crystals

Article
Evaluation of Various Scintillator Materials in
Radiation Detector Design for Positron Emission
Tomography (PET)
Siwei Xie 1 , Xi Zhang 2 , Yibin Zhang 1 , Gaoyang Ying 2 , Qiu Huang 3 , Jianfeng Xu 2, *
and Qiyu Peng 1,4, *
1 Institute of Biomedical Engineering, Shenzhen Bay Laboratory, Shenzhen 518107, China;
xiesw@szbl.ac.cn (S.X.); zhangyibin94@163.com (Y.Z.)
2 State Key Lab of Digital Manufacturing Equipment & Technology, School of Mechanical Science and
Engineering, Huazhong University of Science and Technology, 1037 Luoyu Road, Wuhan 430074, China;
xizhang@hust.edu.cn (X.Z.); m201777026@hust.edu.cn (G.Y.)
3 School of Biomedical Engineering, Shanghai Jiaotong University, 800 Dongchuan Road,
Shanghai 200025, China; qiuhuang@sjtu.edu.cn
4 Department of Molecular Biophysics and Integrated Bioimaging, Lawrence Berkeley National Laboratory,
Cyclotron Road, Berkeley, CA 94720, USA
* Correspondence: jfxu@hust.edu.cn (J.X.); qpeng@lbl.gov (Q.P.); Tel.: +1-510-486-4422 (Q.P.);
Fax: +1-510-486-4422 (Q.P.)




Received: 6 August 2020; Accepted: 23 September 2020; Published: 25 September 2020


Abstract: The performance of radiation detectors used in positron-emission tomography (PET) is

determined by the intrinsic properties of the scintillators, the geometry and surface treatment of the
scintillator crystals and the electrical and optical characteristics of the photosensors. Experimental
studies were performed to assess the timing resolution and energy resolution of detectors constructed
with samples of different scintillator materials (LaBr3 , CeBr3 , LFS, LSO, LYSO: Ce, Ca and GAGG) that
were fabricated into different shapes with various surface treatments. The saturation correction of
SiPMs was applied for tested detectors based on a Tracepro simulation. Overall, we tested 28 pairs of
different forms of scintillators to determine the one with the best CTR and light output. Two common
high-performance silicon photomultipliers (SiPMs) provided by SensL (J-series, 6 mm) or AdvanSiD
(NUV, 6 mm) were used for photodetectors. The PET detector constructed with 6 mm CeBr3 cubes
achieved the best CTR with a FWHM of 74 ps. The 4 mm co-doped LYSO: Ce, Ca pyramid crystals
achieved 88.1 ps FWHM CTR. The 2 mm, 4 mm and 6 mm 0.2% Ce, 0.1% Ca co-doped LYSO cubes
achieved 95.6 ps, 106 ps and 129 ps FWHM CTR, respectively. The scintillator crystals with unpolished
surfaces had better timing than those with polished surfaces. The timing resolution was also improved
by using certain geometric factors, such as a pyramid shape, to improve light transportation in the
scintillator crystals.

Keywords: coincidence timing resolution; positron emission tomography; time of flight; light output;
energy resolution; radiation detector

1. Introduction
Positron emission tomography (PET) has become commercially available with successful
applications in oncology, cardiology and neurology [1,2]. The radiation detector is the core component
of any PET system; its performance (timing resolution, depth of interaction measurement, light output,
decoding accuracy) determines the performance of the PET system [3–6]. There are continuous efforts
to improve the spatial resolution, sensitivity and signal-to-noise ratio (SNR) in the reconstructed

Crystals 2020, 10, 869; doi:10.3390/cryst10100869 www.mdpi.com/journal/crystals

Crystals 2020, 10, 869 2 of 15

PET images since improvements in these characteristics could significantly facilitate the clinical and
preclinical applications of PET imaging [7–12].
The SNR in conventional PET images are limited by the sensitivity of the scanner. There are
two strategies to improve the sensitivity of a PET scanner. The first strategy is to increase the
geometric sensitivity of the scanner by increasing its axial extent to achieve total body coverage [13–16].
This strategy not only improves sensitivity, but it also allows the collection of metabolic and chemical
target information simultaneously from multiple organs in the body, such as the brain, lungs, heart, liver
and kidneys. The second strategy is to incorporate the additional time-of-flight (TOF) information into
the reconstruction to increase the effective sensitivity and SNR in the reconstructed images [9,10,17].
The timing resolution of a PET system is largely determined by the performance of the individual
detector modules. Many factors may affect the timing resolution of the detector modules, including the
structure of detector [18–22], the properties of the scintillator crystal (luminosity and decay time) [23,24];
the optical properties (refractive index and optical attenuation length) of the light guides and coupling
materials (air, MeltmountTM , optical glues, etc.) [25]; the surface treatment of the scintillator crystals and
light guides (saw-cutting, chemical etching and mechanical polishing to varying degrees); the optical
reflectance properties (specular and/or diffuse reflection and spectral reflection coefficient) of the
reflectors (Teflon tapes, ESR films, Lumirror films, Tyvek papers, titanium dioxide paint, multilayer
dielectric high-reflector coating, etc.); the electric and optical characteristics of the photon detectors
(photon detection efficiency, size and fill factor, etc.) [26]; and the performance of the readout electronics
(bandwidth, slew rate, signal–noise ratio, etc.) [27,28]. Photonic crystals can change the propagation
path of scintillation photons by adding microstructures on the crystal surface, thus improving the time
and energy performance of PET detector [29].
Enabled by the developments of lutetium oxyorthosilicate (LSO) and lutetium–yttrium
oxyorthosilicate (LYSO) scintillators, all three major PET manufacturers have introduced commercial
TOF PET cameras that achieve 200~600 ps full-width half-maximum (FWHM) coincidence timing
resolution (CTR). Many studies have indicated that a sub-100 ps CTR is achievable. However, there is
no literature reported clinic PET systems with a timing resolution better than 200 ps yet.
In order to help break through the barrier, we have performed extensive experimental studies
to assess the CTR of PET detectors constructed with samples of different scintillators from different
vendors that were fabricated into different shapes with various surface treatments. The basic reasoning
of the approach chosen in this study is that the CTR is a function of the photon density detected in
the initial moment of an event [20–22]. Hence the CTR can be improved through the enhancement
of the light collection efficiency by optimizing the geometry and surface treatment of the scintillator.
This article not only describes these studies in much greater detail than we previously presented at
the IEEE Nuclear Science Symposium and Medical Imaging Conference [30], but also analyzes the
experimental data in depth and compares the performances of the detectors constructed with various
scintillator materials, vendors, shapes, surface treatments and silicon photomultipliers systematically.
Practical conclusions are drawn, based on the in-depth analyses and the systematic comparisons
of the experimental data, to provide a useful guidance to the design of PET detectors with high
timing resolution.

2. Materials and Methods

2.1. PET Detector Characterization

2.1.1. Type of Scintillators

Twenty-eight pairs of scintillators with various types, sizes, shapes, surface treatments,
and manufacturers were tested for the CTR, light output and energy resolution. Six different types of
scintillator cuboids—including LYSO (Suzhou Jtcrystal, JTC), LFS (Zecotek), LSO (Siemens), GAGG
(Kinheng), LaBr3 (Saint Gobain, SG) and CeBr3 (SG)—with various sizes were tested. The coupling
surface of the scintillator cubes was polished and the other surfaces were unpolished. As shown in
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surface of the scintillator cubes was polished and the other surfaces were unpolished. As shown in
Figure 1a, the scintillators were mounted to the center of two SiPMs (MicroFJ-60035-TSV, SensL) with
Figure 1a, the scintillators were mounted to the center of two SiPMs (MicroFJ-60035-TSV, SensL) with
MeltMount optical glue (refractive index: 1.53). The 6 mm LaBr (Saint Gobain, SG) cube and 2 mm
MeltMount optical glue (refractive index: 1.53). The 6 mm LaBr33 (Saint Gobain, SG) cube and 2 mm
GAGG (Kinheng) cubes are shown in Figure 1b,c. The parameters and labels of those crystals are listed
GAGG (Kinheng) cubes are shown in Figure 1b,c. The parameters and labels of those crystals are
in Table 1.
listed in Table 1.

