band with 4 electrons (in S-p shell) for each direction

of spin; one of these 4 electrons is S, and there is the

same density of states curve for all electrons. The non

S--electrons can be thought of as being d-like near the

bottom of the band and p-like -elsewhere. For the details

we refer reference 60). On the basis of Campbell's model

the behaviour of the polarization at the impurity site,

P., as function of the valence is given in Pig. 33 curve b.

Finally he gave the following expression which will give

the contribution of the E. r, due to conduction electron hf

polarization,

H^gp = A (Z) P_ (0.6 - 0.4 i/[i )

A(Z) are the free atomic hyperfine fields. If we know

the host and impurity moments, v/e can calculate the

contribution from. H -pp. For iron ji, = 2.22 |ir, and for nickel

[I, = 0.606 |i where |i-n is Bohr magneton. Shirley and gq\ 57)

Westenbarger ^ and later Shirley, Rossenblum and Matthias -

also assumed this proportionality of Hp-gp with A(Z) and deduced

from the experim.ental values the empirical relation,

60

2. Pore polarization : This model is due to Freeman and

72)

Watson and they have extensively treated it hy m.eans of

Hartree-Pock calculations. Core polarization is chiefly

caused hy the exchange interaction of an unfilled d shell

with the filled S shells giving rise to a net spin density

at the nucleus. The resulting hyperfitie field (Hp-p) "being

a superposition of the contributions from all S shells. The

regular variation of H, v/ith solute atomic number in the

3d, 4d and 5d transition series is very interesting. In

Fe, £0 and Ni hosts, the fields are negative across the

three series, but they increase suddenly at the solutes

Mn, Ru and Os, and remain large for several elements before

returning to the CSP 'base line' (see Figs. 30, 31 and 32). 72) Freeman and ifetson ' have calculated hyperfine fields per

unpaired spin for 3d group, 4d group and 5d group,

H -, = -125 KOe, H,-, = -375 KOe and H^ = -1200 KOe yu. 40. 50.

respectively. They have also shov/n that within 4d elements,

the magnitude of the H, unpaired d-sp-in does not vary

considerably for different elem.ents. This was later on

confirmed by experiments. For diamagnetic atoms the contri­

bution of Core polarization is relatively small.

3. Overlap polarization ; It is a nev; model proposed by

73) Stearns -. The hyperfine field contribution arising from

61

overlap polarization is due to S electron wave functions

in outer shells of the impurity atom overlapping with the

wave functions of the polarized d electrons of the host.

The magnitude of this contribution depends strongly on

the size of the impurity atom. Overlap polarization is

likely to be of considerable importance for impurities

with high valency, where the outer shell is not completely

ionized and there is a remaining density of bound outer

73) shell S-electrons at the impurity site. Stearns ' has

given this possible explanation for the m easured hyperfine

field of solute atoms in Fe.

(iii) The systematics of the hyperfine fields : The

systematics of the hyperfine fields in ferromagnetic hosts

have been studied in detail by Shirley et al. ' . Since

they published their studies on systematics, many more data

have become availableo Our aim is to review the systematics

in the light of more comprehensive data available now. Taking

the values of the hyperfine fields fromx the recently compiled

table , we have plotted the im.purity hyperfine fields in

the host matrices of Fe, C£ . and M respectively in Figs.

•50, 31 and 32. The following systematic trends are clearly

seen,

1) The magnitude of the hyperfine field is proportional to

the magnetic moment of the host matrix.

e. 2

2) The hyperfine field H is negative in 3d, 4d and 5d

impurities in all the three hosts ?e, , M . Exceptions

39 40 40 are in 4d impurities for Y, Zr in ?£ and Zr in _Co.

3) The field increases gradually with the increase in

the d-electrons and reaches a maxim.um value when the d-

shell is approximately half-full. For 3d impurities;, for

example, the field is maximum for Fe in F^, Fe in _Co, and

Mn in M .

In iron host, the field increases gradually for

Ru, Rh and Pd; the maximum value is obtained for Pd in

Fe. However, the reverse trend is clearly seen for the

same impurity m-etals in the other host matrices _Co and M .

