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  • 8/11/2019 Applications of Liquid Scintillation Counters-6bl

    1/5

    IRE

    TRANSACTIONS ON

    NUCLEAR

    SCIENCE

    ANTHRACENE

    ,,..LIGHT

    PIPE

    RADIOACTIVE

    SPECIMEN

    -GLASS

    MOUNT

    Fig.

    9-Counting

    geometry for

    3- y

    coincidence

    polarized

    nuclei.

    experiments

    with

    4C

    f>

    3u

    L2

    25

    0

    o

    20

    .4

    5

    0

    0.2

    3 0.4

    015 a6

    07

    0.8

    9 1.0

    YC

    Fig.

    10-Original electron

    emission

    angle

    necessary for

    central

    detection

    in

    3-y

    coincidence

    experiments.

    Fig.

    11--sy

    coincidence

    apparatus.

    dences

    between

    electrons

    above

    a

    certain

    energy and

    the

    desired

    gamma

    rays striking

    each

    pair

    of

    gamma

    counters

    are

    recorded,

    as well

    as all

    individual

    counting rates.

    The

    fifth

    gamma

    counter is used

    to

    determine the

    degree of

    nuclear

    polarization

    as

    before.

    As can

    be

    seen

    from

    the

    photograph,

    the

    geometry

    is

    rather tight, so

    that

    correc-

    tions

    for

    angular

    resolution must be

    made.

    Further

    experiments

    with

    this

    type

    of

    apparatus

    are

    in

    progress,

    and

    some changes in

    technique

    are

    being

    planned.

    In

    particular,

    use of

    some of

    the new

    photo-

    multipliers

    which

    can be

    operated

    at

    low

    temperatures

    should

    materially

    reduce

    heat

    leaks

    which are

    troublesome

    with

    the

    presently

    used

    light

    pipe.

    Applications of

    Liquid

    Scintillation

    Counters*

    F.

    NEWTON

    HAYESt

    Summary-The liquid

    scintillator,

    in

    just

    a

    few

    years of de-

    velopment,

    has shown

    itself to

    be

    an extremely

    versatile

    chemical

    system fo r

    radiation

    detection. Its

    evolution has

    been

    characterized

    by

    penetration

    into

    almost

    every

    phase

    of

    experimental

    science.

    A

    survey of the

    most

    notable

    applications of liquid

    scintillation

    counting is

    presented.

    *

    Manuscript

    received by

    the

    PGNS,

    February

    8, 1958. This

    work

    was

    performed under the

    auspices of the

    U. S.

    Atomic

    Energy

    Commission

    t

    Los Alamos

    Sci.

    Lab.

    University

    of

    California,

    Los

    Alamos,

    N

    M

    OWARD

    the end of

    August,

    1957,

    at

    Northwestern

    University,

    Evanston,

    Ill.,

    a

    three-day

    conference on

    liquid

    scintillation

    counting

    was held.'

    There

    were

    sessions

    on

    physics

    and

    chemistry

    of the

    liquid

    scintillator,

    on

    instrumentation for

    liquid

    scintillation

    counters,

    and

    on

    applications

    of

    liquid

    scintillation

    counting.

    Much

    of

    I

    Proceedings of

    the Northwestern

    University

    Conference

    on

    Liquid

    Scintillation

    Counting, to

    be

    published

    by

    Pergamon

    Press Ltd.,

    London,

    Eng.

    351

    45

    166

    December

    AlultIXDoM1a1UfIX Ra

  • 8/11/2019 Applications of Liquid Scintillation Counters-6bl

    2/5

    Hayes:

    Applications

    of Liquid Scintillation

    Counters

    th e

    information

    in

    this

    paper

    has been

    drawn from

    the

    Proceedings

    of

    this

    conference.

    A

    liquid

    scintillator2

    is

    usually

    a

    three-component

    system

    composed

    of

    solvent,

    primary

    solute,

    and

    secondary

    solute.

    An

    energy transfer

    sequence

    proceeds

    from

    solvent

    to

    primary

    solute,

    at which

    point

    the

    process

    has

    realized

    about

    3

    per

    cent

    energy

    efficiency,

    and

    energy

    states

    are

    attained

    which

    allow emission

    in

    the

    350

    to

    400

    m,u

    range.

    However, photon

    emission is

    delayed

    until

    energy

    is

    transferred

    to

    the

    secondary

    solute.

    The

    quantum effi-

    ciency of this

    last

    step

    in

    the transfer is about

    1,

    and

    the

    photon

    emission is

    mostly

    in the

    range

    420

    to 480

    m,u.3

    Such

    a

    spectrum

    of

    photons

    has considerable

    mean-free-

    path

    in

    th e

    scintillator and has a

    high

    matching

    factor

    to

    the

    sensitivity

    spectrum

    of

    a

    photomultiplier

    cathode.

    Toluene

    is

    often

    an excellent

    choice

    as

    a

    solvent4

    because

    it is

    efficient, cheap,

    and

    commercially

    available

    in

    requisite

    purity.