(a)

(b) (c)
Figure
Figure 1.
1. (a)
(a) Silicon
Silicon photomultipliers (SiPMs)and
photomultipliers (SiPMs) andscintillators;
scintillators;(b)
(b)packaged
packaged66mm
mmLaBr
LaBr 3 cubes (LaBr-
3 cubes (LaBr-6)
6) crystals; (c) GAGG-2 crystals.
crystals; (c) GAGG-2 crystals.

Table 1.1.Parameters
Table Parametersofof
thethe
lutetium–yttrium oxyorthosilicate
lutetium–yttrium (LYSO),
oxyorthosilicate lutetium
(LYSO), oxyorthosilicate
lutetium (LSO),
oxyorthosilicate
LFS, GAGG, LaBr3 and CeBr 3 crystals.
(LSO), LFS, GAGG, LaBr3 and CeBr3 crystals.

Size (mm) Size (mm) Surface Treatment of

No.
No. Labels
Labels CrystalCrystal Surface Treatment of Uncoupled Surfaces
(L × W × H) (L × W × H) Uncoupled Surfaces
01 LYSOA-4 4×4×4
01 LYSOA-4 LYSO: 0.2% Ce, 0.1% Ca co-doped 4×4×4
02 LYSOA-6 LYSO: 0.2% Ce, 0.1% Ca co-doped 6×6×6
02 LYSOA-6 6×6×6
03 LSO-6L3.7 6 × 6 × 3.7
03 LSO-6L3.7 LSO 6 × 6 × 3.7
04 LSO-6 6×6×6
LSO
04
05 LSO-6
LFS-2 2×2×2 6×6×6
Unpolished
06
05 LFS-3.7
LFS-2 LFS 3.7 × 3.7 × 3.7 2×2×2
07 LFS-4 4 × 4 × 4 3.7 × 3.7 × 3.7 Unpolished
06 LFS-3.7 LFS
08
07 GAGG-2
LFS-4 GAGG 2 × 2 × 2 4×4×4
09 LaBr-6 LaBr3 6×6×6
08
10 GAGG-2
CeBr-6 CeBr3 GAGG 6×6×6 2×2×2
09 LaBr-6 LaBr3 6×6×6
2.1.2.10Size, Doping
CeBr-6 and Surface Treatment
CeBr 6×6×6
3
Eight pairs of LYSO crystals were tested to study the timing resolutions for different sizes and
surface treatments.
2.1.2. Size, These
Doping and “labelTreatment
Surface LYSOA” crystals were made of co-doped LYSO: 0.2% Ce, 0.1% Ca
provided by JTC. The parameters of the 4 mm and 6 mm cubes (LYSOA-4 and LYSOA-6) are listed
Eight pairs of LYSO crystals were tested to study the timing resolutions for different sizes and
in Table 1. The parameters of the other six sample LYSOA crystals are listed in Table 2. Samples
surface treatments. These “label LYSOA” crystals were made of co-doped LYSO: 0.2% Ce, 0.1% Ca
LYSOA-2 (Figure 2 left), LYSOA-4 (Figure 2 middle), LYSOA-5.5 and LYSOA-6 (Figure 2 right) were
provided by JTC. The parameters of the 4 mm and 6 mm cubes (LYSOA-4 and LYSOA-6) are listed in
used to compare the timing resolutions of the scintillators of different sized cubes. Samples LYSOA-
Table 1. The parameters of the other six sample LYSOA crystals are listed in Table 2. Samples LYSOA-2
6 and LYSOA-6L3 were used to compare the timing resolutions of the scintillators of different lengths.
(Figure 2 left), LYSOA-4 (Figure 2 middle), LYSOA-5.5 and LYSOA-6 (Figure 2 right) were used to
These “sample LYSOB” crystals were made of co-doped LYSO: 0.1% Ce, 0.1% Ca provided by
compare the timing resolutions of the scintillators of different sized cubes. Samples LYSOA-6 and
JTC. Samples LYSOA and LYSOB were used to compare the timing resolutions of the scintillators
LYSOA-6L3 were used to compare the timing resolutions of the scintillators of different lengths.
with different-doped values, when comparing crystals with the same shape and size (LYSOA-4 to
LYSOB-4, LYSOA-6 to LYSOB-6).Similarly, samples LYSOA-6 (LYSOA-4) and LYSOP-6 (LYSOP-4)
Crystals 2020, 10, x FOR PEER REVIEW 4 of 16

were used to compare the timing performance of the crystals of different surface treatments. When
testing these 6 mm crystal cubes (LYSOA-6 and LYSOP-6), the bias voltage and trigger level added
Crystals 2020, 10, 869 4 of 15
to the Sensl SiPM ranged from 26 V to 32.5 V and 20 mV to 140 mV, respectively.

Table 2. Parameters
Table 2. Parameters of the LYSO
of the LYSO cube
cube crystals.
crystals.

SizeSize
(mm) (mm) SurfaceTreatment
Surface Treatmentof of
No. No. Label
Label Crystal
Crystal
(L ×(LW× ×WH) × H) Uncoupled
Uncoupled Surfaces
Surfaces
01 01 LYSOA-2
LYSOA-2 2 × 2 ×
2×2×2 2
02 LYSOA-5.5 LYSO:
02LYSOA-5.5 LYSO:0.2%
0.2% Ce,
Ce, 0.1%
0.1% Ca 5.5 5.5
× 5.5 × 5.5
× 5.5 × 5.5
03 03LYSOA-6L3 co-doped (JTC)
LYSOA-6L3 Ca co-doped (JTC) 6×6×3 3
6 × 6 ×
Unpolished
Unpolished
04 LYSOA-3L6
04LYSOA-3L6 3 × 33×× 36× 6
05 05 LYSOB-4
LYSOB-4 LYSO:0.1%
LYSO: 0.1% Ce,
Ce, 0.1%
0.1% Ca 4 × 44×× 44× 4
co-doped (JTC)
06 06 LYSOB-6
LYSOB-6 Ca co-doped (JTC) 6 × 66×× 66× 6
07 07 LYSOP-4
LYSOP-4 LYSO:0.2%
LYSO: 0.2% Ce,
Ce, 0.1%
0.1% Ca 4 × 44×× 44× 4 Polished
Polished
co-doped (JTC)
08 08 LYSOP-6
LYSOP-6 Ca co-doped (JTC) 6 × 66×× 66× 6