4) In the case of 5d impurities, the maximum value of H ^

is obtained at Ir for all the three hosts.

5) For 5p impurities, the field starts with a negative

value when 5p electrons are one or two and gradually

53 reacnes a maximum positive value for I and falls off

to zero and then to a small negative value as the shell

gets fullo

6) In 4f impurities, as we increase gradually the num-her

of 4f electrons;, the field changes from, a negative value

to a largo positive value soffiewhere between Eu and G-d

and then to a large negative value. The curve is very

steep with a large slope.

63

B. THE HYPER.FIWB FIELS AT ^^^Re NUCLEI IN NICKEL LATTICE AT ROOM TEMPERATURE

1. Source Preparation : For the present measurement

pure tungsten metal (99.99^) in pov/der form is sealed in

vacuum in quartz tube and got irradiated with thermal

neutrons in the CIRUS reactor at Trombay (India). Traces

of radioactive tungsten m.etal powder are melted with pure

nickel powder (99.9%) in an argon atmosphere using an

induction furnace. The resulting shltring ball of the

alloy is hammered into a flat disc (thickness less than

0.5 mm); annealed at 850 C for 15 hrs and is gradually

cooled to room temperature,

2. Experimental Set-up : The electronic set up is the

same as described in the magnetic moment measurement

except that a Nal(Tl) scintillator is replaced by a

5.1 cm. X 5.1 cm lead loaded plastic scintillator (covered

by an aluminium cover of sufficient thickness to absorb

p-rays) in stop channel for the detection of 72-keT y-rajs.

It is done to improve the time resolution of the electronics.

The time resolution of this arrangement for the start and

stop channel energy settings respectively at 4-80- and

72-ke? is found to be 1.5 nsec (EWHM) with a slope of

0.24 nsec. An external polarizing field of 2 KOe is

applied perpendicular to the plane of the detectors and

the data are accumulated in a Packard 400 channel analyzer.

64

3. Experimenta?!. Results and Analysis of the Data : The

observed counts in the time sjjectrum ¥(H,t) in the presence

of an external magnetic field H perpendicular to the plane

of the detectors may he v/ritten for the case under study as,

W(H,t)i=: A + B e"*/^ [C Sin (4''-.5-t +0)] (4-1)

The spectra obtained with the magnetic field up (f) and

the magnetic field down (i) have modulations of opposite

phase v/hen the detectors are kept at r35 to each other.

The function R(t) is plotted in Pigo 34. The Larmor

frequency of the oscillations is extracted from the data

using the Fourier transform technique, described by Matthias

52)

and Shirley ^ (see Fig= 35). In this case also the double

Larm or frequency is obtained from the absolute transform

F(<x ) and it is = 184-0 +1.0 M z . The measured Larmor

frequency is related to effective magiietic field through

relation, cr

co^ = - -ifJkl (4-2)

The effective field PI ^ is, thus, calculated from the

experimentally measured g-factor^ The effective magnetic

field,

- eff = "^ext ^"^int ^^'5)

where H -t- is the external polarizing field. The H. ,

is calculated using the sign of the H ^^ and the known

direction of H ,. The hyperfine field

u

c

CN *- o ;=: w o o ^ o o o ^ o

• ^ ;

H rv

S5

u H X w

H

2

00

^ :

o •a;

u o

C fc, fc O

^ . ^

O « H > .'H

:w

O + I

o I

DC

+ 0.3 .--^

>»+0.2

^ 40.1

< 0.0 ^

^ -0.1

I.-0.2 E < -0.3

1 1 . . .^F(Cx))

-

.•••• # • \

• ^ •• A

• A / A ^

- V A A A /

1 1 160 180 200

GJ in MHz

220

F I G . 35 THE FOURIER TRANSFORMS OF R ( t ) FOR

''^'^ReNl IN AN EXTERNAI. POLARIZING

Mi^NETIC FIELD OF 2 KOe.

65

\ f " int - f^ Ms + 471 Ms • D (4-4)

where the second and the third terms on the right hand side

in relation (4-4) are respectively the correction terms

due to the Lorentz field and the demagnetization field.

