New Detectors for Gamma and Neutron Studiesand Neutron

New Detectors for Gamma New Detectors for Gamma and Neutron Studiesand Neutron Studiesand Neutron Studiesand Neutron Studies

DOE SBIR Phase IIDOE SBIR Phase IIDOE SBIR Phase II DOE SBIR Phase II Kanai Shah, Jarek Glodo, Edgar van Loef, William Higgins,

Rastgo Hawrami, Urmila Shirwadkar, S. Mukhopadhay

Radiation Monitoring Devices, Watertown, MA, USA

www.rmdinc.com

a dynasil member company

Outline

o Requirements for Gamma Ray & Neutron Scintillators

o New elpasolite scintillators -Cs2LiYCl6:Ce (CLYC), Cs2LiLaCl6:Ce (CLLC) & Cs LiLaBr :Ce (CLLB)& Cs2LiLaBr6:Ce (CLLB)

o RMD Corporate Background and C i li tiCommercialization

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Requirements for Gamma & Neutron Scintillators

o High Energy and Timing Resolution

o High Light Yieldo High Light Yield

o High Proportionality

o Fast Response

o Good Spectral Match with Optical Detectors

o Neutron-Gamma Pulse shape and/or Pulse Height Discrimination Capability

o High Efficiency for Gamma-Rays and Neutrons

o Low Costwww.rmdinc.com


o Low Cost

Proportionality and Its Implications

12%

hm) 1.4

8%

10%

@ 6

62 k

eV (f

wh BGO

GSOBaF2

LSOLu3Al5O12:Sc

K L Cl CYAlO3:Ce 1.2

1.3NaI:TlCsI:TlCsI:Na

ht O

utpu

t

2%

4%

6%

gy R

esol

utio

n @ K2LaCl5:Ce CaF2:Eu

NaI:TlCsI:TlYAlO3:Ce

L Cl C

LaBr3:CeRbGd2Br7:Ce

1.0

1.1

Rel

ativ

e Li

gh

0%0 2,000 4,000 6,000 8,000 10,000 12,000 14,000

Ener

g

Luminosity (photoelectrons / MeV)

Theoretical Limit(Counting Statistics)

LaCl3:Ce

0.91 10 100 1000

Electron Energy (keV)

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Gamma Scintillators

Material Light Yield(Photons/MeV)

Emission(λmax, nm)

Energy resolution@662 keV

(R, %)

Non-Proportionality(ΔL, %)

PrincipalDecay Time (s)

(ns)

NaI:Tl 38,000 415 6-7 15 230CsI:Tl 52,000 540 6-7 13 1000LaBr3:Ce 63,000 360 3 10 17Cs2LiYCl6:Ce 20 000 370 4 2 1** 50 ~1000Cs2LiYCl6:Ce 20,000 370 4 2 1 , 50, 1000Cs2LiLaCl6:Ce 35,000 400 3.4 2 1**, 60, 400Cs2LiLaBr6:Ce 60,000 410 3 2 ~ 55, 270

** - for gamma excitation only

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Neutron Scintillators

Material Dopant Emissionnm

Light Yieldph/MeV

Light Yieldph/n

Decayns

PSDp / p /

Li-Glass Ce 395 4,000 6,000 75 N

LiI Eu 470 12,000 50,000 1400 N, ,

LiF/ZnS Ag 450 75,000 160,000 1000, N

CLYC Ce 300*, 390 21,000 70,000 1*, 50, Y, , , , ,1000

CLLC Ce 300*, 400 35,000 110,000 1*, 60,400

Y400

CLLB Ce 410 60,000 180,000 55, 270 Y

* Core Valence Luminescence (CVL)www.rmdinc.com


* Core Valence Luminescence (CVL)

Elpasolites

• High light yieldCs2LiYCl6 High light yield 70,000 to 180,000 ph/neutron; 20,000 to 60,000 ph/MeV

CLYCCs2LiYCl6

• High gamma equivalent >= 3 MeV

CLLCCs2LiLaCl6

• High energy resolution - as high as 3% FWHM @ 662 keV

• Pulse height discrimination

CLLC

Cs2LiLaBr6 • Pulse height discrimination • Pulse shape discrimination• Cubic structure

CLLBCs2LiLaBr6

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• Cubic structure

Summary of properties

Cs2LiLaCl6:CeCLLC

Cs2LiLaBr6:CeCLLB

Cs2LiYCl6:CeCLYC

Density, g/cm3 3.5 4.2 3.3Emission, nm 290CVL,

400Ce3+ 410Ce3+290CVL, 390Ce3+

Decay time, ns 1 CVL,60, 400 55, 270

1 CVL,50, ~1000

Max. light yield, ~ 35,000 ~ 60,000 ~ 20,000ph/MeV

Light yieldph/n

~ 110,000 ~ 180,000 ~ 70,000

GEE, MeV ~3.1 3.2 ~3.1Best ER @662 keV 3.4 2.9 3.9PSD Excellent Possible Excellent

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Cs2LiLaBr6 (CLLB) vs LaBr3 Structure

CLLB - cubic LaBr3 - hexagonal

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Bridgman Grown Crystals

1 in CLYC

eM

elt z

one

zone

1 in

olid

ifica

tion

CLLC CLLB

So 2 in CLYC

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Scintillation Characteristics1 5

