REVIEW

after glow intensity exceeds specific limitations, image

Development of medical degradation occurs due to memory effects. The decay time
and after glow are the time properties of scintillation but
scintillator the decay time describes the behavior of the specific lu-
1 1,2 minescence center. And the after glow is often induced by
LIU Bo & SHI Chaoshu some traps from crystal detects. High density has a good
1. National Synchrotron Radiation Laboratory, University of Science and stopping power and can shorten the radiation length of
Technology of China, Hefei 230029, China scintillator which can decrease the volume of scintillator
2. Department of Physics, University of Science and Technology of
China, Hefei 230026, China
and detection facility as well as the cost. The light emitted
by the scintillator should have a good spectral match to
Abstract This review presents the scintillators require- photodetectors in order to ensure the high detection effi-
ments for the medical imaging modalities. The history and ciency. However, the ideal scintillator does not exist, so
the development in recent years of the medical scintillators each modality must compromise, selecting the most suit-
(mainly for GSO:Ce, LSO:Ce, LuAP:Ce) are expatiated in able combination of properties from available scintillators.
detail. The conventional medical scintillators such as NaI
(Tl) and BGO are not well satisfied with the requirements
Since Rontgen discovered X-ray in 1895 and two
in some aspects. For example, the NaI (Tl) has a low den-
British doctors took the first X-ray picture one year
sity and a comparatively long decay time and BGO has a
later[1], the ray (X-ray or γ-ray) imaging techniques have relatively low light yield. Opportunities for improving the
played a vital role in diagnosing disease because they can scintillators used for medical imaging systems still exist in
help the doctors to observe the interior of patients bodies. some aspects as they are somewhat far from the theoreti-
A rapid development has been got in medical imaging cal limits.
field especially for the X-and γ-ray imaging techniques More and more scientists are devoting their effort to
since the 1950s. The imaging techniques make use of the the research in medical scintillators which have become a
detection of rays and deal with electronic system and focus in recent years. New excellent scintillators are
computers. The function of the scintillator in the imaging ceaselessly proposed. More and more reports about medi-
systems is to absorb the incident high energy photon and cal scintillator appeared in recent international confer-
convert it into visible light. Medical imaging systems ences on inorganic scintillator. The first international con-
contain four modalities, namely planar X-ray imaging, ference on medical scintillator was held in 2000, Russia.
X-ray computed tomography (X-ray CT), single photon The development of medical scintillator will impulse the
emission computed tomography (SPECT) and positron enhancement in medical diagnosis.
emission tomography (PET). With the increasing re-
quirements for medical imaging equipment, the demand 1 Scintillator requirements for medical imaging
for the scintillators as the detection materials in imaging In the field of medical imaging, the energy of the
systems is enormous. About 175 metric tons of scintillator photons detected is between 15 and 600 keV. The detec-
are required annually and the demand for the various scin- tion system must be very efficient because there is a limit
tillators is shown in table 1[2]. of radiation dose absorbed by patients as safety concerns.
The improvement of signal-to-noise ratio cannot be ob-
Table 1 Annual volume of medical scintillator tained by increasing the ray source intensity but achieved
Annual production Annual scint. by increasing the sensitivity of detector. In the range of 15
Modality
(screens) volume/m3

511 keV, photon energies used for medical imaging
Planar X-ray 1000000 50
have the attenuation length of 2
10 cm in tissue. When
X-CT 2000 0.15 the photons come into the human body, their interactions
SPECT 2000 6 result in the Compton scattering due to the low effective
PET 50 0.5 atomic number of tissue and most photons undergo con-
tinually Compton scattering until they leave the body. The
In general, an ideal medical scintillator should have 10%
15% γ photons without the scattering can form the
the following properties: (1) high luminous efficiency; (2) accurate image and other photons scattered come into
short decay time; (3) no after glow; (4) high density; (5) being the background. In order to improve the quality of
short radiation length; (6) good spectral match to imaging, the reducing of Compton scatter photons is nec-
photodetectors; and (7) low cost[2]. The luminous effi- essary.
ciency must be very high in order to reduce the radiation Now the development of scintillators used in planar
dose to patients as safety concerns. Short decay time will X-ray imaging, e.g. Gd2O2S:Tb and LaOBr:Tb, and used
improve the time-resolution of detecting high energy in X-ray CT, e.g. (Y,Gd)2O3:Eu,Pr and Gd2O2S:Pr,Ce,F, is
photon. The after glow is also a critical parameter. If the relatively mature. The attention is mainly focused on the

