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Chapter 4 Scintillation Detectors

4.1. Basic principle of the scintillator

Scintillator
Ionizing
radiation
Light
(visible, UV)
Light
sensor


Fig. 4.1. Principle of the scintillation detectors.

Scintillates are one of the oldest types of radiation detector because measurements could be
made with photographic film. Images could be collected or intensity measurements could be
made. Measurements were also made with the human eye observing the brightness of frequency
of flashes in the scintillator. Nowadays the light output is converted into voltage pulses that are
processed in the same way as pulses from proportional counters, semiconductor detectors etc.
The whole point of scintillation detectors is that we want to produce a large light output in the
visible range.

There are two commonly used types of scintillators, inorganic crystals and organic scintillators.
The scintillation mechanism is different for these two types.

4.2. Inorganic Scintillators

Conduction
Valence
Conduction
Valence
Conduction
Valence
Insulator Semiconductor Conductor

Fig. 4.2. Band structure for electron energies in solids.

The scintillation mechanism depends on the structure of the crystal lattice. In a pure inorganic
crystal lattice such as NaI, electrons are only allowed to occupy selected energy bands. The
forbidden band or band gap is the range of energies in which electrons can never be found in the
pure crystal.

In the pure crystal, absorption of energy can elevate electrons from the valence band to the
conduction band leaving a gap in the valence band. However, the return of an electron to the
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valence band with the emission of a photon is an inefficient process. Few photons are released
per decay, the energy is emitted by other mechanisms. In addition, band gap widths in pure
crystals are such that the resulting emitted photon is too high to lie within the visible range.

Small amounts of impurities are therefore added to the crystal. Tl is added to NaI in trace
amounts. The impurities are called activators, they create special sites in the lattice at which the
band gap structure, the energy structure, is modified. The energy structure of the overall crystal
is not changed, just the energy structure at the activator sites.


(a) Pure crystal


(b) Activated crystalline scintillator
Fig. 4.3. Energy band structure of an inorganic scintillator.

At the few activator sites within the sample, the energy structure is modified. Energy states are
created within what would be the forbidden band in the pure crystal. The electron can de-excite
through these levels back to the valence band.

The energy levels created by the activators presence within the crystal are narrower than in the
pure crystal.

The photons emitted by the transitions of electrons from upper to lower states will be lower in
energy than in the pure crystal: The emission spectrum is shifted to longer wavelengths and will
not be influenced by the optical absorption band of the bulk crystal.

The photons are emitted in the visible range.


Fig. 4.4. The emission spectra of several common scintillators.

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A charged particle (e.g. a photoelectron) passing through the crystal will create a large number
of electron-hole pairs.

The positive hole quickly drifts to the location of an activator site and the site is ionized. The
activator sites are preferentially ionized because the ionization energy of the activator is less
than a typical lattice site.
The electron elevated to the conduction band is free to migrate through the crystal and will
do so until it encounters an ionized activation site.
The electron drops into the impurity site, creates a neutral impurity configuration with its
own set of excited states.

transition
Excited configuration ground state

De-excitation occurs quickly with a high probability of photon emission.
The activator is chosen so that the photon is visible.
The typical half-life of the activator excited states are 10
-7
seconds with the migration of the
electrons through the crystal taking a much shorter time. The timing of the light output is
therefore dependent on the half-life of the state.

Types of inorganic scintillators:
Alkali halide: NaI(Tl), CsI(Tl), CsI(Na), LiI(Ei)
Other slow Inorganics: BGO, CdWO
4
, ZnS(Ag)
Cerium-Activated Fast Inorganics: GSO, YAP, YAG, LSO, LuAP, LaBr
3




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4.3. Organic Scintillators

The scintillation mechanism in organic materials is quite different from the mechanism in
inorganic crystals. In inorganic scintillators, e.g. NaI, CsI the scintillation arises because of the
structure of the crystal lattice.

The fluorescence mechanism in organic materials arises from transitions in the energy levels of a
single molecule and therefore the fluorescence can be observed independently of the physical
state. For example anthracene is observed to fluoresce as
a polycrystalline material
a vapor
part of a mixed solution

Practical organic scintillators are organic molecules which have symmetry properties associated
with the electron structure.


Fig. 4.5. Energy levels of organic molecules.

Energy from a charged particle is absorbed and excites the electron into a variety of excited
states - the singlet states (spin = 0) are labeled S
1
, S
2
, S
3
in Fig. 4.5. For organic scintillators the
spacing between S
0
and S
1
is 3 to 4 eV, the spacing between the upper states is much smaller.