Figure 2.2. LYSO

LYSOcubes
cubeswith
with sizes
sizes × 2 3mm
of 2of×22 ×× 2 mm 4 × 4 × 4 mm3 (middle)
3 (left), 4 × 4 × 4
(left), mm3 (middle)
and 6 ×and 6 ×3 (right).
6 × 66 ×mm 6 mm3
(right).
These “sample LYSOB” crystals were made of co-doped LYSO: 0.1% Ce, 0.1% Ca provided by
JTC.
2.1.3.Samples
Shape LYSOA and LYSOB were used to compare the timing resolutions of the scintillators with
different-doped values, when comparing crystals with the same shape and size (LYSOA-4 to LYSOB-4,
Scintillation crystals were fabricated into different shapes (cubes, cuboids, pyramids and frusta)
LYSOA-6 to LYSOB-6).Similarly, samples LYSOA-6 (LYSOA-4) and LYSOP-6 (LYSOP-4) were used to
to investigate the effects of geometric shapes on the detector performance. Cuboid-shaped crystals
compare the timing performance of the crystals of different surface treatments. When testing these
have the disadvantage of requiring most of the photons to be reflected multiple times before being
6 mm crystal cubes (LYSOA-6 and LYSOP-6), the bias voltage and trigger level added to the Sensl SiPM
absorbed by the photodetector, which can reduce timing resolution. Therefore, we also designed and
ranged from 26 V to 32.5 V and 20 mV to 140 mV, respectively.
tested some crystals with a pyramid shape. The scintillating photons reflected from the pyramid
surface
2.1.3. will change their flight angle and emit directly to the coupling surface, which may increase
Shape
the light output and improve timing resolution. Similarly, scintillating photons in a crystal with a
zigzag Scintillation
slope maycrystals
also bewere fabricated
reflected intoslope
by the different
and shapes
directly(cubes,
emit tocuboids, pyramids
the coupling and frusta)
surface. Tableto3
investigate
shows the parameters of the six odd-shaped scintillation crystals, where LYSOP indicateshave
the effects of geometric shapes on the detector performance. Cuboid-shaped crystals the
the disadvantage crystal,
pyramid-shaped of requiring mostindicates
LYSOH of the photons to bewith
the crystal reflected multiple timestop,
a pyramid-shaped before
LYSOFbeingindicates
absorbeda
by the photodetector,
frustum-shaped which
crystal, LYSOTcanindicates
reduce timing resolution. Therefore,
a pyramid-shaped top crystalwe also
with designedsurface
a sawtooth and tested
and
some crystals with a pyramid shape. The scintillating photons reflected from
LYSOTP indicates the crystals with two pyramids. Figure 3a,b show the pictures of LYSOF-6,the pyramid surface will
change their flight angle and emit directly to the coupling surface, which may increase
LYSOH-6, LYSOP-4 and LYSOT-6 and LYSOTP-6 crystals, respectively. Figure 4 shows the design the light output
and improveoftiming
dimensions variousresolution. Similarly, scintillating photons in a crystal with a zigzag slope may
shaped crystals.
also be reflected by the slope and directly emit to the coupling surface. Table 3 shows the parameters of
the six odd-shaped scintillation crystals, where LYSOP indicates the pyramid-shaped crystal, LYSOH
indicates the crystal with a pyramid-shaped top, LYSOF indicates a frustum-shaped crystal, LYSOT
indicates a pyramid-shaped top crystal with a sawtooth surface and LYSOTP indicates the crystals
with two pyramids. Figure 3a,b show the pictures of LYSOF-6, LYSOH-6, LYSOP-4 and LYSOT-6 and
LYSOTP-6 crystals, respectively. Figure 4 shows the design dimensions of various shaped crystals.

2.1.4. Position and Manufacturer

Four pairs of scintillators were tested to investigate differences in boule position and manufacturers.
When a crystal is cut from different positions of the scintillator boule, its performance may also be
different. Therefore, we tested two 2 mm, 0.2% co-doped LYSO with Ce and Ca crystal cuboids
(LYSOAH-2 and LYSOAT-2), which were taken from the tail or head of the same crystal boule.
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Crystals 2020, 10, 869 5 of 15

Table
Table 3.
3. Parameters
Parameters of
of the
the odd-shaped
odd-shaped LYSO
LYSO crystals.
crystals.
Table 3. Parameters of the odd-shaped LYSO crystals.
Surface Treatment of
No. Label Crystal Size Surface Treatment of
No. Label Crystal Size Uncoupled Surfaces
Uncoupled
Surface Surfaces
Treatment of
01 No. Label
LYSOP-4 Crystal Size
Figure
01 LYSOP-4 Figure 4a4a Uncoupled Surfaces
02
02 LYSOP-6
LYSOP-6
01 LYSOP-4 Figure
Figure 4b
Figure 4b
4a Polished
Polished
03
03 02 LYSOP-6LYSO:
LYSOH-6
LYSOH-6 LYSO: 0.2%
0.2% Ce,
Ce, 0.1%
0.1% Ca
Ca co-
co- Figure
Figure 4c
Figure 4b
4c Polished
04 03 LYSOH-6
LYSOF-6 LYSO: 0.2%
doped Ce, 0.1% Ca Figure4d4c
04 LYSOF-6 doped (JTC)
(JTC) Figure
Figure 4d
04 LYSOF-6 co-doped (JTC) Figure 4d
05
05 LYSOT-6
LYSOT-6 Figure
Figure 4e4e Unpolished
Unpolished
06
06 05 LYSOT-6
LYSOTP-6
LYSOTP-6 Figure 4f
Figure
Figure 4e
4f Unpolished
06 LYSOTP-6 Figure 4f

(a)
(a)

(b)
(b)
Figure
Figure 3.
3. (a)
3. (a) LYSOF-6
LYSOF-6 (left),
(left), LYSOH-6
LYSOH-6 (middle)
(middle) and
and LYSOP-4
LYSOP-4 (right)
(right) crystals;
crystals; (b)
(b) LYSOT-6
LYSOT-6 (left)
(left) and
and
and
LYSOTP-6
LYSOTP-6 (right)
(right) crystals.
crystals.
LYSOTP-6 (right) crystals.

(a)
(a) (b)
(b) (c)
(c)

(d)
(d) (e)
(e) (f)
(f)
Figure
Figure 4.4. Shape
4.Shape
Shapeandand
and size
size of the
the odd-shaped
of odd-shaped
odd-shaped scintillator
scintillator configurations.
configurations. (a)
(a) LYSOP-4
LYSOP-4 crystal,
crystal, (b)
(b)
Figure size of the scintillator configurations. (a) LYSOP-4 crystal, (b) LYSOP-6
LYSOP-6
LYSOP-6 crystal,
crystal, (c)
(c) LYSOH-6
LYSOH-6 crystal,
crystal, (d)
(d) LYSOF-6
LYSOF-6 crystal,
crystal, (e)
(e) LYSOT-6
LYSOT-6 crystal
crystal and
and (f)
(f) LYSOTP-6
LYSOTP-6
crystal, (c) LYSOH-6 crystal, (d) LYSOF-6 crystal, (e) LYSOT-6 crystal and (f) LYSOTP-6 crystal.
crystal.
crystal.

2.1.4.
2.1.4. Position
Position and
and Manufacturer
Manufacturer
boule.
Finally, sample C crystals were made of LYSO crystal provided by SG. These crystals were used
to compare the timing resolution of equivalent LYSO crystals from different manufacturers. The
parameters of those crystals are listed in Table 4.
Crystals 2020, 10, 869 6 of 15