Chinese Science Bulletin Vol. 47 No. 13 July 2002 1057

REVIEW
scintillator used in SPECT and PET imaging systems. 50% PET market [6]. But BGO has a low light yield (20%
SPECT is based on detecting individual photons
25% of NaI (Tl)) and a long decay time (~300 ns),
emitted randomly by radioactive drug (such as 99mTc with which is not benefit for the improvement of time resolu-
the emission of 140 keV photons) which is introduced into tion. New scintillators used in PET and γ cameras ought to
the body either by injection or inhalation. In practice, the have high atomic number (high Z value), high light yield
only material used in SPECT is NaI:Tl. The scintillator and fast decay time compared to BGO. Actually, the emis-
requirements for SPECT are, in order of decreasing im- sions of Ce3+ has fast decay time from several to several
portance, (1) high luminous efficiency; (2) high density
tens ns. If we could find a high density matrix and Ce3+
(>3.5 g/cm3); (3) low cost; (4) good match of emission
could be doped into the matrix easily, our aim for research
spectrum to PMT (300
500 nm); and (5) short decay
new medical scintillators would be achieved. In fact, the
time (<1 µs)[1].
recent development for medical scintillators is based on
Similar to SPECT, the patient for PET imaging is
this idea. At the same time, many problems such as the
injected with a biologically active, radioactively labeled
drug that localizes at targeted sites in the body. The dif- crystal growth technique and the improvement for energy
ference is that the drug (commonly used e.g. 11C, resolution should be solved. Nowadays, the extensively
13 15 18
N, O, F) is positron-emission radionuclide. The emit- studied Ce3+ doped materials with high density have
ted positron combines with a nearby electron leading to an Lu2SiO5:Ce(LSO:Ce),Gd2SiO5:Ce (GSO:Ce) and LuAlO3:
annihilation which creates the back-to-back emission of Ce (LuAP:Ce). Some properties of the scintillators are
two 511 keV γ photons. The scintillator requirements for listed in table 2.
PET are, in order of decreasing important, (1) short at- () LuAP: Ce. In 1973, Weber introduced YAlO3:
tenuation length (<1.2 cm) ; (2) short decay time (<300 Ce (YAP:Ce)[7] and some groups researched its scintillate
ns); (3) low cost; (4) high luminous efficiency (>8000 properties[8ü11]. YAP:Ce has a fast luminescence but a low
photons/MeV); and (5) good match of emission spectrum density. In order to improve its stopping power, the heavi-
to PMT (300
500 nm) [1]. In practice, the most common est element lutetium in lanthanide group was used to sub-
material used in PET is Bi4Ge3O12 (BGO). stitute for yttrium, LuAP:Ce in some laboratory[12ü18]. At
2 New medical scintillator room temperature, the LuAP:Ce has an emission band
It took one century for CaWO4 polycrystal powder to peaked at 355 nm which is excited by VUV (fig. 1). The
be used as scintillator[3]. Thallium doped sodium iodide, decay time is 11 and 28 ns, respectively. The light yield is
NaI (Tl), introduced by Hofstadter in 1948[4] was the most 20% higher than BGO. The density of LuAP:Ce is 8.34
popular scintillator used in the detectors for the following g/cm3 which is heavier than that of YAP:Ce. So the
tens of years because of its high light yield. However, NaI LuAP:Ce is a promising scintillator. However, no reliable
(Tl) has a low density (3.76 g/cm3) and a long radiation growth production processes have been obtained yet. Us-
length, which confines the energy resolution and reduces ing the Czochralski method, only very small crystal
the imaging quality. This is the reason why Weber et al.[5] samples could be obtained[14,19]. The LuAP:Ce samples of
proposed a new heavy scintillator BGO (7.13 g/cm3) in 5×5×50 mm3 were prepared by Petrosyan et al. using the
1973, which has been extensively studied as a promising Bridgeman method[20]. The different methods and differ-
scintillator. Nowadays, the BGO has occupied more than ent preparing conditions can result in the great diversities