    In situations

    where

    its

    fire

    hazard

    and

    toxicity

    become

    important

    considerations,

    th e

    less

    volatile

    solvents

    triethylbenzene

    or

    isopropylbiphenyl5

    may be

    used.

    The

    solvent

    combination

    of

    p-dioxane

    and

    naphthalene

    is

    very

    useful6

    when water must

    be

    dissolved

    in

    the

    liquid

    scintillator.

    The most

    popular

    primary

    solutes7 are

    p-terphenyl,

    2,5-diphenyloxazole

    (often

    referred to

    as

    PPO)

    and

    2-(4-biphenylyl)-5-phenyl-1, 3,

    4-oxadiazole

    (sometimes

    called

    PBD).

    Today s

    most

    useful

    secondary

    solutess

    are

    2,5-p-phenyl-

    ene-bis(5-phenyloxazole) (almost

    always

    referred

    to

    as

    POPOP and

    9,10-diphenylanthracene.

    For

    the

    last five

    years

    the

    most

    popular

    liquid

    scintillator

    has

    been

    composed

    of

    toluene,

    p-terphenyl,

    and a

    secondary

    solute.

    There

    ar e

    no

    unequivocal

    optima

    in

    solute

    con-

    centrations9

    where

    economy

    is

    the

    natural

    antagonist

    of

    performance.

    A

    solution of 5

    g/1

    p-terphenyl

    and 0. 5

    g/ 1

    POPOP

    in

    toluene

    is

    now

    considered

    to be

    a

    superior liquid

    scintillator

    over

    the million-fold

    range

    in

    volume

    found

    in

    liquid

    scintillation detectors.

    This

    solution

    yields

    about

    8

    photons,

    air-saturated,

    or

    10

    photons,

    inert-gas

    saturated,

    per

    kev

    deposited

    by

    an

    exciting particle

    at

    minimum

    2

    F.

    N.

    Hayes,

    Liquid scintillators:

    attributes and

    applications,

    Intern.

    J.

    Appl.

    Radiation

    and

    Isotopes,

    vol.

    1,

    pp . 46-56;

    July,

    1956.

    3

    D.

    G.

    Ott,

    F.

    N.

    Hayes,

    E.

    Hansbury,

    and

    V.

    N.

    Kerr, Liquid

    scintillators.

    V.

    Adsorption and

    fluorescence

    spectra

    of

    2,5-diaryloxa-

    zoles and

    related

    compounds,

    Am.

    Chem.

    Soc.,

    vol.

    79, pp .

    5448-

    5454;

    October,

    1957.

    4

    F. N.

    Hayes, B. S.

    Rogers,

    and P.

    C.

    Sanders,

    Importance

    of

    solvent in

    liquid

    scintillators,

    Nucleonics,

    vol.

    13, pp .

    46-48;

    January,

    1955.

    5

    W.

    L.

    Buck

    and R. K.

    Swank,

    Use

    of

    isopropylbiphenyl as

    solvent in

    liquid

    scintillators,

    Rev.

    Sci.

    Instr., vol.

    29, p.

    252;

    March,

    1958.

    6

    W. H.

    Langham, W. J.

    Eversole,

    F.

    N.

    Hayes,

    and

    T.

    T.

    Trujillo,

    Assay

    of

    tritium

    activity

    in

    body fluids

    with use

    of

    a

    liquid

    scintillation

    system,

    J.

    Lab.

    Clin.

    Med., vol.

    47,

    pp .

    819-825;

    May,

    1956.-

    7F.

    N.

    Hayes,

    D.

    G.

    Ott, V.

    N.

    Kerr,

    and

    B.

    S.

    Rogers,

    Pulse

    height

    comparison of

    primary

    solutes,

    Nucleonics,

    vol. 13, pp .

    38-41;

    December,

    1955.

    8

    F.

    N.

    Hayes,

    D.

    G.

    Ott,

    and V. N.

    Kerr,

    Pulse-height

    com-

    parison

    of

    secondary

    solutes,

    Nuicleonics,

    vol.

    14,

    pp . 42-45;

    January, 1956.

    D.

    G. Ott,

    see

    footnote 1.

    ionization. A

    liquid

    scintillator

    responds

    to

    th e

    densely

    ionizing

    5-mev

    alpha

    particle

    as

    though

    it

    were

    a

    0.5-mev

    electron.

    The

    liquid

    scintillator is a

    member of

    th e

    organic

    scintillator

    family

    which

    also

    includes

    crystals, plastics

    and

    gels.

    It

    has

    certain

    useful

    properties

    which

    clearly

    differentiate

    it

    from its

    organic relatives,

    as

    well as

    from

    inorganic-crystal

    and

    noble-gas

    scintillators.

    These

    are:

    low

    cost,

    ease

    of

    preparation,

    high transparency,

    short

    decay

    time,

    absence

    of

    self-dictated size

    limitation,

    and

    ease

    of

    alteration.