Table 4. Parameters of the LYSO taken from different positions of the crystal boule.
Finally, sample C crystals were made of LYSO crystal provided by SG. These crystals were
Size (mm) Surface Treatment of Uncoupled
No. used to
Label Crystal of equivalent LYSO crystals from different manufacturers.
compare the timing resolution (L × W × H) Surfaces
01 TheLYSOAH-2
parameters of0.2%
those
Cecrystals
co-dopedare listed
LYSO in Table
(from 4.
head boule)
2×2×2
02 LYSOAT-2 0.2% Ce co-doped LYSO (from tail boule)
Unpolished
03 LYSOC-3.7Table 4. Parameters of the LYSO taken from different
3.7positions of the crystal boule.
× 3.7 × 3.7
LYSO crystal (SG)
04 LYSOC-5 5×5×5
Size (mm) Surface Treatment of
No. Label Crystal
(L × W × H) Uncoupled Surfaces
2.2. Experimental Setting 0.2% Ce co-doped LYSO
01 LYSOAH-2
(from head boule) 2×2×2
An experimental system with excellent timing resolution was constructed in this study. As
0.2% Ce co-doped LYSO Unpolished
02 LYSOAT-2
shown in Figure 5, the system consists
(from tailofboule)
two PET detectors, a Keithley 2400 source meter, two
custom-designed
03 amplifier
LYSOC-3.7 boards, two leading edge discriminators
3.7 × 3.7 × 3.7 (LEDs), a time-to-amplitude
LYSO crystal (SG)
converter (TAC),
04 an NI PCI-7833R board and a PC. Each custom-designed
LYSOC-5 5×5×5 amplifier board split the
signal from the SiPM into an energy signal and a timing signal and then amplified them. Two stages
2.2. Experimental
of current feedbackSetting amplifiers (AD8000, Analog Devices, Inc.) were used to amplify the timing
signals with a total gain system
An experimental of 200.with
Theexcellent
−3 dB bandwidth and the
timing resolution wasslew rate of in
constructed thethis
amplifier
study. Asare 1.5 GHz
shown
and in4100 V/μs,
Figure 5, therespectively.
system consists The amplified
of two timing
PET detectors, signals2400
a Keithley were fed meter,
source to two twoLEDs (CANBERRA®,
custom-designed
Model 454). Note
amplifier boards,thattwotheleading
Modeledge
454 discriminators
is a device with four channels
(LEDs), of conventional
a time-to-amplitude converter constant
(TAC), an fractional
NI
PCI-7833R board
discriminators (CFDs). andWe a PC.
haveEach custom-designed
modified its internalamplifier
circuits andboard split the the
converted signal
fourfrom
CFDs theinto
SiPM LEDs.
into an energy signal and a timing signal and then amplified them.
The outputs of the LEDs were fed to the TAC (ORTEC , Model 566), which measured the time
® Two stages of current feedback
amplifiers
interval between(AD8000,
pulsesAnalog
to Devices,
its startInc.)
andwerestopused to amplify
inputs and the timing signals
generated with a total
an analog gain ofpulse
output
200. The −3 dB bandwidth and the slew rate of
proportional to the measured time. The full scale of the TAC was the amplifier are 1.5 GHz and 4100 V/µs, respectively.
set to 50 ns and the FWHM of the
The amplified timing signals were fed to two LEDs (CANBERRA® , Model 454). Note that the Model
timing resolution of the Model 566 TAC was 10 ps for all ranges according to the datasheet. The
454 is a device with four channels of conventional constant fractional discriminators (CFDs). We have
outputs of the TAC and the amplified energy signals were connected to the NI PCI-7833R board, a
modified its internal circuits and converted the four CFDs into LEDs. The outputs of the LEDs were
PCI-based reconfigurable
fed to the TAC (ORTEC®I/O device
, Model with
566), whicha FPGA
measured andthe eight
timeanalog-to-digital converters
interval between pulses on-board.
to its start and
A LabVIEW program was developed to control the FPGA to perform
stop inputs and generated an analog output pulse proportional to the measured time. The full scaleevent triggering and of read
out the energy
the TAC wasand timing
set to signals.
50 ns and The timing
the FWHM resolution
of the timing of theofreadout
resolution the Model electronics
566 TAC was were 10 calibrated
ps for
withall
pulses
ranges generated
accordingfrom to theadatasheet.
signal generator.
The outputsTheof timing
the TACresolution of the readout
and the amplified energyelectronic
signals were system
was connected
12.7 ps ±to0.1 thepsNI(mean
PCI-7833R± standard deviation),
board, a PCI-based which is only
reconfigurable slightly
I/O device withworse
a FPGA than andthe timing
eight
analog-to-digital
resolution of the Model converters on-board.
566 TAC.

Figure 5. Schematic
Figure 5. Schematicofofthe
theexperimental setupwith
experimental setup withreadout
readout electronics.
electronics.

A LabVIEW program was developed to control the FPGA to perform event triggering and read
out the energy and timing signals. The timing resolution of the readout electronics were calibrated with
pulses generated from a signal generator. The timing resolution of the readout electronic system was
Crystals 2020, 10, 869 7 of 15

12.7 ps ± 0.1 ps (mean ± standard deviation), which is only slightly worse than the timing resolution of
the Model 566 TAC.
The new high-density (HD) cell SiPM (AdvanSiD) coupled to 6 mm LaBr3 crystal cubes (Table 1)
was tested at different bias voltages and trigger levels. This is a highly sensitive photon detector in
the near-ultraviolet (NUV) and blue light regions. The SiPM size was 6 × 6 mm2 with 40,000 cells of
20 × 20 µm2 cell pitch. The bias voltage and trigger level added to the AdvanSiD SiPM ranged from
36 V to 39 V and 10 mV to 350 mV, respectively. The bias voltage and trigger level added to the Sensl
SiPM ranged from 26 V to 32.5 V and 20 mV to 140 mV, respectively. The energy spectrum and time
spectrum of each experiment were recorded.
Two detectors using identical scintillator crystal configurations were mounted head-to-head with
a 10 mm gap with a 22 Na point source (Eckert and Ziegler, 0.74 MBq) centrally located between them for
coincidence imaging. Unless otherwise stated, the scintillators were wrapped with the same reflector
(Teflon tape), coupled with using the same optical glue (MeltMount) with the same pair of SiPMs
(6 mm SensL J-series) and tested with the same readout electronics with identical settings in terms of
bias voltage (31.5 V), amplifier gain (200) and trigger level (40 mV). Note that we used MeltMount glue
to construct the detectors. Thus, we were able to mount and unmount the scintillators conveniently
and use the same pair of SiPMs repeatedly.
Approximately one million coincidence events were acquired for each coincidence pair of
scintillator crystals within the energy window of 450 keV to 550 keV and were analyzed for the
time spectrum and calculation of CTR. The trigger time differs for coincidence events with the same
rise time, but different energy peaks. Therefore, the timing measurements were not accurate when
the leading-edge discriminator was implemented, especially for the large range of energy windows.
Therefore, the energy value of coincidence events was used to correct the time signal. The timing
resolution was raised by approximately 10% after compensation. Typically, the FWHM of the peak of
the time spectrum was calculated as the timing resolution of the coincidence event.

2.3. Saturation Correction

The saturation correction of SiPMs was applied for all the tested detectors based on Tracepro
simulation; the correction process is shown in Figure 6a. First, the Tracepro was used to optically
simulate the interaction of gamma photons in the scintillators, track the scintillation photons and get
the simulated light output. The characteristic parameters of those scintillators in the simulation are
shown in Table 5, which was provided by the vendors. The SiPM has different detection efficiency for
photons with different wavelength (λ). In the simulation, when λ is 420 nm, the detection efficiency is
up to 52%. Depending on the crystal specifications, scintillation photons from 2300 to 7000 (the area
between the two red vertical lines) can eventually reach the coupled SiPM.
Second, according to the cross-sectional area of the scintillators, the conversion function between
the reached photons number and the detected photons number was obtained through Matlab modeling.
The SensL MicroFJ-60035-TSV SiPM has 22,292 microcells. Figure 6b shows the conversion function
curves when the crystal coupling area are 2 × 2 mm2 , 4 × 4 mm2 and 6 × 6 mm2 , respectively, taking into
account of the influence of the thickness of optical glue (0.1 mm) and protective glass (0.35 mm) on
SiPM, corresponding coupling microcells are about 5.8 k, 15.9 k and 22 k, respectively. In the simulation,
we assume that the scintillating photons simultaneously reach the avalanche diode in the SiPM.
Third, the light output obtained by the Tracepro was converted into the light output actually
detected by SiPM through the conversion function. Finally, the uncorrected measured energy spectrum
was converted into corrected energy spectrum by matching the peak position of 511 keV with simulated
light output. The corrected light outputs and energy resolutions were calculated from the corrected
energy spectrum.
 Crystals 2020, 10, x FOR PEER REVIEW 8 of 16
Crystals 2020, 10, 869 8 of 15
Crystals 2020, 10, x FOR PEER REVIEW 8 of 16

(a)
(a) (b)
(b)
Figure
Figure6.6.(a)
(a)Flowchart
Flowchartof
ofthe
the saturation correction;(b)
saturation correction; (b)conversion
conversionfunction.
function.
Figure 6. (a) Flowchart of the saturation correction; (b) conversion function.
Table
Table 5.5.5.Characteristic
Table Characteristic
Characteristic parameters
parameters of
parametersof the
ofthe tested
tested
the crystals.
crystals.
tested crystals.
Peak
PeakEmission
Emission Refractive
Refractive DecayTime
Decay Time Absolute
Absolute Light
Light Output
Output
Crystal
Crystal Peak Emission Absolute Light Output
Crystal Wavelength
Wavelength (nm) Refractive
(nm) Index
Index Index Decay Time (ns) (10(10
(ns)
(ns) 3 Photon/MeV)
3 Photon/MeV)
Wavelength (nm) (103 Photon/MeV)
0.2% co-doped
0.2% co-doped LYSO
LYSO 420
420 1.82
1.82 35
35 32 32
0.2% co-doped LYSO 420 1.82 35 32
0.1%
0.1% co-doped
co-doped LYSO
LYSO 420
420 1.82
1.82 41
41 39 39
0.1% co-doped LYSO 420 1.82 41 39
LFS
LFS 420
420 1.82
1.82 35
3535 38 38
LFS 420 1.82 38
LSO
LSO
LSO 420
420
420 1.82
1.82
1.82 40
4040 30 3030
GAGG
GAGG
GAGG 530
530
530 1.9
1.9
1.9 50
5050 32 3232
LaBr
LaBr
LaBr 33
3 370370
370 1.9
1.9
1.9 16
1616 60 6060
CeBr
CeBr
CeBr3 3 3 380380
380 1.9
1.9
1.9 17
17 17 68 6868