Table 2 Properties of scintillators

Density Radiation Energy
Light yield/ Decay Wave- Refractive Hygro-
Scintillator length Zeff resolu-
photons/MeV /gCcm-3 /ns length /nm index scopic
/cm tion137Cs(%)
NaI(Tl) 38000 3.7 230 415 2.59 51 1.85 7.0 Strong
CsI(Tl) 60000 4.5 1000 560 1.85 54 1.80 9.0 Slight
BGO 8000 7.13 300 480 1.12 74 2.15 9.5 No
LSO:Ce 25000 7.35 11/36 420 1.14 66 1.82 12.0 No
GSO:Ce 8000 6.7 56/600 440 1.38 59 1.85 7.8 No
YSO:Ce 10000 4.54 37/82 420 9.0 No
YAP:Ce 16000 5.37 28 360 2.24 34 1.93 11.0 No
LuAP:Ce 9600 8.34 11/28 355 No
Lu0.3Y0.7AP:Ce 14000 6.19 25 360 53 No
Lu0.3Gd0.7AP:Ce 10800 7.93 360 63
Gd2O2S:Tb 70000 7.3 545 64 2.1
Y2O2S:Tb 60000 4.9 545

1058 Chinese Science Bulletin Vol. 47 No. 13 July 2002

 REVIEW
130, 175 and 255[28], and its spectral component
belongs to the transition 5d4f of Ce3+ (3.45 eV). Be-
cause there is no thermal stimulated electric-conduction
signal to be detected, the trapped electrons can directly
enter the 5d state of Ce3+ without going into the conduc-
tion band. An ideal trap related to oxygen vacancies was
proposed and validated by the annealing experiment.
Mares reported that color centers such as O− and F+ can be
induced by γ-ray irradiation (3000 Gy dose)[33]. The tem-
perature dependence, instability of light yield and the
change of decay time are closely related to the defects, so
it is important to enhance the defects research which will
contribute to the improvement of the scintillation proper-
Fig. 1. Emission spectra of LuAP:Ce at RT and low temperature ex- ties.
cited by 152 nm.
() RE2SiO5:Ce. During the development of new
in scintillate properties[19, 21]. Other lutetium phases, espe- medical scintillators, silicate doped Ce3+ is another focus.
cially the garnet phase, can arise in the samples. The Such materials include YSO:Ce, GSO:Ce, LSO:Ce and
growth of LuAP:Ce is a hard task because it is very diffi- LGSO:Ce. The YSO:Ce has been commercially used as
cult to stabilize the lutetium orthoaluminate phase. A pos- phosphor[34,35]. The GSO:Ce single crystal was introduced
sible way to overcome the difficulty is to grow mixed or- by Takagi et al. in 1983[36]. The GSO:Ce has faster decay
thoaluminate crystals, especially using yttrium and gado- time than BGO and higher density and intrinsic energy
linium,namelyLux(RE3+)1-xAP:Ce(RE3+=Y3+ or Gd3+)[22,23]. resolution than the NaI:Tl[37ü39]. The LSO:Ce was first
In addition, present research shows that the light yield of proposed by Melcher et al. in 1992[40] and got a prompt
Lux(RE3+)1−xAP:Ce is higher than that of LuAP:Ce, which development due to its high light yield, high density and
is one of the reasons of developing Lux(RE3+)1−xAP:Ce. fast decay time and it becomes a very promising scintilla-
Large crystals with good quality were grown for tor for PET[41ü49]. The LGSO:Ce (Lu1−xGdxSiO5:Ce) was
Lux(Y3+)1-xAP:Ce with x=0.1, 0.2 and 0.3. There is no firstly reported by Yamamoto[50] in 1998 and its properties
were described by some groups[46,51]. The LGSO is a new
garnet phase in crystals. Lux(Gd3+)1−xAP:Ce crystals were
obtained with a range between 0.6 and 0.7[24ü26]. The
and very promising scintillator due to its lower back-
ground radiation in comparison to the LSO. But the pre-
light yield of Lux(RE3+)1−xAP:Ce is about 40%
75% sent development stage of the LGSO shows that the
higher than that of BGO. For the application of PET, LGSO has about 20% lower light output and worse energy
Lu0.3Y0.7AP:Ce is a promising material. Lux(Gd3+)1−xAP: resolution than LSO.
Ce has higher Zeff and density but lower light yield than The emission spectrum of RESO:Ce exhibits the
Lux (Y3+)1−xAP:Ce. In the application of PET and SPECT, presence of two sets of emissions ascribed to the lumi-
high density material has a short radiation length which nescence centers Ce1 and Ce2 respectively as shown in
can decrease the thickness of scintillators and increase the figs. 2 and 3. At 11 K, there are two emission bands
spatial resolution. The LuAP:Ce is the heaviest material peaked at 430 nm of Ce1 centers and at 480 nm of Ce2
among all studied scintillators at present. The final aim is centers under the excitation of 345 and 378 nm, respec-
to find an optimal growth method and increase the light tively. At 296 K, the intensity decreases slightly for Ce1.
yield. The Lux (RE3+)1−xAP: Ce should be a transient ma- However, there is a remarkable decrease for Ce2 and the
terial from the YAP:Ce to LuAP: Ce. emission wavelength shifts towards the short wavelength
There are many kinds of traps in the REAP:Ce crys- about 460 nm. Therefore, the Ce1 emission is dominant at
tals which can be reflected by thermoluminescence (TL). room temperature. Shi et al. reported the emission of
It is not very clear about the origin of these traps but their GSO:Ce excited by vacuum ultraviolet (VUV)[52]. It was
existence can seriously affect their scintillation properties discovered that under the excitation of 189 nm, no lumi-
especially for the stability of light yield and scintillation nescence quenching occurred until the temperature up to
decay time. The traps in the crystals can influence the 453 K and another two new band peaks, which come from
stability of light yield and the scintillation decay Ce2 centers or some defects, appeared at 581 and 652 nm.
time[28]. The reports about TL of LuAP:Ce are very abun- At low temperature (6 K) a narrow excitation band peaked
dant[27,29ü32]. Experimental results show that the TL of at 6.5 eV and a wide band peaked at 22.5 eV were ob-
LuAP: Ce peaks at 360, 500, 600, 730 K corresponding to served, the former is related to the transition from the va-
the trap depths ranging from 0.7 to 1.9 eV[28] and the TL lence band to the conduction band; the latter is the excita-
below the room temperature appear at 183 and 266 K[30]. tion of a mixture state with 5p,5d core level located in
The TL of LuxY3+1−xAP:Ce appears at 50, 100
Gd3+. The emission spectra of LSO:Ce excited by 188 nm