    The 5

    g/1 p-terphenyl

    and

    0.5

    g/1

    POPOP

    solution

    in

    toluene

    has

    a

    materials

    cost of

    about

    2.80/1.,

    and

    it s

    preparation

    time is

    the

    short

    time

    required

    through

    heating

    and/or stirring

    to

    dissolve

    the

    solutes in

    th e

    solvent. This

    solution

    has

    an

    average mean-free-path

    for

    its

    emitted

    light

    of th e

    order

    of 10

    meters,

    and

    it s

    decay

    time is

  • 8/11/2019 Applications of Liquid Scintillation Counters-6bl

    3/5

    IRE

    TRANSACTIONS

    ON NUCLEAR SCIENCE

    SMALL-VOLUME

    INTERNAL-SAMPLE

    COUNTING

    Since

    1951,

    small-volume liquid scintillation

    counters

    have

    been used for beta-counting

    of

    isotopically

    labeled

    organic compounds

    found

    especially

    in biological,

    chemical,

    and

    industrial

    research.

    Historically,

    the

    simplest case

    in

    the

    chemistry

    of

    this

    detector

    was developed

    first.

    Gaseous, 2

    3

    liquid

    and

    solid

    compounds

    soluble in

    toluene

    were

    dissolved

    directly in

    the

    liquid

    scintillator

    and,

    for C' 4

    and higher energy

    beta

    emitters, counting

    effi-

    ciencies

    from 50

    to

    100 per

    cent

    were

    obtained. This

    represented

    improvement

    over

    Geiger

    and ionization

    chamber

    measurements

    in that

    sample

    processing

    was

    kept

    to a

    minimum,

    thereby

    allowing

    considerable

    saving

    in

    the

    over-all

    assay time.

    Such

    considerations

    as correc-

    tions

    for

    self-absorption

    and geometry

    disappeared since

    the

    dissolution

    of

    the sample

    makes

    it

    infinitely

    thin

    throughout

    the

    detector and

    gives

    it a

    47r

    geometry.

    Especially

    for liquid and

    solid

    samples, the

    liquid

    scin-

    tillation

    method

    offers

    a

    considerable

    chance for high

    sensitivity.

    Guinn has made

    comparisons

    with

    thin-

    window

    Geiger

    counting

    of

    minimum specific

    activity

    detectable

    to I10

    per cent

    standard deviation

    in

    30-

    minute sample

    counting

    time and

    30-minute background

    counting time.

    He

    finds

    that the liquid

    scintillation

    counter

    may yield

    higher

    concentration sensitivity by

    the

    following

    factors:

    7,800

    fo r

    H3,

    1,000

    fo r

    C'4,

    870

    for

    S33,

    156

    fo r

    Cl36, and

    60

    fo r p32.

    Guinn

    quotes

    counting

    ef-

    ficiencies

    of 25

    per

    cent

    for

    H3,

    75

    per

    cent

    fo r

    C14,

    and

    100 per

    cent fo r

    p32.

    Many

    workers

    have

    reported

    successful

    routine

    analyses

    of

    binary

    and

    ternary

    mixtures

    of

    beta-emitting isotopes.

    This

    takes advantage

    of

    the

    energy

    dependence

    of

    light

    output

    from

    a

    liquid

    scintillator.

    Some

    examples

    are

    H3-C14,

    H3-Na22,

    and H3_C'4_p32.

    For

    compounds

    insoluble

    in

    toluene,

    two variants

    in

    the

    scintillator system

    have been

    developed.

    The

    first

    is

    effecting

    a

    solution

    of the

    sample

    without

    seriously

    impairing

    the scintillating

    action

    of the

    solution,

    an d

    the

    second

    is

    dispersal

    of

    the insoluble

    sample

    in

    a

    finely

    divided

    state

    throughout

    the

    scintillator.

    The

    first

    method

    can

    be

    accomplished

    by

    use of

    the

    water-miscible

    solvent

    systems,

    p-dioxane

    and

    naphthalene

    or

    toluene

    and

    ethanol,

    or

    by

    chemical treatment

    of the

    sample

    to

    make

    it

    soluble

    in

    toluene.14

    5

    The

    second method

    was

    first

    tried

    with

    no

    suspending

    agent'6

    and

    then with

    agents

    11

    M.

    S.

    Raben

    an d

    N.

    Bloembergen,

    ' Determination

    of

    radio-

    activity

    by

    solution

    in

    a

    liquid scintillator,

    Science,

    vol.

    114, pp.

    363-364; October,

    1951.

    12

    B. N.

    Audric

    an d

    J.

    V. P.

    Long,

    Use of

    dissolved

    acetylene

    in

    liquid

    scintillation

    counters for the measurement

    of

    carbon-14

    of

    low specific

    activity, Nature,

    vol.

    173,

    pp.

    992-993;

    May,

    1954.

    13

    G.

    W.

    Barendsen,

    Radiocarbon

    dating

    with

    liquid

    CO2

    as

    diluent

    in

    a

    scintillation

    solution,

    Rev. Sci.

    Instr.,

    vol.

    28,

    pp.

    430-432;

    June,

    1957.

    N.

    S.

    Radin,

    see footnote

    1.

    J.

    M.

    Passman,

    N. S.

    Radin,

    and J.

    A.

    D.