In the present experiment H , = 2.0 KOe; A-nMs'D = 2.0 KOe

(for the source shape used) according to the tahle given

by Bozorth -. The saturation magnetization 4-%'i'ls for

nickel is 6.08 KOe. 'ihe final value of the hyperfine

field at Re nuclei in nickel matrix at 300 K (room

temp.) is

Hj f (300°K) = -107 + 3 KOe.

C. THE HYPERFIHE FIELD AT ^^Sc NUCLEI IN IRON MATRIX AT ROOM TEMPERATURE

1. Source Preparation : The liquid source, obtained from

NSEC (USA), is evaporated on a thin iron foil (99.99%pure)

which ,is later melted in Argon atmosphere inc ide an induction

furnace and slowly cooled dovm to room temperature. The

resulting shining ball is rolled into a thin foil thickness

less than 0.5 mm and is annealed at 850°C for about 24 hrs.

and then slowly cooled down to room temperature.

2. Experimental Set-up : The electronic set-up is exactly

same as it was used in the magnetic moment measurement of the

68-keV state in Sc discussed in Chapter III. Here a dif­

ferent geometry of the detectors and magnet is used since

66

rough estimates showed tha,t the attenuation of the

amplitude is considerable because of the finite time

resolution of the detectors. The time resolution (PWHM)

of the system for energy gatings around 70 keV is 15 nsec.

The external polarising field is 3 We, . Nuclear data 512

Channel analyzer is used to accumulate the data.

5. Experimental Results and Analysis of the Data : The

time depeiident angular correlation perturbed by the

external magnetic field in S-direction iflay be written as ',

-- _ - 1 -iN'.v.t W (k^, k^. t,H) = :> .V (1) A^ (2) ~j-3- e

rj J k

^ 4^(9^.0j) rl i6^, 0^ (4-5)

This may be simplified to the following form for k<s 2

W (t,H) = 1 + A22 ?2 ^^°^ ®i^ ^9 ^^°^ e2) + 3A22 Sin 0-

X Sin 02 X Cos 0-, • Cos 02 Cos2(>-4t + '^•^-^'i)

+ I A22 Sin^ 0-j_ X Sin^ ©g Cos 2(t t+j -jZf )

(4-6)

where 0-, , 0^, f>^ and jZp are the polar and azimuthal angles

of the two y-^ays respectively. In normal geometry

9 = 0 = 1 but in the present hyperfine field (H- )

measurements 0-1=7 and 0p = 7 — (°^ "j) ^'^^ "^^^ expression

for ¥(H,t) is,

¥(H,t) = I+I/I6A22 ± 3/4 A22 Cos..:5-jt + 3/16 A22 Cos 2<- t

(4-7)

67

v/liere V«'()i,t) is phase shifted hy 180° for the two values

of 9po In the geometry suggested "by Raghavan and Raghavan

the magne-cic field is in the plane of the detectors at 45

to the first detector, while the second detector is placed

successively at 180° and 90° to the first. The normalized

sum and difference in the coinciderce counting rates at

these two angles give the ratio,

R(t) = o^Ml^ll - N (90^)] (4.8) [N(180°) + N (900)]

3/2 A22 Cos -.jj t

1+1/16 A22 + 3/16 A22 Cos 2-j.t

The modulation frequency in this geometry is simply Larmor

frequencyCcV compared to 2 ' in the conventional geometry.

The function R(t) vs time is plotted in Fig. 36. Using

the Fourier transform technique the larmor frequency (ui )

obtained from the ahsolute transform ?(••") ( see Fig. 37) is

= 34.0 + 0.3 MHz. With the help of experimentally knovm

g-factor the value of H r,_p is calculated. The H. , is eiI inx

calculated using the sign of the H^r. and the known

direction of H , ,. The sign of the internal field is

measured by us for the first time. It is obtained from

the known anisotropy of the unperturbed angular correla­

tion and the phase of the sign wave (when the modulated

time spectrum is carefully extrapolated to zero time).

Using the relation (4-4) the value of H, „ is obtained

O:

CO t^ ^ G r^ ^ CO Q O O . O o O

o o o ^ o o o + • + i l l

U

c

E

o|

H.

N;

O

<!