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REVIEW
at room temperature and low temperature are shown in fig. In PET application, LSO:Ce is the best substitute for
4. At 11 K, the excitation peaks of LSO:Ce lie in 356 nm BGO. But it is difficult to develop LSO due to the high
(Ce1) and 376 nm (Ce2) and the emission peaks lie in 393, cost of Lu2O3. In addition, the stability of light output is
427 nm (Ce1) and 460 nm (Ce2)[39]. Above the room rather poor for different samples, and even poor for the
temperature the emission spectrum ranges from 410 to different parts in the same single crystal[45]. The basic
440 nm but it varies with the samples as well as the exci- opinion for the instability of LSO luminescence lies in the
tation spectrum[43] which may be caused by defects and existence of two different centers, Ce1 and Ce2[43,47]. At
traps from the immature growth technique. room temperature the luminescence from two kinds of Ce
centers induces the reduction in energy resolution of 10%
with 662 keV radiation. There are two sets of Ce centers
in GSO:Ce, but at room temperature the luminescence
quenching occurs on Ce2[43]. So the stability of GSO:Ce
luminescence is better than LSO:Ce, so is the energy
resolution. Therefore, GSO:Ce is a good material to sub-
stitute for BGO in the PET system.
3 Light yield nonproportionality and the intrinsic
energy resolution of scintillator
An ideal scintillator would produce a number of
scintillation photons that is proportional to the energy
deposited in the crystal. But the ideal behavior has not
been observed and all scintillators are characterized by
Fig. 2. Emission spectra of GSO:Ce at different temperatures excited some degree of light yield nonproportionality[53]. In 1956,
by 345 nm (Ce1). it was first discovered that NaI (Tl) scintillation photon
production was not strictly governed by Poisson statistics
and there was apparently some additional broadening
which was intrinsic energy resolution[54]. At the same time,
the NaI (Tl) scintillation yield nonproportionality was
observed[54]. The two phenomena mentioned above had
been studied independently until Iredale[56] and Zerby[57]
reported in 1961 that the NaI(Tl) light yield nonpropor-
tionality significantly contributes to intrinsic energy reso-
lution. Many reports about the scintillation yield
nonproportionality and the energy resolution have been
published in recent years[58ü62]. All scintillators except for
YAP:Ce[15] are characterized by the nonproportionality
response with incident energy. For example, the LSO
shows a clear sublinear increase and the light yield in-
Fig. 3. Emission spectra of GSO:Ce at different temperatures excited
by 378 nm (Ce2). creases hardly when the incident energy is above 800
keV[48]. Recent results show the nonproportionality re-
sponse with energy directly related to the crystal structure
but not to the dopant[15]. So GSO, YSO and LSO have a
similar nonproportionality response. The LuAP:Ce should
also have a similar response to YAP:Ce due to the same
reason. But the experimental results show a significant
diversity probably caused by defects from the immature
crystal growth technique[62].
The energy resolution, ∆E/E, where ∆E is the full
wave at half maximum (FWHM) of the full energy peak
and E is the energy at the maximum measured with a scin-
tillator coupled to a photomultiplier, can be written as[58]
(∆E/E)2 = (δ SC)2 +(∆N/N)2,
where δSC is the intrinsic resolution and ∆N/N is the pho-
Fig. 4. Emission spectra of LSO:Ce at RT and low temperature excited toelectron statistical contribution.
by 188 nm. The intrinsic resolution is connected with many ef-