    Cooper,

    Liquid

    scintillation

    technique

    for

    measuring

    carbon-14-dioxide

    activity,

    Anal.

    Chem.,

    vol.

    28, pp.

    484-486; April,

    1956.

    18

    F.

    N.

    Hayes,

    B. S.

    Rogers,

    and

    W. H.

    Langham,

    Counting

    suspensions

    in

    liquid

    scintillators,

    Nucleonics,

    vol.

    14,

    pp.

    48-51;

    March,

    1956.

    which

    yield

    rigid

    gels17 or

    thixotropic

    solutions. 8 9

    A

    very

    satisfactory

    new

    suspension

    procedure

    20

    is

    the use

    of

    a 25 per

    cent solution

    of

    polystyrene in

    a

    toluene-

    solvent liquid

    scintillator.

    This gives

    a transparent

    solution

    viscous

    enough

    to

    support suspended

    matter

    during

    reasonable

    counting

    times

    but

    fluid

    enough

    to

    allow

    further

    addition after

    the original

    counting

    period of a

    substance

    which can

    serve

    as

    an

    internal

    standard

    fo r

    efficiency

    calibration. The

    specific

    application

    of this

    procedure

    has involved

    samples

    of 10 g of ashed

    and

    powdered

    bone in

    15

    ml

    of the

    viscous

    scintillator

    from

    which

    bone sample

    assays

    as

    low as 10 Sr90

    d/min/g

    can

    be determined.

    Quenching2

    of

    th e

    scintillation

    process and

    absorption

    of th e

    emitted light

    may be corrected

    for,

    in

    homogeneous

    systems,

    by

    use of

    soluble internal

    standards.2 22

    Electronics

    for

    small-volume

    internal-sample

    liquid

    scintillation

    counting

    has been

    distinguished

    by

    having

    either one photomultiplier

    in

    a single

    channel

    circuit2326

    or

    two

    photomultipliers

    in coincidence.27 28

    The com-

    plexity

    of

    th e

    coincidence-type

    circuitry

    is

    required,

    with

    the

    present

    state

    of

    photomultiplier

    development, for

    counting

    applications

    with

    low-energy

    beta

    emitters

    wherein great

    sensitivity

    is

    required. That

    Pringle29 30

    has

    accomplished

    single channel

    counting of

    natural-C'4

    for

    dating

    of archaeological

    specimens

    as

    old as 38,500

    years

    with

    i9 per

    cent

    precision,

    is a

    tribute

    to his

    complete

    coordination

    of

    optimization

    in effectiveness

    of

    shielding,

    elimination

    of electrical

    noise,

    selection

    of

    a

    photomultiplier

    with

    a

    low

    noise

    to

    gain

    ratio, and

    use of

    a

    scintillator

    system

    with

    high

    photon

    yield.

    Nir' has

    reported

    on

    liquid

    scintillation

    counting of

    natural tritium

    and

    its

    applications

    to

    hydrology

    and

    B. L.

    Funt and

    A.

    Hetherington,

    Suspension counting

    of

    carbon-14

    in

    scintillating gels,

    Science,

    vol.

    125,

    pp. 986-987;

    May,

    1957.

    18

    S. Helf,

    see footnote

    1.

    C.

    C.

    White

    and

    S.

    Helf,

    Suspension

    counting

    in

    scintillating

    gels,

    Nucleonics,

    vol.

    14, pp .

    46-49;

    October, 1956.

    20

    H. Foreman, se e

    footnote

    1.

    21

    V.

    N.

    Kerr,

    F.

    N.

    Hayes,

    and D.

    G.

    Ott,

    Liquid

    scintillators.

    III.

    Th e

    quenching

    of

    liquid-scintillator

    solutions

    by organic

    com-

    pounds,

    Intern.

    J. Appl.

    Radiation

    and ISotopes, vol.

    1, pp .

    284-

    288; January,

    1957.

    22

    D. L. Williams,

    F.

    N.

    Hayes,

    R. J.

    Kandel,

    and

    W.

    H.

    Rogers,

    Preparation

    of C14

    standard

    for

    liquid

    scintillation

    counters,

    Nucleonics,

    vol.

    14,

    pp .

    62-64;

    January,

    1956.

    23

    B.

    Gordon

    and

    T. S.

    Hodgson,

    se e

    footnote

    1.

    24

    E.

    C.

    Farmer

    and

    I.

    A.

    Berstein,

    Determination

    of

    specific

    activities of

    C'4-labeled

    organic

    compounds

    with

    a

    water-soluble

    liquid

    scintillator, Science,

    vol.

    1 15, p p.

    460-461;

    April,

    1952.

    25

    D. J. Rosenthal

    and

    H. 0.

    Anger,

    Liquid

    scintillation

    count-

    in g

    of

    tritium

    and C 4-labeled

    compounds,

    Rev. Sci.

    Instr.,

    vol.

    25,

    pp .

    670-674;

    July,

    1954.

    26

    J.

    C.

    Roucayrol

    and

    E.

    Oberhausen,

    Measurement

    of

    activity

    of

    compounds

    traced

    with

    low-energy

    beta

    emitters,

    Science,

    vol.