1.0

1.5

CVL

gamma

rb. u

nits

1.0

1.2

Ce3+

CLYC

its

0.5 Ce3+ prompt

Ce3+ STE

inte

nsity

, ar

0 4

0.6

0.8 prompt & STE

nsity

, arb

. un

1.2 neutron

0 200 400 600 800 10000.0

time, ns

250 300 350 400 450 5000.0

0.2

0.4

CVLinte

n

0.6

0.8

1.0 Ce3+ STE

neutron

y, a

rb. u

nits

250 300 350 400 450 500

wavelength, nm

CVL Core Valence L minescence0 200 400 600 800 10000.0

0.2

0.4

inte

nsity

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CVL - Core Valence LuminescenceSTE - Self Trapped Excitons

0 200 400 600 800 1000

time, ns

Proportionality of Elpasolites

1.10

1.05

1.10yi

eld

1.00 NaI:Tlve

ligh

t y

0 90

0.95 CLYC:Ce CLLC:Ce CNLI:Ce CLLB:CeLaBr :Ce

rela

tiv

10 100 1000

0.90 LaBr3:Ce

energy, keV

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gy

Energy Resolution of Elpasolites

2

units

7%NaI:Tl

CLYC:Ce

CLLC:Ce

nsity

, arb

. 7%

3.9%

3.4%

1CNLI:Ce

CLLB:Ce

C

inte

n

3.4%

2.9%

2 9%

200 300 400 500 600 700 800

LaBr3:Ce

energy, keV

2.9%

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Thermal Neutron Detection

6neutron

CLYC

0

2

4

E=4.5%

662 keV 137Cs Am/Be 3500 keV

ts

o High Gamma EE

1

2

3

E=3.4%sity

, arb

. uni

662 keV 3100 keV

CLLC

o High energy resolution

o Single full energy peak

2

3662 keV

CLLB

0

inte

ns

g gy p

o PHD

0 1000 2000 30000

1 E=3.0% 3200 keV

gamma equivalent energy, keV

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Pulse Shape Discrimination – overview

CLYC CLLC CLLB

60 CLYC

1 0

1.2

CLLC 100

CLLB

20

40

neutron gamma

inte

nsity

0 2

0.4

0.6

0.8

1.0 neutron gamma

inte

nsity

, arb

. uni

ts

10-1

CLLB neutron gamma

nten

sity

, arb

. uni

ts

0.0 0.5 1.0 1.5 2.0 2.5 3.00

time, s 0 200 400 600 800 1000

0.0

0.2

time 0 500 1000 1500 2000

10-2

in

time, ns

180

200CLYC #48a-01P / R980

160

18023513

0.55

60

80

100

120

140

160

180

3672

66552

ndow

2 /

win

dow

1

60

80

100

120

140

160

5239

neutron gamma

ndow

2 /

win

dow

1

0 40

0.45

0.50

neutron gamma

dow

2 /

win

dow

1

0 20 40 60 80 100 120 140 160 180 2000

20

40total

179786

neutron gamma

full integral

win

0 20 40 60 80 100 120 140 160 180 2000

20

40 5239total

99549

CLLC #24-1 in slice / R2059

full integral

win

10000 20000 30000 40000 500000.35

0.40CLLB #16 / R2059total: 7150 ctsneutron: 2008 ctsgamma (1): 120 cts

window 1

win

Fi 4 G /N l h di i i i (PSD) l f CLYC CLLC d CLLB Th

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PSD, CLYC Ø1 inch x 15 mm sample, 95% 6Li

140

160

180

200

34318

CLYC #48a-01P / R980

ow 1 N

20

40

60

80

100

120

win

dow

2 /

win

do

180

200CLYC #48a-01P / R980

0 20 40 60 80 100 120 140 160 180 2000

20116839

window 1

Na

80

100

120

140

160

18035

w 2

/ w

indo

w 1

0 20 40 60 80 100 120 140 160 180 2000

20

40

60

43312

window 1

win

dow

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do

CLYC: 6Li vs. natLi

2 0

1.5

2.0

>95% 6Li

CLYC:Ce 3.4 MeVAm/Be Spectra

c/gr

am

1.0

coun

ts/s

ec

Enrichment significantly improves detection of

th l t

0 0

0.57% 6Li (natural)

477 keV 3.3 MeVinte

nsity

, thermal neutrons.

0.0 0.5 1.0 1.5 2.0 2.5 3.0 3.50.0

energy, MeV

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Potential Applications

o Nuclear & particle physics research

o Homeland securityy

o Neutron diffraction

o Oil well logging

o Nuclear waste characterizationo uc ea aste c a acte at o

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RMD Corporate Background & Commercialization Historyy

Founded in 1974, now part of Dynasil Family 80 Research Staff 40 Ph.D. & 11 M.S. 45,000 ft2 lab & manufacturing space Clean rooms Full digital machine shop

In house prototyping & production In-house prototyping & production

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RMD - Products Overview

64-elem ent APD Array13m m x 13m m Si APDCZT Arrays

CdTe Detectors CsI Im aging ScreensLPA-1 Lead-in-Paint Analyzer

RadCam 2000TM Portable RadCam 2000TM Im ageNavigatorTM Surgical Probe

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G am m a/Video Im agerg g

Dynasil/RMD Scintillator CommercializationCommercialization

• Varied strategies employed for commercialization of scintillators funded by DOE SBIR NP Program.

• CeBr3 a licensing agreement has been executed with a large companyCeBr3, a licensing agreement has been executed with a large company, production is expected to begin next year• CLYC and related compositions, RMD is establishing a pilot-line in a Phase III program.

D il tl i d Hil C t l ith ifi i f• Dynasil recently acquired Hilger Crystals with a specific aim of commercializing RMD’s very active scintillator research. Hilger has been commercializing scintillators over several decades.

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Acknowledgements

We gratefully acknowledge the support provided by the US Department of Energy

(DOE)

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Documents

New Detectors for Gamma and Neutron Studiesand Neutron