1060 Chinese Science Bulletin Vol. 47 No. 13 July 2002

 REVIEW
fects such as inhomogeneities in the crystal which causes The fast decay time with the order of nanosecond
local variations of the light yield, non-uniform reflectivity can be obtained from the transition from the 5du4f of RE.
of the crystal surface, as well as the nonproportional re- Ce3+ is the most widely used element because of its 5du
sponse of the scintillator[58]. The photoelectron statistical 4f allowed transition. Secondly, luminescence of Pr3+ is
contribution can be calculated as follows: selected. The 5d energy level of Pr3+ is the next higher
∆N/N = 2.36D(1+ε )1/2/N1/2, than that of Ce3+, thus they are sometimes used as dopants
where N is the number of photoelectrons and the variance to create luminescence with the decay time of nanosecond
of the electron multiplier gain. The typical value of ε for order. In order to get a high effective luminescence of
XP2020Q PMT is 0.1. Ce3+, the energy gap of the host must be higher than the
In the case of APD (avalanche photodiodes), the en- energy difference of 5d and 4f of Ce3+.
ergy resolution ∆E/E can be derived as In current applications of CT , PET and SPECT, the
(∆E/E)2 =(δ SC ) 2 +(∆N/Ne-h)2+(∆noise /Ne-h)2, scintillators are all single crystal forms. In fact, ceramic
where ∆N/Ne-h and ∆noise /Ne-h are the e-h pair statistical form is also chosen and being studied. Ceramic materials
contribution and the noise contribution, respectively. often show more uniformity than single crystals because
For using high light yield scintillator such as CsI (Tl), ceramic materials reflect the average properties of many
NaI (Tl) and LSO, the energy resolution is mainly deter- very small scintillator crystals. Another advantage of ce-
mined by the intrinsic energy resolution of the crystals. ramic is the easy preparation compared with the growth of
The improvement of the intrinsic energy resolution of single crystal. It is noted that the ceramic materials must
scintillator is the key element to enhance the energy reso- be transparent for the PET and SPECT application.
lution of the detector and imaging quality. The photons From the above discussion, Ce3+ doped scintillators
with fixed energy are used in PET or SPECT, but most such as LuAP, GSO and LuSO have become the research
photons with energy loss due to Compton scatter may focus in the development of new medical scintillators.
cause some Compton scatter peaks at the low energy side Although their light yield is still lower than that of
of full energy peak. Therefore, the energy resolution is NaI(Tl), their fast decay time and high densities show that
important for PET and SPECT. they are promising scintillators for PET and SPECT. But
A theoretical calculation method, which deals with many problems have not been solved technically, so the
the intrinsic energy resolution, induced by the energy non- related researches are still under way.
proportional response of scntillators was developed by
Acknowledgements This work was supported by National Natural
Valentine[61]. This theory can calculate the electron re- Science Foundation of China (Grant Nos. 59732040 and 19774053) and
sponse and γ photon response, respectively and the results the Foundation of High Level University.
accord well with those of the experiments.
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