3. Results
3. 3. Results
Results
3.1. Photodetectors
3.1.
3.1. Photodetectors
Photodetectors
First, we compared the performance of the 6 mm SensL J-series SiPMs (Figure 7a) with the 6 mm
First,
First,
AdvanSiDwewecompared
comparedthe
NUV SiPMs
the performance
performance
(Figure of the
7b) by using
66 mm
a pairmm SensL
of 6SensL
J-series
J-series
mm LaBr
SiPMs
SiPMs(Figure
(Figure 7a)7a)
with
3 cubes (LaBr-6). The FWHM CTRs
thethe
with 6 mm
6 mm
AdvanSiD
AdvanSiD NUV SiPMs (Figure 7b) by using a pair of 6 mm LaBr 3 cubes (LaBr-6).
were represented by the colors and contour lines. The SensL SiPM 3without time walk compensationCTRs
NUV SiPMs (Figure 7b) by using a pair of 6 mm LaBr cubes (LaBr-6). The
The FWHM
FWHM CTRs
were represented
wereachieved
represented byby
its best thecolors
the colorstiming
coincidence andcontour
and contour lines.
lines.
resolution The
ps SensL
The
of 77 SensLSiPM
FWHM whenwithout
SiPM bias time
without
the walk
time
voltage wascompensation
walk compensation
31.5 V and
achieved its
the trigger
achieved best coincidence
levelcoincidence
its best timing
was 40 mV. Similarly, resolution of
the AdvanSiD
timing resolution 77 ps
SiPM
of 77 FWHM when
pswithout
FWHMtime the
when bias
walkthe voltage
compensation wasachieved
bias voltage 31.5
wasV and
31.5 V
the
and itstrigger
thebest level
CTR of
trigger was 40
75 pswas
level mV.
FWHM Similarly,
when
40 mV. the AdvanSiD
the bias voltage
Similarly, SiPM without
was 38.5 V SiPM
the AdvanSiD time
and thewithoutwalk compensation
trigger level
timewas 75 mV.
walk achieved
These
compensation
its results
best CTR
achieved its of 75CTR
showed
best ps FWHM
that the
of 75 when
twopsSiPMs
FWHMthehadbias
no voltage was
significant
when the bias 38.5 V and
differences
voltage inthe
was trigger
timing
38.5 levelthe
resolution.
V and was 75 mV.level
Therefore,
trigger These
the was
results
6 mmshowed that the
SensL SiPMs weretwo SiPMs
used in allhad no significant
of the tests describeddifferences
below. in timing resolution. Therefore, the
75 mV. These results showed that the two SiPMs had no significant differences in timing resolution.
6 mm SensL SiPMs were used in all of the tests described below.
Therefore, the 6 mm SensL SiPMs were used in all of the tests described below.

(a) (b)
Figure 7. Contour plots
(a) of the FWHM CTR. (a) SensL J-series SiPMs; (b) AdvanSiD
(b) NUV HD SiPMs.
Figure7.7.Contour
Figure Contourplots
plotsof
of the
the FWHM
FWHM CTR.
CTR. (a)
(a)SensL
SensLJ-series
J-seriesSiPMs;
SiPMs;(b) AdvanSiD
(b) NUV
AdvanSiD HDHD
NUV SiPMs.
SiPMs.
3.2. Surface Treatment
LYSO samples LYSOA-6 and LYSOP-6 were used to compare the timing resolution of the
crystals of different surface treatments. For these tests, the bias voltage and trigger level added to the
Crystals 2020, 10, 869 9 of 15
SiPM ranged from 26 V to 32.5 V and 20 mV to 140 mV, respectively. The best CTR of the polished
crystal was 146 ps with a bias voltage of 31 V and a trigger level of 40 mV (Figure 8a). The best CTR
of
3.2.the unpolished
Surface crystal was 129 ps with a bias voltage of 31.5 V and a trigger level of 40 mV (Figure 8b).
Treatment
Clearly, the timing resolution of the unpolished crystal is better than that of the polished crystal,
LYSO samples LYSOA-6 and LYSOP-6 were used to compare the timing resolution of the crystals
regardless of the bias voltage and the trigger level. When the cubic crystal surface is absolutely
of different surface treatments. For these tests, the bias voltage and trigger level added to the SiPM
smooth, nearly half of the scintillating photons are not received by the SiPM due to total internal
ranged from 26 V to 32.5 V and 20 mV to 140 mV, respectively. The best CTR of the polished crystal
reflection (TIR). In contrast, the unpolished surface can change the flight angle of the scintillating
was 146 ps with a bias voltage of 31 V and a trigger level of 40 mV (Figure 8a). The best CTR of the
photons, thereby breaking the limit of the TIR and increasing the light output and timing resolution.
unpolished crystal was 129 ps with a bias voltage of 31.5 V and a trigger level of 40 mV (Figure 8b).

(a) (b)
Figure 8.
8. Contour
Contourplots of of
plots thethe
FWHM CTR
FWHM of 0.2%
CTR co-doped
of 0.2% LYSO.
co-doped (a) Polished
LYSO. crystal;
(a) Polished (b)
crystal;
unpolished crystal.
(b) unpolished crystal.

Clearly,
3.3. Timing andtheEnergy
timing resolution of the unpolished crystal is better than that of the polished crystal,
regardless of the bias voltage and the trigger level. When the cubic crystal surface is absolutely
3.3.1.
smooth, Type of Scintillators
nearly half of the scintillating photons are not received by the SiPM due to total internal
reflection (TIR). In contrast, the unpolished surface can change the flight angle of the scintillating
The cubic crystals listed in Tables 1 and 2 were used to investigate how the CTR varied with the
photons, thereby breaking the limit of the TIR and increasing the light output and timing resolution.
scintillator material. The CTRs of those cubic crystals are shown in Figure 9a. The timing resolution
of
3.3.the halogen
Timing andcrystal
Energy(LaBr-6:77 ps, CeBr-6:74 ps) was the best as shown in Figure 9b and the GAGG
crystal (193 ps) was the worst. The timing resolution of the other crystals were at the same level. In
detail, the CTRs
3.3.1. Type of LFS-2, LFS-3.7 and LFS-4 were 119 ps, 126.4 ps and 142.8 ps, respectively, which
of Scintillators
was worse than those of the 0.2% Ce, 0.1% Ca co-doped LYSO for the same size. The CTRs of LYSO-
The cubic crystals listed in Tables 1 and 2 were used to investigate how the CTR varied with the
3.7 (SG), LYSO-5 (SG) and LSO-6 were 110.1 ps, 126.7 ps and 132.9 ps, respectively. In general, the
scintillator material. The CTRs of those cubic crystals are shown in Figure 9a. The timing resolution of
larger the cubic crystal, the worse the timing resolution tends to be. The relative light outputs and
the halogen crystal (LaBr-6:77 ps, CeBr-6:74 ps) was the best as shown in Figure 9b and the GAGG crystal
energy resolutions of cubic crystals with the same surface treatments are shown in Figure 9c,d with
(193 ps) was the worst. The timing resolution of the other crystals were at the same level. In detail,
corrected for saturation effects of SiPMs. The light output of the 4 mm 0.2% co-doped LYSO cubic
the CTRs of LFS-2, LFS-3.7 and LFS-4 were 119 ps, 126.4 ps and 142.8 ps, respectively, which was
(LYSOA-4) crystal was used as a reference and it was set to 100%. Similar, the larger the cubic crystal,
worse than those of the 0.2% Ce, 0.1% Ca co-doped LYSO for the same size. The CTRs of LYSO-3.7
the worse the light output tend to be.
(SG), LYSO-5 (SG) and LSO-6 were 110.1 ps, 126.7 ps and 132.9 ps, respectively. In general, the larger
the cubic crystal, the worse the timing resolution tends to be. The relative light outputs and energy
resolutions of cubic crystals with the same surface treatments are shown in Figure 9c,d with corrected
for saturation effects of SiPMs. The light output of the 4 mm 0.2% co-doped LYSO cubic (LYSOA-4)
crystal was used as a reference and it was set to 100%. Similar, the larger the cubic crystal, the worse
the light output tend to be.