P

ft

H

H

m to >

K H

&4

CO in MHz

FIG. 37 THJB FOURIER TRANSFORMS OF R ( t ) FOR Uk

ScFe IN AN EXTERNAL POLARIZING MAGNETIC F U L D OF 3 KOe.

o c

D O

o r

r c H H

<

H O

o

3

H o

ft a

a

3 P: ^

>

I H O

m

H O

z

^

r

2

a:

c H

O 2

M

?

S 1-

N or;

c

9 M

M Z

>

H

o a N) o o o o o o J — I 1 I I

after appropriate corrections for the lorentz field and

.the demagnetization field. In the present experiment

on ^^Sc Pe H , = 3»00 KOe, An xMs-E = 4.18 (the value — ext 74) of D is obtained from the table of Bozoroth . . The

saturation magnetization Y " MS for iron is 6.97 KOe,,

44 The final value of the hyperfine field at So nuclei

in iron lattice at 300° K is H ^ (300°K) = -94+3 KOe.

D. RESULTS AND DISCUSSION '"-

Our measured values of H, r. at room temperature are

tabulated in Table 7 along with the other available experi­

mental values in literature. Table 7 also gives a view of

H, in ReRi and ScPe systems using various techniques. Our

75)

value is in excellent agreement with Raghavan's ' who has

quoted a value = -105 + 3 KOe. Hov/ever, they used a dif-

ferent geometry ^ of detectors and magnet because the time

resolution of their spectrometer was comparable xvith the

expected time period of the oscillations. 77) Kontani and Itoh ' using spin-echo technique obtained

' int "" ~^^° i ^ ^^^ ^* 4.2°K for the internal field on Re in

Ni matrix. If we presume that the impurity magnetization

follows the Brioullioun function obeyed by the host matrix,

the value of the hyperfine field at room temperature is

expected to be^-5 /^less. Our value is-^10 Ailarger than

the value "reported by Kontani„ It may be probably because

our impurity concentration is low thus reducing the impurity-

69

impurity interactions which would result in a larger field.

The other possible explanation is that the impurity does

not follov/ the host magnetization curve with the possibility

of a localized moment at the impurity.

78) Kogan et ale from their nuclear orientation

experiments have determined the hyperfine field H, on Sc

in Te. Measured to an order of magnitude, they reported a

value of 100 EOe. The nuclear magnetic_resonance studies

of Koi '' gave them a value of 58 KOe. The values reported

by them vary by a factor of 2, Moreover, the M R studies

often contain impurity-impurity interactions because of the

poor sensitivity of the technique. Therefore, we have

measured the hyperfine field using TDPAC technique and it

is = -94 ± 3 KOe. In this technique, the concentration

of the impurity atoms is so small that the impurity-impurity

interactions are completely negligible. 'Eone has measured

the oign of the hyperfine field so far. The determination

of the sign of the hyperfine field on Sc in Pe_ is important

for the studies of the systematics. The -ve sign determined

by us agree with the prediction from the systematics of the

hyperfine fields.

Even though the detailed mechanisms'responsible for

the observed large hyperfine fields on the impurity nuclei

in ferromagnetic hosts are not well understood, the studies

of the systematics of the observed fields show a definite

70

trend as a function of the impurity atomic number. If we

expect a smooth variation of the hyperfine field values

around the So and Re impurities in F£ and Ni respectively,

71) the expected values from the systematics ' (see Pigs. 30-32) are;

\ f "^^ ^ * impurity) |_e = -90 KOe

Fxj ^ Re (5d impurity) Ni = -120 KOe.

which are consistent with our experimental values.

It is often found that the hyperfine fields on

dilute diamagnetic impurity atoms are proportional to the

host magnetic moment. Benski et al."' reported H,

ScNi = 25.9 + 0.3 KOe. Our m-easured value H, ScFe is =

-94 + 3» These values are proportional to the respective

host magnetic moments (ji„. = 0.606 |j.-p, |i-p = 2.22 |J-n).