    122,

    pp .

    201-202;

    July,

    1955.

    27

    R.

    D. Hiebert

    and

    R.

    J.

    Watts,

    Fast-coincidence

    circuit

    for

    H3

    and

    C'4 measurements,

    Nucleonics,

    vol.

    11,

    pp . 38-41;

    Decem-

    ber,

    1953.

    28

    F.

    N.

    Hayes

    and

    D.

    G.

    Ott,

    Los Alamos

    Doc.,

    LA-2095; 1957.

    29

    R.

    W.

    Pringle,

    W.

    Turchinetz,

    and

    B. L.

    Funt,

    Liquid

    scintil-

    lation techniques

    for

    radiocarbon dating,

    Rev.

    Sci.

    Instr.,

    vol.

    26,

    pp.

    859-865-

    September,

    1955.

    B

    Fn adS

    Dnlk

    0

    R.

    W.

    Pringle,

    W.

    Turchinetz,

    B. L. Funt,

    and S.

    S.

    Danyluk,

    Radiocarbon

    age

    estimates

    obtained

    by

    an

    improved

    liquid

    scintil-

    lation

    technique, Science,

    vol.

    125,

    pp .

    69-70;

    January,

    1957.

    168

    December

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    Hayes: Applications

    of

    Liquid Scintillation

    Counters

    meteorology.

    He

    has

    enriched the

    natural tritium

    in

    water

    from

    rain,

    ground

    water,

    and

    lakes,

    and

    has

    ex -

    changed

    the resultant water with

    toluene under

    acid

    catalysis. After this

    treatment,

    25

    per

    cent

    of

    the

    original

    tritium resided in the toluene.

    With this

    toluene as

    the

    solvent

    of

    a

    liquid

    scintillation

    counter,

    operating

    at

    -70C in

    coincidence,

    a

    limiting

    sensitivity

    of

    one

    tritium

    atom

    in 1018

    hydrogen

    atoms

    was

    realized.

    The

    counting

    efficiency

    for

    tritium

    was

    45

    per

    cent.

    Bell

    has

    used

    liquid

    scintillation

    counting

    of

    tritium

    in

    tritium-labeled water

    because

    of its

    ready

    applicability,

    both

    to

    great

    numbers

    of

    samples

    and

    to

    realization

    of

    high

    sensitivity.

    He

    has carried

    out

    experiments

    on

    model

    as

    well as actual

    rivers,

    assaying

    tritium

    activity

    vs

    time

    and position

    relative

    to the

    point

    of

    entry

    of

    the

    original

    labeled

    water

    sample.

    Guinn'

    has

    quoted

    some industrial

    applications

    of

    small-

    volume,

    internal-sample

    liquid

    scintillation

    counting

    in

    industrial research.

    Examples

    are:

    tritium

    counting

    of

    exhaust water after

    use of tritium-labeled

    lubricating

    oi l

    to

    follow

    the

    rate

    of

    combustion

    of

    such

    oils

    in

    operating

    engines,

    C' 4

    counting

    to

    determine the

    stability

    of

    a

    fuel

    oil

    additive

    in

    long-term

    storage,

    S35

    counting

    to

    estimate

    the

    exchange

    of

    hydrogen

    sulfide

    with

    sulfur

    atoms

    in

    metal

    sulfide

    catalysts,

    and

    p3 2

    counting

    to

    study

    entrain-

    ment

    in

    aqueous

    large-scale

    distillation

    columns

    with

    P32-labeled

    phosphoric

    acid

    as a

    nonvolatile

    tracer.

    Langham

    has reported

    on

    th e

    small-volume,

    internal-

    sample liquid

    scintillation

    counting

    of

    H3,

    C 4,

    Na22,

    S35,

    Ca45

    5r90 j131

    CS134,

    CS137,

    U233,

    U235,

    and Pu239,

    i

    various chemical

    forms,

    as

    a

    part

    of a

    biological

    and

    medical research

    program.

    As an

    example

    of

    part

    of

    th e

    tritium applications,

    counting

    of

    tritium

    water

    which

    appears

    in

    the

    blood

    and

    urine

    of a

    person

    after

    ingestion

    has

    led

    to such

    physiological

    data

    for

    that

    person

    as

    gastric

    hold-up

    time, equilibrium time

    between

    gas-

    trointestinal

    tract and

    blood,

    equilibrium time

    between

    blood and total

    body fluids,

    total

    body

    water,

    rate of

    turn-over

    of

    body

    water, per

    cent lean

    body

    mass,

    and

    per

    cent

    gross

    body

    fat. Another

    similar

    and

    quite

    practical

    applications of

    tritium

    water

    counting

    is

    th e

    on-the-hoof

    determination

    of

    per

    cent

    body

    fat

    in

    a

    steer.

    Roucayroll

    in

    France

    has taken

    paper

    chromatograms

    of

    C'4,

    1131,

    and

    P32-labeled

    compounds, has

    wet

    th e papers

    with

    a

    liquid

    scintillator,

    and

    has

    then

    scanned them

    with

    a

    single

    photomultiplier.