3.3.2. Size, Doping and Surface Treatment

Figure 10a shows the CTR for the cuboid-shaped LYSO crystals listed in Table 2. Investigating
the size of the crystal cubes, the CTR of the 2 mm cube crystal was better than that of the 6 mm cube
crystal and the CTRs of the 4 mm cube crystals were in between (Figure 10a). In long crystals, the time
distribution of the photons (particularly the first photons) reaching the photodetector is wider, due to
a larger distribution of the photon pathways. Thus, larger time jitters were introduced in the long
crystals. Consistently, the larger the scintillator, the lower the light output (Figure 10b). The 4 mm
cubic crystal achieved the best energy resolution as shown in Figure 10c.
 3.7 (SG), LYSO-5 (SG) and LSO-6 were 110.1 ps, 126.7 ps and 132.9 ps, respectively. In general, the
larger the cubic crystal, the worse the timing resolution tends to be. The relative light outputs and
energy resolutions of cubic crystals with the same surface treatments are shown in Figure 9c,d with
corrected for saturation effects of SiPMs. The light output of the 4 mm 0.2% co-doped LYSO cubic
(LYSOA-4) crystal was used as a reference and it was set to 100%. Similar, the larger the cubic crystal,
Crystalsthe
2020, 10, 869
worse the light output tend to be. 10 of 15

(a) (c)

(d)
9. (a)9.CTR
FigureFigure values,
(a) CTR (b)(b)time
values, timespectrum ofthe
spectrum of the6 6mm
mm CeBr
CeBr 3 cube;
3 cube; (c) relative
(c) relative light outputs
light outputs and (d) and
energy resolutions of cubic crystal.
(d) energy resolutions of cubic crystal.
Crystals 2020, 10, x FOR PEER REVIEW 11 of 16

3.1.2. Size, Doping and Surface Treatment

Figure 10a shows the CTR for the cuboid-shaped LYSO crystals listed in Table 2. Investigating
the size of the crystal cubes, the CTR of the 2 mm cube crystal was better than that of the 6 mm cube
crystal and the CTRs of the 4 mm cube crystals were in between (Figure 10a). In long crystals, the
time distribution of the photons (particularly the first photons) reaching the photodetector is wider,
due to a larger distribution of the photon pathways. Thus, larger time jitters were introduced in the
long crystals. Consistently, the larger the scintillator, the lower the light output (Figure 10b). The 4
mm cubic crystal achieved the best energy resolution as shown in Figure 10c.

(a) (b)

(c)

Figure 10.Figure 10. (a)(b)

(a) CTRs, CTRs, (b) relative
relative lightlight outputs
outputs andand
(c)(c)energy
energy resolutions
resolutions of of
2 mm, 4 mm
2 mm, and 6and
4 mm mm6 mm side
side LYSO cubes crystal.
LYSO cubes crystal.
Investigating the size of the rectangular-prism crystals, the CTRs of LYSOA-6L3, LYSOA-3L6
and LSO-6L3.7 were 119 ps, 128.4 ps and 127.8 ps, respectively. By comparing LYSOA-6L3 and
LYSOA-6, it can be inferred that a short crystal length can achieve a better timing resolution when
the cross section is the same.

3.3.3. Shape
 Crystals 2020, 10, 869 11 of 15

Investigating the doping and surface treatment, the timing resolution of the 0.2% Ce co-doped
LYSO crystals (LYSOA-4 and LYSOA-6) were better than that of the matching 0.1% Ce co-doped LYSO
crystals (LYSOB-4 and LYSOB-6). However, the light output of the 0.2% Ce co-doped crystals were
lower than that of 0.1% Ce co-doped LYSO crystals. The energy resolution of the 0.2% Ce co-doped
LYSO were similar with that of 0.1% Ce co-doped LYSO crystals. In addition, the unpolished 4 mm
and 6 mm crystal cubes (LYSOA-4 and LYSOA-6, the black line in Figure 10a,b) had better light output
and timing performance than that of the equivalent polished crystals (LYSOP-4 and LYSOP-6, the red
line in Figure 10a,b).
Investigating the size of the rectangular-prism crystals, the CTRs of LYSOA-6L3, LYSOA-3L6 and
LSO-6L3.7 were 119 ps, 128.4 ps and 127.8 ps, respectively. By comparing LYSOA-6L3 and LYSOA-6,
it can be inferred that a short crystal length can achieve a better timing resolution when the cross
section is the same.

3.3.3. Shape
The CTR and relative light output of six types of odd-shaped 0.2% co-doped LYSO crystals
(LYSOH-6, LYSOP-4, LYSOF-6, LYSOP-6, LYSOT-6, LYSOTP-6) are shown in Figure 11a. The CTR
and light output of the LYSOP-4 and LYSOP-6 crystals were better than those of the reference sample
LYSOA-6 crystal, which illustrates that the tapered structure may contribute to improve timing
resolution and light output. However, the performance of several other odd-shaped crystals (LYSOF-6,
LYSOH-6, LYSOT-6, LYSOTP-6) were on the same level as the 6 mm crystal cube. The typical time
spectrum
Crystals 2020, 10, of the LYSOP-4
x FOR crystal is shown in Figure 11b.
PEER REVIEW 12 of 16

Figure 11. (a)

Figure 11. CTR andand
(a) CTR thethe
relative
relativelight
lightoutput six types
output of six typesofofodd
odd crystals
crystals (blue
(blue points);
points); (b) time
(b) time
spectrum
spectrum of LYSOP-4.
of LYSOP-4.
3.3.4. Position and Manufacturer
3.3.4. Position and Manufacturer
Investigating the scintillator manufacturers, the CTRs of the cubic crystals LYSOC-3.7 and
Investigating
LYSOC-5.5 the scintillator
supplied by SG were manufacturers,
110.1 ps and 126.7 the
ps,CTRs of the This
respectively. cubicresult
crystals LYSOC-3.7
confirms that the and
LYSOC-5.5 supplied
smaller the by SG
crystal cube, thewere
better110.1 ps and
the timing 126.7 ps,
resolution. Therespectively.
crystal was at This result
the same levelconfirms that the
as the timing
smaller the crystal
resolution cube,
and light the of
output better the timing
the crystal providedresolution.
by JTC. The crystal was at the same level as the
Investigating the position of the crystal within
timing resolution and light output of the crystal provided the boule,bythe CTRs of LYSOAH-2 and LYSOAT-2
JTC.
were 110.2 ps and
Investigating the99.1 ps, respectively.
position Thesewithin
of the crystal crystals were
the taken
boule, from
the different
CTRs positions ofand
of LYSOAH-2 theLYSOAT-
same
crystal boule, which shows that crystal taken from the tail of the crystal boule may
2 were 110.2 ps and 99.1 ps, respectively. These crystals were taken from different positions of theachieve a better
sametiming resolution.
crystal boule, which shows that crystal taken from the tail of the crystal boule may achieve a
better timing resolution.