Each of the S levels is subdivided into a series of levels with much finer structure (corresponding
to the vibrational states of the molecule). The typical spacing is 0.15 eV. The 2
nd
subscript
denotes the fine structure level.

Spacing between S states is 3-4 eV, spacing in vibrational structure is 0.15 eV

Scintillation Mechanism
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At room temperature, average energy is approximately 0.025 eV so all molecules are in the
S
00
state.
When the charged particle passes through, kinetic energy is absorbed by the molecules, and
electrons are excited to the upper levels.
The higher states S
2
, S
3
, de-excite quickly (picoseconds) to S
1
state through radiationless
transitions (internal conversion).
States such as S
11
, S
12
that have extra vibrational energy and are not in thermal equilibrium
with neighboring molecules, quickly lose energy.

After negligibly short time a population of excited molecules in S
10
state is produced as the
net effect of the excitation process.

Scintillation light, prompt fluorescence, is emitted in transitions between S
10
and the ground state.
The prompt fluorescence intensity at time t following excitation is described by
I=I
0
e
-t/

where is the fluorescence decay time for the S
10
level.

In most organic scintillators, is the order of a few nanoseconds therefore organic scintillators
are fast.

The lifetime for the T
1
state is much longer than the S
1
state. T
1
is populated by a transition
called an intersystem crossing. The lifetime of the T
1
state can be ms.

T
1
S
0
transitions give rise to phosphorescence (delayed light emission).
T
1
lies below S
0
, therefore the wavelength of the emitted phosphorescence is longer than the
wavelength of the fluorescent light. The phosphorescent light can be discriminated from the
scintillation light on the basis of timing and wavelength.

The energy level scheme explains why organic scintillators can be transparent to their own
fluorescence emission. All fluorescence emissions (except S
10
S
00
) have a lower energy
than the minimum required for absorption. There is little overlap between emission and
absorption spectra, therefore the emitted light mostly passes straight on through the scintillation
medium.

Types of organic scintillators:
Pure organic crystals: Anthracene, Stilbene
Liquid organic solutions: by dissolving an organic scintillator in a solvent
Plastic scintillators: dissolving & polymerizing


4.4. Photomultiplier Tubes (PMT) and Photodiodes

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In order to provide a useful measurement device, an electrical signal has to be formed from the
scintillation light. Two main types of device are used to do this; the photomultiplier tube and the
photodiode.

A. Photomultiplier Tube (PMT)
Photomultiplier tubes are extremely good at
converting light into an electrical signal; electrical
pulses can be obtained from a few hundred visible
photons.

Photocathode
Photomultiplier tubes are vacuum tubes in which the
first major component is a photocathode. A light
photon may interact in the photocathode to eject a
low-energy electron into the vacuum. This process can
be thought to occur in three steps

1) absorption of the photon and energy transfer to the
electron in the photocathode material
2) the migration of the photoelectron to the surface of
the photocathode
3) escape of the electron from the photocathode
surface.
Fig. 4.6. Basic elements of a PMT.

The energy available to be transferred from a scintillation photon to an electron is, for blue
scintillation light, approximately 3 eV. However, some of this energy is lost in electron-electron
collisions as the electron migrates to the surface and then the potential barrier at the surface
vacuum interface (the work function) must be overcome in order for the electron to enter the
vacuum. There are therefore energy limitations on the system posed by the potential barrier at
the surface/vacuum interface and the interactions in the material.

Some limitations are placed on the materials that can be used for the photocathode. Typically
metals have a work function of 3 ~ 4 eV, semiconductors 1.5 ~ 2 eV.

In addition, the thickness of the material that can generate photoelectrons into the vacuum is
limited, because there is a rate of energy loss as the electron migrates to the surface. For metals
this energy loss rate is relatively high and an electron will have its energy drop below the
potential barrier after traveling only a few nanometers. In semiconductors the electron can travel
20 30 nanometers, before its energy drops below the barrier. In either case only a thin layer of
material contributes photoelectrons into the vacuum. The cathodes are sometimes designed so
that the light is incident on one side, while the electrons are ejected on the other. The
photocathode is therefore extremely thin, because of the problems of electron interaction in the
material, and is therefore semi-transparent to visible light. This means that a large proportion
(more than half) of the light passes straight through without interacting with the photocathode.
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Even if the work function is low, the necessary thinness of the photocathode means that they can
only convert, at best, a small proportion of the photons.

The problems of work function and electron interactions in the material mean, in addition, that
all photocathodes have an energy cut-off with respect to the frequency of the light that can
generate photoelectrons into the vacuum. Some light frequencies cannot create electrons with
enough energy to overcome the potential barrier. The energy cut-off is usually in the infra-red or
near infra-red part of the spectrum.