77)

In the case Rhenium., Kontani et al. " reported

^\f ^eli = -100; % f "eCo = 442; H .. RePe = -760KOe. Our

measurement for Y^^^r. ReNi is in agreement with that of

Konta.ni et al. However, the observed fields are not

proportional to the host magnetic moments (|j . = 0.606 u-g,

[ip = 1.72 iJ,-o, |i-c,,, = 2.22 |i-n). This may .he due to the

formation of localised moments as pointed out in the

earlier part of the discussion, A formal Hamiltonian of the impurity atom is quite

57) complicated and may be written ' ,

71

[:} L(1+1) - k.]?-t - ||[(L"S)(I»I) + (L^I)("I'^)]

the symbols are explained in reference 57,1 The present

measurements on the impurity hyperfine fields were carried

out in cubic matrices and the impurity concentration is

negligibly small and, therefore, the electronic spin

dipole contribution is zero. For the impurities of our

interest ioe., Sc and Re in the ferromagnetic hosts of

Fe and Ni respectively, the orbital contribution to the

impurity hyperfine fields is also small. The main

contribution to the impurity hyperfine fields in ferro-

magnets come from

a) Conduction electron polarization (CEP)

b) Core polarization (CP)

c) Overlap polarization (OP).

The conduction electron polarization arises largely

from the polarization at the nucleut- from the conduction

electrons having an S-character. From the fact that the

conduction band S-electron states are similar to atomic

states near the solute nucleus, it was shown by Shirley,

57) Rosenblum and Matthias ' that,

^CEP " P ns

v/here H i s the f ree atomic hyper f ine f i e l d and p i s t he ns ''•^ ^

72

polarization at the solute, Prom the experimental data

it was derived * ^

H-, r. = 0.027 lxip H for dilute impurities in Pe_

= 0.030 UM H for dilute impurities in Co ^Co ns ^ —

= 0.024 UTIT- H for dilute impurities in Ni ^Wi ns ^ —

so that the predicted values are

\f ScFe = -47 KOe

\f ^eii = -155 KOe

The free atomic hyperfine fields were obtained from

Campbell '.

However, for the transition element impurities,

K . = pH + 2 (S > H. hf •' ns ^ z' d

where Hn is the Core polarisation hyperfine field arising

from, one unpaired d-electron. The calculations of Preeman no or) \

and Watson ' ' showed that

for 3d elements H, x>-.- - 125 KOe per unpaired spin

for 4d elements H, ^ - 375 KOe per unpaired spin

for 5d elements H, - -1200 KOe per unpaired spin

They have also showi that within the 4d elements, the

magnitude of the H, , does not vai-y considerably for dif­

ferent elements. This result was later confirmed by the

experimental results. For diamagnetic atoms, the contri­

bution from the core polarization is small. Since the

73

core polarisation of the d-electrons is always negative,

the sign of the field on Sc iii Ie_ can he explained using

this modelo However, since the magnitude of the d-electron

spin moment on the solute is - 0.3 jig„ The ohse:?ved field

of -107 KOe for Re in lli cannot be explained using this

model.

The observed small field in magnitude compared to

the predicted value from the systema.tics of the core polari­

zation model on ReM may be due to a finite positive field

73) arising from the overlap polarization ' of the host 3d

electrons and the impurity valence electronsc This effect

is expected to be larger in heavier solutes like Re.

In the model due to Campbell ^ the contribution

from conduction electron polarization could be calculated

using the formula

H -gp = A(Z) V^ (0.6 + 0.4 fi/ji )

A(Z) are the free atomic hyperfinc fields and are tabulated

ho)

by Campbell; the host polarization i' =-0.12 S-electrons. y

If we know the host and impurity moments viz., (i. and }i, ,

we can calculate the contribution from Hp-pp.

Balabanov and Delyagin ^ have obtained a very good

fit of the experimental hyperfine fields to an empirical

equation

E/[i = Z^*^ [-2.48 + 0.113 (x)- 9)^]

74

v/here i> i s the number of e lectrons outside the closed'

s h e l l , Z i s the numher of closed she l l e lec t rons and i s 0

equal to 18, 36, 68 for IV, Y and VI group elements» The

values predicted by this model for hyperfine fields of

our interest are H,^ ScPe . + 152 KOe and H, ReM^-304

KOe» In the case ofSc in Pe the predicted value is •-

+152 KOe compared to the experimental value of -94 KOe.