4. Summary and Discussion

The CTRs, corrected energy resolution and corrected relative light outputs of the tested
scintillator detectors are summarized in Table 6. The sample CeBr-6 achieved the best CTR (74 ps)
Crystals 2020, 10, 869 12 of 15

4. Summary and Discussion

The CTRs, corrected energy resolution and corrected relative light outputs of the tested scintillator
detectors are summarized in Table 6. The sample CeBr-6 achieved the best CTR (74 ps) and the GAGG-2
crystal achieved the worst CTR (193 ps). The LaBr-6 crystal achieved the best relative light output (1.75)
and the GAGG-2 crystal achieved the worst relative light output (0.65). The LaBr-6 crystal achieved the
best energy resolution (6.4%) and the LYSOTP-6 crystal achieved the worst energy resolution (12.9%).
Figure 12 shows a comparison of the CTR and the light output for all of test crystals except LaBr-6
and CeBr-6. There is a general trend, that the larger the light output of the crystal, the better the time
performance. The timing resolution and light output of several rhenium silicate-based crystals (LYSO,
LFS, LFS, etc.) are at the same level.
The CTR of the 2 mm GAGG cubes was 193 ps. However, we note that the SensL SiPM had a much
lower photon detection efficiency (PDE) for 530 nm compared to that for 420 nm. Thus, the measured
light output from GAGG was 47% lower than that of LYSO. According to the relationship between the
CTR and the light output of the crystal, the CTR of the 2 mm GAGG cubes improves to 117 ps if the
effect of the low PDE for 530 nm was compensated.
The idea for an odd-shaped crystal came from the study of photonics crystals, which are a kind of
micronano structure on the crystal surface that guides and controls the propagation of scintillating
photons to increase the light output and time performance of the detector. The macroscopic structure
does not meet the expectations, but it is possible when the profiled structure is on the nanometer scale.

Table 6. Testing results of all the scintillator detectors.

Surface Cube Size (mm) Energy Relative Light

No. Label CTR (ps)
Treatment (L × W× H) Resolution Output
1 LYSOA-4 4×4×4 8.4% 1 106
2 LYSOA-6 6×6×6 8.9% 0.88 129
3 LSO-6L3.7 6 × 6 × 3.7 10.7% 0.88 127.8
4 LSO-6 6×6×6 10.4% 0.85 132.9
5 LFS-2 Unpolished 2×2×2 12.5% 1.14 119
6 LFS-3.7 3.7 × 3.7 × 3.7 8.9% 1.04 126.4
7 LFS-4 4×4×4 10.2% 0.93 142.8
8 GAGG-2 2×2×2 10.7% 0.65 193
9 LaBr-6 6×6×6 6.4% 1.75 77
10 CeBr-6 6×6×6 NA NA 74
11 LYSOA-2 2×2×2 11.8% 1.03 95.6
12 LYSOA-5.5 5.5 × 5.5 × 5.5 8.4% 0.87 127
13 LYSOA-6L3 6×6×3 9.8% 0.78 119
Unpolished
14 LYSOA-3L6 3×3×6 9.5% 0.94 128.4
15 LYSOB-4 4×4×4 8.7% 1.14 127.1
16 LYSOB-6 6×6×6 9.7% 1.01 138.9
17 LYSO-P4 4×4×4 7.8% 0.90 124
Polished
18 LYSO-P6 6×6×6 8.3% 0.82 146
19 LYSOP-4 Figure 4a 7.6% 1.21 88.1
20 LYSOP-6 Figure 4b 7.7% 1.25 94.5
21 LYSOH-6 Figure 4c 10.8% 0.83 131.5
Polished
22 LYSOF-6 Figure 4d 11.2% 0.83 125.8
23 LYSOT-6 Figure 4e 10.6% 0.79 165
24 LYSOTP-6 Figure 4f 12.9% 0.83 187.6
25 LYSOAH-2 2×2×2 12.2% 0.98 110.2
26 LYSOAT-2 2×2×2 12.9% 0.92 99.1
Unpolished
27 LYSOC-3.7 3.7 × 3.7 × 3.7 10.6% 0.98 110.1
28 LYSOC-5 5×5×5 9.9% 0.89 126.7
 21 LYSOH-6 Figure 4c 10.8% 0.83 131.5
Polished
22 LYSOF-6 Figure 4d 11.2% 0.83 125.8
23 LYSOT-6 Figure 4e 10.6% 0.79 165
24 LYSOTP-6 Figure 4f 12.9% 0.83 187.6
25 LYSOAH-2 2×2×2 12.2% 0.98 110.2
26 LYSOAT-2 2×2×2 12.9% 0.92 99.1
Crystals 2020, 10,27869 Unpolished 13 of 15
LYSOC-3.7 3.7 × 3.7 × 3.7 10.6% 0.98 110.1
28 LYSOC-5 5×5×5 9.9% 0.89 126.7

Figure 12. Comparison of the CTR and corrected light output for tested crystals.
Figure 12. Comparison of the CTR and corrected light output for tested crystals.
The CTR of the 2 mm GAGG cubes was 193 ps. However, we note that the SensL SiPM had a
In this study,
much the
lower number
photon of samples
detection efficiencyfor all configurations
(PDE) is small,
for 530 nm compared to that and some
for 420 nm. results
Thus, themay not be
representative. Especially when the crystals were taken from different positions of the crystal boule
(LYSOAH-2 and LYSOAT-2), the difference of CTR may not be as big as tested. The sensitivity of the
PET scanners is related to the length of the crystal. In a typical commercial PET scanner, the length of
the crystal is approximately 20 mm. It is possible to build a TOF-PET detector with three layers of
scintillators. While the detector meets the sensitivity requirements of the PET scanner, the measured
CTRs are expected to drop below 70 ps.

5. Conclusions
In summary, we can conclude from the testing results that: (1) a 74 ps FWHM CTR was measured
with a pair of 6 mm side CeBr3 cubes. It is possible to achieve a CTR below 50 ps if the PET detector
is constructed by smaller LaBr3 crystals; (2) an 88.1 ps FWHM CTR was measured with a pair of
4 mm LYSO: Ce, Ca pyramids, which shows that a change in the shape of the crystal can improve the
timing resolution; (3) the two SiPMs from SensL and AdvanSiD have no significant differences with
respect to timing resolutions; (4) the crystals with unpolished surfaces have better timing than those
with polished surfaces; (5) LYSO: Ce, Ca from different venders and LSO from Siemens have similar
performances; (6) 0.2% co-doped LYSO crystals have a better CTR than that of 0.1% Ce co-doped
LYSO; (7) 0.2% co-doped LYSO crystals have a better timing resolution than that of LFS; (8) the CTR
measurements are related to the size of the crystals. The 2 mm crystals have better timing than 4 mm
crystals and the 4 mm crystals have better timing than 6 mm crystals.
The conclusions drawn from these experimental studies provide some practical guidance in terms
of the design of PET detectors with high timing resolution. However, many other practical factors,
including costs, detector efficiency or stopping power, accuracy of the decoding of the positions of
gamma interaction and effects of Compton scatters, need to be considered and carefully balanced,
Crystals 2020, 10, 869 14 of 15

when designing PET detectors for different applications such as the whole-body imaging and the
organ-specific imaging.

Author Contributions: Conceptualization, Q.P. and S.X.; methodology, X.Z.; formal analysis, Y.Z.; investigation,
G.Y.; data curation, Q.H.; writing—original draft preparation, S.X.; writing—review and editing, J.X.; funding
acquisition, Q.P. All authors have read and agreed to the published version of the manuscript.
Funding: This research was funded by National Natural Science Foundation of China (grant number 51627807),
the 111 Project (grant number B16019), Hubei International Cooperation Project (grant number 2018AHB001) and
the National Institutes of Health, National Institute of Biomedical Imaging and Bioengineering (grant number
R01EB006085). The APC was funded by Shenzhen Bay Laboratory.
Conflicts of Interest: The authors declare no conflict of interest.