    Special

    techniques

    have

    been

    developed fo r

    handling

    toluene-soluble,

    as

    well

    as

    toluene-

    insoluble,

    compounds.

    Arnold

    3

    has

    been able to

    effect

    very

    sensitive counting

    of

    natural

    C'4

    in

    a

    100-ml

    scintillator

    solution,

    whose sol-

    vent

    is a

    mixture of

    hexane

    and octane

    equivalent

    to

    47

    g

    of

    carbon.

    The

    solvent was

    prepared

    in the

    sequence:

    sample,

    carbon

    dioxide,

    acetylene,

    the

    6-carbon

    and

    8-carbon

    polymers of

    acetylene,

    and

    hexane

    and octane.

    Baranov,

    Goldanskii

    and

    Roganov32

    in

    Moscow

    have

    made

    a

    high-energy

    neutron

    dosimeter

    from

    a 70-ml

    volume of

    a

    liquid

    scintillator

    which

    serves both as

    a

    source

    of

    carbon

    and

    as

    a

    detector of C

    disintegration

    positrons.

    The C

    results

    from the

    C'2(n,

    2n)C reaction

    which has

    a

    20.6-mev

    threshold.

    The useful

    range of the

    dosimeter

    is

    from 40 to

    400

    mev.

    LARGE-VOLUME

    EXTERNAL-SAMPLE COUNTING

    The

    large liquid

    scintillation

    counter is

    usually

    more

    notable

    for the

    large

    number of

    photomultipliers used

    than

    for

    th e

    large

    volume

    of

    liquid,

    since

    many

    2-inch

    cathodes

    are

    required

    in

    a

    large

    counter to

    allow even

    a

    small fraction

    of

    the

    inner surface

    to

    be

    photosensitive.

    It is common

    practice

    to

    furnish

    the remainder

    of

    the

    inner

    surface

    with a

    diffuse

    reflector

    whose index

    of

    refraction is

    higher than that

    of the scintillator

    which

    bathes

    it.

    An interesting

    difference

    between

    the

    small and

    large

    scintillation

    counters involves

    the lifetime

    of a

    solution

    used

    in

    filling

    the

    counter.

    This time

    is

    usually

    quite

    short

    with

    the

    small

    counters,

    since the solution

    is

    asso-

    ciated with

    only

    one

    counting

    sample and must be

    replaced

    by

    a

    new

    solution when

    th e next

    assay

    is

    run.

    The labora-

    tory

    in which 100

    analyses a

    day ar e

    run,

    using

    25

    cm3

    of scintillator

    for each

    sample,

    will

    use up 2.5

    liters

    in

    such

    a

    day.

    In 120

    such

    days, the total

    volume used

    will

    equal

    the 0.3

    m3

    volume

    of

    the oft-termed

    giant

    liquid

    scintillation

    detector

    used

    in the 1953 search

    fo r

    th e

    free

    neutrino.

    Whereas

    the small

    detector

    is

    continuously

    being

    refilled, th e

    large detector

    filling

    tends to

    stay put.

    This

    introduces

    an

    important

    question

    for

    large

    detectors

    as

    to aging

    of a

    liquid

    scintillator.

    A

    specific quotable

    case

    involves a

    Los

    Alamos

    counter

    whose

    p-terphenyl-aNPO-

    toluene

    filling after 3'

    years

    still

    had 0.86 of

    its

    original

    pulse height. A loss

    in

    efficiency

    on

    standing

    in a

    detector

    may arise

    from

    leaching of

    trace

    materials

    from the

    reflector, the

    container,

    cement,

    or

    0-rings,

    or

    from

    chemical

    action

    of

    dissolved

    oxygen

    on

    th e

    scintillator

    components.

    It

    seems to

    be

    important

    in the use

    of

    triethylbenzene

    in

    a

    large counter

    to

    replace the

    dissolved

    and free air

    in the

    counter

    with an

    inert gas

    such as

    argon.

    A

    fascinating

    property

    of

    large-volume

    liquid

    scintilla-

    tion

    detectors

    which

    have

    good light

    collection

    efficiency

    is

    their

    ability to

    give

    sharp energy

    resolution

    for

    energetic

    gamma

    rays.

    The

    dimensions

    of

    the

    detector allow

    an

    entering

    gamma

    ray

    to

    impart

    essentially

    al l of

    its energy

    to

    the

    scintillator by

    multiple

    Compton

    scattering.

    A

    0.06 m3

    square

    cylindrical

    detector8 with

    about 4 per

    cent

    of

    it s

    internal

    surface

    photosensitive

    and

    with an

    internal

    titanium

    dioxide

    reflector gave

    about

    13.5 per

    cent

    resolu-

    tion

    (full

    width at half

    maximum)

    for

    4.43-mev

    gammas

    from

    excited C'2

    and,

    with

    decreasing gamma

    energy,

    J.

    R.

    Arnold,

    Scintillation

    counting of

    natural

    radiocarbon: 32

    P. S.

    Baranov, V.

    I.