For Re in M the prediction of the sign—of the hyperfine

field is correct but the magnitude is three times the

experimental value. This model is quite empirical with

the result that no plausible explanation for the observed

large deviations may be offered.

It looks that none of the existing models can

correctly explain the observed fields in ScPe and ReNi.

The observed field on ScFe both in magnitude and sign

may be qualitatively explained by the conduction electron

polarization and the core polarization model suggested

by Shirley et al. The field on Re in Ni may be understood

if v/e assume that the conduction electron polarization

and the overlap polarisation are vectorially added to

give the final experimental value. ^

The observed width (P¥HM) for ^^ScPeA-29 x 10~^ eV _q

compared to the natural width of 4.4 x 10 eV is considerably

large. This, discrepancy is attributed to some finite proba­

bility where the Sc atom is not substitutional ^ ith iron

75

matrix. Since the spin of the intermediate state 68-keV

in Sc is 1, the quadrupole interactions are zero.'

Similarly, the observed v/idth (PWHM) for 'ReNl _q

'•../80 X 10 eV" compared to the natural width of 1.25 x

- 9 / \ •

10 eV is also considerably large. This may he, (i) Re

atom is not substitutional to the nickel matrix and (ii)

since the spin of the intermediate state 206-keV in "I on

Re is 5/2, hence there may be quadrupole interactions.

+ CD

0) u ?

03 CD

S CQ

H ;:i CD H •H a

o W Hi pq <a! EH

0 Pi •H ^H ^ 0 ft t> ^

4^ PJ 0 0! (D i4 ft

0)

+ CH

o P! o ra •H fH

ft o o

'xi Q) ^ m •H H rQ p! ft

Q) H ^ C

H •H

> OS

•H ^

CQ 0) O Pi CD PI CD

' ^ CD

CD

o< •H

O CD

H ID

• H

CD Pi •H

^ CD ft >5

M

EH

- P CQ O

W

o

-p

PJ 0

H

76

i n o

o < PH O

c~-! > •

w CO

1 0

CQ 03 0

0 CQ 0 PI

O <J PH

n

a

CO c-

i-q PM s

C7 c~-

p: S ^

H CO

Hi P^ "^

Q) U

CQ 03 0 S

+3

-a f R 0 0 S KJ 0 P

PH

O < i !

PM O

K>

+ 1 Ln O H 1

CM

+ 1 LA O H

1

tS~\

+ 1 [ > O H 1

O r

+ 1 O O H

CO in o

o H

tA

+ -* cn

1

« ft S 0

K> m r\i

0 W

« Hi

O o to

o Hi

r--00 H

o 1 CO

H

'vD <-

LPi

•^ VD < •

o o

•H S

•H S

•H S

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77

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83

PUBLICATIONS

1 "2 "2 "1 Q'7 1 PV

lo Nuclesir L i fe t ime Measurements i n Cs, Au and Re;

D.K. Gupta and G.N. Rao, I I T / K Technical Report 5 / 7 1 ,

March 1971. QQ

2. Nuclear Level S tud ies of Ru; D.K. Gupta et a l . ,

Nuc l . Phys, A180 (1972) 311 . 3 . Nuclear L i fe t ime Measurements of Some Exc i t ed S t a t e s

i n ^hs, 151^3, 133^3, 170.^^^ 187p^^ ^ ^ , 19JZ^„

L,K. Gupta and G.N. Rao, Nucl. Phys„ A182 (1972) 669

Lifetime and Magnetic Moment of 68-keV State in Sc;

D.K. Gupta et al., Proc. Nucl. Phys. and Sol. St.

Phys. Symp., BARC, Bombay (India) U B (1972) 349.

Timing Properties of Ge(Li) Detector (ORTEC Model

8100 - 65 SNo. 67-D); A.K, Singhvi, D.K. Gupta and

G.N. Rao, Proc. Nucl. Phys. and Sol. St, Phys. Symp.

BARC, Bombay (India) liB (1972) 555.

Hyperfine Pield Measurements on Sc in Pe and Re in

Ni; D.K. Gupta et al., IIT/K Technical Report No.

20/72, August 1972, (Under process of Publication

in Phys. Rev. B).