The sensitivity of a photocathode is usually quoted in terms of the quantum efficiency. The
quantum efficiency of the photocathode is defined as the probability for the conversion of light
to an electrical signal and is defined as

Quantum efficiency = number of photoelectrons emitted/ number of incident photons

The quantum efficiency is a strong function of wavelength of the incident light, and an effort is
made to match the spectral response of the photocathode to the emission spectrum of the
scintillator in use. The average quantum efficiency over the emission spectrum of a typical
scintillator is about 15 to 20 percent while the peak quantum efficiency is 25 ~ 30 %. The
standard for quotation is the number of photoelectrons per keV energy loss by fast electrons in a
NaI(Tl) crystal. For the peak quantum efficiency, about 8 ~ 10 photoelectrons are produced per
keV energy loss. Therefore, the average energy loss required to create a single photoelectron (or
one basic information carrier) is ~ 100 eV, which is much bigger than the values in gas-filled or
semiconductor detectors. Presently, multialkali (based on Na
2
KSb) and bialkali (based on
K
2
CsSb) materials are usually used for the photocathode.


Fig. 4.7. The spectral sensitivities of photocathode materials.
Electron Multiplication

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A PMT takes the electrical signal from the photocathode and amplifies through a dynode chain
by the process of electron multiplication.

Electrons are ejected from the photocathode into the vacuum with an energy of 1 eV and are
accelerated by a voltage of a few hundred volts toward an electrode. The accelerated electron has
an energy of a few hundred electron volts upon arrival at the electrode; this deposition of kinetic
energy can result in the re-emission of secondary electrons. It typically takes 2-3 eV to excite an
electron in the dynode, so 100 V can theoretically create 30 electrons.

However, there is the same problem as in the photocathode; electrons must be near the surface to
be emitted, otherwise they lose too much energy through collisions and are unable to overcome
the potential barrier at the surface. Only a small proportion of the electrons excited up to the
conduction band reaches the surface and creates secondary electrons.

The overall multiplication factor for a single dynode is given by

= number of secondary electrons emitted / primary incident electron
is typically 4 ~ 6 for voltages of a few hundred volts.

Multiple Stage Multiplication

Photomultiplier tubes employ dynode chains of several stages of multiplication to create electron
gains of the order of 10
6
.

Electrons are created in the photocathode, and accelerated toward the first dyode, where
secondary electrons are emitted. The secondary electrons are accelerated by the electric field
toward a second dynode, where they create secondary electrons, and so on. This can be repeated
many times.

The overall gain for the PM tube =
N


Where N is the number of multiplication stages, is the fraction of electrons collected by the
multiplier structure, and is the multiplication factor for a single electrode.

For typical tubes is around 5 and approaches unity. 10 stages of multiplication result in an
overall tube gain of 5
10
or 10
7
.

Statistics of Electron Multiplication

The emission of secondary electrons from the dynodes is a statistical process, so the
multiplication factor is not a fixed constant but varies from event to event around a mean
value. Therefore pulses are amplified overall down the dynode chain by a mean value which has
some statistical variation.

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We measure a final mean voltage that has statistical spread, i.e. we measure not just a single
energy, but a mean energy with a spread. The dynode chain therefore affects the energy
resolution of the system.

We can assume a simple model where the production of secondary electrons follows a Poisson
distribution about an average yield.

A single photoelectron incident on the first dynode results in a mean number of secondary
electrons of . The relative variance is thus 1/.

The process is compounded over N identical stages of the PM tube, and the mean number of
electrons collected at the anode is given by
N
.

The relative variance in this number is 1/+1/
2
+1/
3
++1/
N
1/(-1)

The variance in the dynode chain adds to the poor observed energy resolution of scintillation
detectors.



Fig. 4.8. Different configurations of PMTs.


B. Photodiodes

An alternative way to detect the scintillation light is the use of a silicon photodiode. This is a
semiconductor device which consists of a thin layer of silicon in which the light is absorbed after
which free charge carriers (electrons and holes) are created. Electron and holes are collected at
the anode and cathode of the diode. Most frequently used are PIN diodes operated in reverse bias
mode.
Photodiodes have potential advantages: higher quantum efficiency and compact size. However,
electronic noise is a major problem due to the small signal amplitude.

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References

1. G.F. Knoll, Radiation Detection and Measurement - 3
rd
edition (Chapters 16 to 18), John Wiley & Sons,
1999.