    Goldanskii,

    and V. S.

    Roganov,

    Dos-

    I.

    The

    counting

    method,

    Science,

    vol. 119,

    pp.

    155-157;

    January,

    imeter

    for

    high-energy

    neutrons,

    Rev. Sci.

    Instr., vol.

    28,

    pp . 1-29-

    1954.

    1032;

    December, 1957.

    1958

    169

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    IRE

    TRANSACTIONS

    ON NUCLEAR SCIENCE

    responded according to the relationship:

    Per

    cent

    R

    =

    kE

    1/2

    The earliest large-volume counters

    were about 0.03

    m3

    in

    volume

    and were used for studies

    of cosmic

    rays33 and

    of total absorption

    of

    gamma rays.34 It was indeed a

    spectacular

    increase

    when

    Cowan

    and Reines35 jumped

    to 0. 3 m3

    for th e Hanford

    phase of

    the

    search fo r the free

    neutrino. Hydrogen,

    for the

    most

    part

    in

    th e toluene

    solvent,

    was allowed

    to

    be transmuted

    by

    neutrinos

    to

    give, in

    each

    interaction,

    a

    positron

    and a n eu tr on . The

    positron gave

    a

    prompt

    scintillation

    and then

    after a short

    slowing

    down

    time,

    the neutron was

    captured in cadmium

    to give

    about

    9.1

    mev

    of

    gammas,

    which

    contributed a

    delayed

    scintillation. The

    cadmium was in

    th e

    form of

    cadmium propionate,

    which was

    dissolved in

    th e

    scintilla-

    to r

    with

    th e

    help

    of methanol.

    A similar detector

    has

    been used

    to set a

    1022

    years lower

    limit

    on the lifetime

    of

    a nucleon36

    and

    to

    measure

    th e

    distribution

    of fission neutron

    multiplicities.37'38

    In th e

    latter application

    an

    81

    per

    cent

    efficiency

    for

    couniting

    neutrons

    of

    a

    few

    mev

    was

    realized.

    By

    this

    time,

    cadmium

    2-ethylhexanoate

    was

    found to be

    a

    better

    homogeneous

    source

    of cadmium

    than cadmium

    propionate

    and

    metha-

    nol.

    This

    same 0.3

    m3

    detector

    system

    has been

    used in

    a

    velocity

    as

    well

    as

    time

    distribution

    study

    of

    prompt-

    neutron

    emission

    from

    spontaneous

    fission

    modes

    of

    Cf232.39

    Both boron-loaded40 and cadmium-loaded4 liquid

    scintillation counters

    have

    been used

    for neutron detection.

    A 0.57

    m3

    detector

    has been

    used

    in an

    attempt

    to

    identify

    double

    beta

    decays.42

    Most

    of

    th e volume

    served

    as

    a cosmic

    ray

    and

    gamma ray

    anticoincidence

    shield.

    A

    small

    detector

    in th e

    center,

    which

    used

    th e

    same

    liquid

    as

    th e

    outer

    detector,

    was a

    two-section coincidence

    detector

    for betas.

    Harrison'

    has

    reported

    that

    he is

    now

    studying

    the

    strength

    of th e

    interaction

    between

    cosmic

    ray ,u-mesons

    33

    F.

    B. Harrison,

    Large-area

    liquid

    scintillation

    counters,

    Nucleonics,

    vol.

    10,

    pp.

    40-45;

    June,

    1952.

    34

    M.

    R.

    Cleland

    and H.

    W.

    Koch, High-energy

    gamma-ray

    spectrometer,

    Nucleonics,

    vol.

    10 , p.

    41; March,

    1952.

    35

    C.

    L.

    Cowan, Jr.,

    F.

    Reines,

    F. B.

    Harrison,

    E. C.

    Anderson,

    and F.

    N.

    Hayes,

    Large liquid

    scintillation

    detectors,

    Phys.

    Rev.,

    vol.

    90,

    p.

    493;

    May,

    1953.

    36

    F. Reines,

    C.

    L.

    Cowan,

    and M.

    Goldhaber,

    Conservation

    of th e

    number

    of

    nucleons,

    Phys. Rev.,

    vol.

    96, pp .

    1157-1158;

    November,

    1954.

    37

    B. C.

    Diven,

    H. C.

    Martin,

    R. F.

    Taschek,

    and J.

    Terrell,

    Multiplicities

    of

    fission

    neutrons,

    Phys.

    Rev.,

    vol.

    101,

    pp .

    1012-

    1015;

    February,

    1956.

    38

    D.

    A.

    Hicks,

    J.

    Ise,

    Jr.,

    and R.

    V.

    Pyle,

    Probabilities

    of

    prompt-neutron

    emission

    from

    spontaneous fission,

    Phys.

    Rev.,

    vol.

    101,

    pp.

    1016-1020;

    February,

    1956.

    3

    W.

    E.

    Stein

    and S.

    L.

    Whetstone,

    Jr.,

    submitted to

    Phys.

    Rev.

    40

    L. M.

    Bollinger

    and

    G.

    E.