References
1. Hoh, C.K. Clinical use of FDG PET. Nucl. Med. Boil. 2007, 34, 737–742. [CrossRef]
2. Kitson, S.L.; Cuccurullo, V.; Ciarmiello, A.; Salvo, D.; Mansi, L. Clinical applications of positron emission
tomography (PET) imaging in medicine: Oncology, brain diseases and cardiology. Curr. Radiopharm. 2009, 2,
224–253. [CrossRef]
3. Lamprou, E.; Gonzalez, A.J.; Sanchez, F.; Benlloch, J.M. Exploring TOF capabilities of PET detector blocks
based on large monolithic crystals and analog SiPMs. Phys. Med. 2020, 70, 10–18. [CrossRef] [PubMed]
4. Xie, S.; Zhang, X.; Peng, H.; Yang, J.; Huang, Q.; Xu, J.; Peng, Q. PET detectors with 127 ps CTR for the
Tachyon-II time-of-flight PET scanner. Nucl. Instrum. Methods Phys. Res. Sect. A Accel. Spectrom. Detect.
Assoc. Equip. 2019, 933, 48–55. [CrossRef]
5. Alekhin, M.S.; De Haas, J.T.M.; Khodyuk, I.V.; Krämer, K.W.; Menge, P.R.; Ouspenski, V.; Dorenbos, P.
Improvement of γ-ray energy resolution of LaBr3 : Ce3+ scintillation detectors by Sr2+ and Ca2+ co-doping.
Appl. Phys. Lett. 2013, 102, 161915. [CrossRef]
6. Gundacker, S.; Acerbi, F.; Auffray, E.; Ferri, A.; Gola, A.; Nemallapudi, M.V.; Paternoster, G.; Piemonte, C.;
Lecoq, P. State of the art timing in TOF-PET detectors with LuAG, GAGG and L(Y)SO scintillators of various
sizes coupled to FBK-SiPMs. J. Instrum. 2016, 11, P08008. [CrossRef]
7. Conti, M. State of the art and challenges of time-of-flight PET. Phys. Med. 2009, 25, 1–11. [CrossRef]
8. Moses, W.W. Recent advances and future advances in time-of-flight PET. Nucl. Instrum. Methods Phys. Res.
Sect. A Accel. Spectrom. Detect. Assoc. Equip. 2007, 580, 919–924. [CrossRef]
9. Surti, S.; Karp, J.S. Advances in time-of-flight PET. Phys. Med. 2016, 32, 12–22. [CrossRef]
10. Conti, M.; Bendriem, B. The new opportunities for high time resolution clinical TOF PET. Clin. Transl. Imaging
2019, 7, 139–147. [CrossRef]
11. Hsu, D.F.C.; Ilan, E.; Peterson, W.T.; Uribe, J.; Lubberink, M.; Levin, C.S. Studies of a next-generation
silicon-photomultiplier–based time-of-flight PET/CT system. J. Nucl. Med. 2017, 58, 1511–1518. [CrossRef]
[PubMed]
12. Vandenberghe, S. [I180] Recent developments in time-of-flight PET. Phys. Med. Eur. J. Med. Phys. 2018, 52,
69. [CrossRef]
13. Lyu, Y.; Lv, X.; Liu, W.; Judenhofer, M.S.; Zwingenberger, A.; Wisner, E.R.; Berg, E.; McKenney, S.E.;
Leung, E.K.; Spencer, B.A.; et al. Mini EXPLORER II: A prototype high-sensitivity PET/CT scanner for
companion animal whole body and human brain scanning. Phys. Med. Boil. 2019, 64, 075004. [CrossRef]
14. Zhang, X.; Zhou, J.; Cherry, S.R.; Badawi, R.D.; Qi, J. Quantitative image reconstruction for total-body PET
imaging using the 2-meter long EXPLORER scanner. Phys. Med. Boil. 2017, 62, 2465–2485. [CrossRef]
15. Badawi, R.D.; Shi, H.; Hu, P.; Chen, S.; Xu, T.; Price, P.M.; Ding, Y.; Spencer, B.A.; Nardo, L.; Liu, W.; et al.
First human imaging studies with the EXPLORER total-body PET scanner. J. Nucl. Med. 2019, 60, 299–303.
[CrossRef]
16. Cherry, S.R.; Jones, T.; Karp, J.S.; Qi, J.; Moses, W.W.; Badawi, R.D. Total-body PET: Maximizing sensitivity to
create new opportunities for clinical research and patient care. J. Nucl. Med. 2017, 59, 3–12. [CrossRef]
17. Lecoq, P. Pushing the limits in time-of-flight PET imaging. IEEE Trans. Radiat. Plasma Med. Sci. 2017, 1,
473–485. [CrossRef]
18. Guo, L.; Tian, J.; Chen, P.; Derenzo, S.E.; Choong, W.-S. Improving timing performance of double-ended
readout in TOF-PET detectors. J. Instrum. 2020, 15, P01003. [CrossRef]
Crystals 2020, 10, 869 15 of 15

19. Gundacker, S.; Knapitsch, A.; Auffray, E.; Jarron, P.; Meyer, T.; Lecoq, P. Time resolution deterioration with
increasing crystal length in a TOF-PET system. Nucl. Instrum. Methods Phys. Res. Sect. A Accel. Spectrom.
Detect. Assoc. Equip. 2014, 737, 92–100. [CrossRef]
20. Carrier, C.; LeComte, R. Effect of geometrical modifications and crystal defects on light collection in ideal
rectangular parallelepipedic BGO scintillators. Nucl. Instrum. Methods Phys. Res. Sect. A Accel. Spectrom.
Detect. Assoc. Equip. 1990, 294, 355–364. [CrossRef]
21. Huber, J.S.; Moses, W.W.; Andreaco, M.S.; Loope, M.; Melcher, C.L.; Nutt, R. Geometry and surface treatment
dependence of the light collection from LSO crystals. Nucl. Instrum. Methods Phys. Res. Sect. A Accel.
Spectrom. Detect. Assoc. Equip. 1999, 437, 374–380. [CrossRef]
22. Danevich, F.A.; Kobychev, V.V.; Kobychev, R.V.; Kraus, H.; Mikhailik, V.B.; Mokina, V.M.; Solsky, I.M. Impact
of geometry on light collection efficiency of scintillation detectors for cryogenic rare event searches. Nucl.
Instrum. Methods Phys. Res. Sect. B Beam Interact. Mater. At. 2014, 336, 26–30. [CrossRef]
23. Chen, J.; Mao, R.; Zhang, L.; Zhu, R.-Y. Large size LSO and LYSO crystals for future high energy physics
experiments. IEEE Trans. Nucl. Sci. 2007, 54, 718–724. [CrossRef]
24. Mao, R.; Zhang, L.; Zhu, R.-Y. Optical and scintillation properties of inorganic scintillators in high energy
physics. IEEE Trans. Nucl. Sci. 2008, 55, 2425–2431. [CrossRef]
25. Janecek, M.; Moses, W.W. Measuring light reflectance of BGO crystal surfaces. EEE Trans. Nucl. Sci. 2008, 55,
2443–2449. [CrossRef]
26. Wagatsuma, K.; Miwa, K.; Sakata, M.; Oda, K.; Ono, H.; Kameyama, M.; Toyohara, J.; Ishii, K. Comparison
between new-generation SiPM-based and conventional PMT-based TOF-PET/CT. Phys. Med. 2017, 42,
203–210. [CrossRef]
27. Sui, T.; Zhao, Z.; Xie, S.; Xie, Y.; Zhao, Y.; Huang, Q.; Xu, J.; Peng, Q. A 2.3-ps RMS Resolution Time-to-Digital
Converter Implemented in a Low-Cost Cyclone V FPGA. IEEE Trans. Instrum. Meas. 2019, 68, 3647–3660.
[CrossRef]
28. Song, Z.; Zhao, Z.; Yu, H.; Yang, J.; Zhang, X.; Sui, T.; Xu, J.; Xie, S.; Huang, Q.; Peng, Q. An 8.8 ps
RMS Resolution Time-To-Digital Converter Implemented in a 60 nm FPGA with Real-Time Temperature
Correction. Sensors 2020, 20, 2172. [CrossRef]
29. Salomoni, M.; Pots, R.; Auffray, E.; Lecoq, P. Enhancing light extraction of inorganic scintillators using
photonic crystals. Crystals 2018, 8, 78. [CrossRef]
30. Peng, Q.; Xie, S.; Sui, T.; Yang, M.; Huang, Q.; Xu, J. Experimental assessments of the timing performances of
detectors constructed with LaBr3, CeBr3, LFS, LSO, LYSO, GAGG scintillators. In Proceedings of the 2017
IEEE Nuclear Science Symposium and Medical Imaging Conference (NSS/MIC), Atlanta, GA, USA, 21–28
October 2017; pp. 1–2.

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