    Thomas,

    Boron-loaded

    liquid

    scintillation

    neutron

    detectors,

    Rev. Sci.

    Instr.,

    vol.

    28 , pp . 489-496;

    July,

    1957.

    41

    F.

    Reines,

    C.

    L.

    Cowan,

    Jr.,

    F.

    B.

    Harrison,

    and

    D. L.

    Carter,

    Detection

    of neutrons

    with

    large liquid

    scintillation

    counter,

    Rev.

    Sci.

    Instr.,

    vol.

    25,

    pp .

    1061-1070;

    November,

    1954.

    42

    C.

    L.

    Cowan, Jr.,

    F. B.

    Harrison,

    L. M.

    Langer,

    and F.

    Reines,

    A test of

    neutrino-antineutrino

    identity,

    Nuovo

    cimento,

    vol.

    3,

    pp . 649-651;

    March,

    1956.

    and carbon nuclei which ar e part

    of

    a large-volume

    detector. The

    1.4 m3 of liquid is contained in a polyethylene

    container to minimize background above 5

    mev

    by remov-

    in g the Fe(n, -y) source of background which

    occurs

    with

    an iron

    container.

    In case

    al l

    this mention of

    volume in

    m3 is difficult to

    visualize,

    a

    corollary

    consideration in

    weight

    units is

    interesting. One m3 of a liquid scintillator

    weighs

    about

    one

    ton.

    The

    most giant,

    large-volume, external sample detector

    reported to

    date43

    is

    th e 1.8

    m3

    volume, three

    of

    which

    were

    used

    at th e same time, for

    the

    Savannah

    River

    phase

    of

    th e

    search

    for the free neutrino. In this case, the

    identifiable

    neutrino

    interactions

    took place in two water

    targets containing

    cadmium

    chloride

    oriented in a

    double-

    decker

    sandwich-array

    with the

    three

    scintillation counters.

    Delayed gamma

    coincidences from

    positron

    annihilationl

    followed

    by neutron-cadmium

    reaction were d et ec te d in

    th e liquid

    counters. Each

    counter had 110 5-inch photo-

    multipliers,

    half

    of which were

    at

    each end

    of

    a slab

    configuration.

    The

    solution

    which

    was

    used

    was

    3

    g/1

    p-terphenyl

    and 0. 2

    g/1 POPOP in

    triethylbeuizenie.

    Biological and

    medical

    employment of large-volume,

    external-sample liquid scintillation detectors44 has made

    use

    of

    an

    enveloping,

    4r-approximating geometry around

    th e sample

    which

    is

    easily

    introduced

    into

    th e

    countinlg

    position

    in

    an

    axially-oriented cylinder inside

    an

    annular

    ring

    of

    liquid.45

    Two versions

    which

    exist

    at

    Los Alamos

    ar e the small-animal

    counter

    whose scintillator volume

    is

    0.036

    m3,

    and the

    Human

    Counter46

    (0.42 m3). Both

    counters

    are used

    in

    studying

    gross as well as

    specific

    metabolism

    of

    radioisotopes

    in

    live experimental animals

    and

    human

    beings.

    Reines,

    1 while

    speculating

    on th e

    limits in

    size

    on

    a li(uid

    scintillation

    detector,

    conjured

    up

    a vision of

    a

    10

    m

    X 10

    m

    cylinder holding about 700

    m3

    of

    liquid.

    It has a few

    hundred 5-inch

    photomultipliers

    and

    an

    efficient diffuse

    reflector,

    and

    gives

    about

    50

    per

    cent

    resolution

    for

    a

    1-mev

    event.

    The time

    response

    of this

    detector

    is limited

    by

    the

    velocity

    of

    light,

    it

    has as

    much

    mass

    pe r

    uinit

    area

    as the entire

    atmosphere,

    and

    it

    represents

    a total

    absorber

    for

    charged particles

    up

    to 1.5

    bev,

    considering

    ionization

    as the

    only process contributing

    to

    energy

    loss.

    Such

    a

    detector,

    which

    is

    almost

    400

    times

    larger

    than the

    largest

    in use

    today,

    may

    not be

    made for

    many years,

    but

    as

    its

    size

    is

    approached,

    today's

    large-volume

    counters

    will

    have to be

    renamed.

    43

    C. L.

    Cowan, Jr.,

    F.

    Reines,

    F.

    B.

    Harrison,

    H.

    W.

    Kruse,

    and

    A. D.

    McGuire,

    Detection

    of the free neutrino:

    a confirma-

    tion, Science,

    vol.

    1 24 , p p. 103-104;

    July,

    1956.

    44

    W.

    H.

    Langham,

    se e footnore 1.

    45

    M.

    A.

    Va n

    Dilla,

    R.

    L.

    Schuch,

    and

    E. C.

    Anderson,

    A

    large

    47r

    gamma-ray detector,

    Nitcleonics,

    vol.

    12, pp . 22-27;

    September,

    1954.

    46

    E.

    C.

    Anderson,

    R.

    L.

    Schuch,

    J. D.

    Perrings,

    and W.

    H.

    Langham,

    The Los

    Alamos

    human

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    December