Fabrication and Luminescent Property of Polycrystalline Cerium-doped Lutetium Oxyorthsilicate Scintillation Ceramics

doi:10.15541/jim20170322

Abstract

Abstract:

Fabrication processing of cerium-doped lutetium oxyorthsilicate (Lu₂SiO₅:Ce³⁺, LSO:Ce) scintillation materials was systematically investigated in this article. Spherical LSO:Ce precursor powder was fabricated through spray drying from the synthetic LSO:Ce precursor sol. Single-phased LSO:Ce spherical powders with A-type and B-type crystal structure were achieved under the calcining temperature of 1000℃ and 1100℃ starting from the spherical LSO:Ce precursor powder, respectively. The LSO:Ce powders with the diameter of about 2 μm are solid spherical granules, which are assembled from a set of nano-sized grains. The LSO:Ce ceramics with the average grain size of 1.3 μm were sintered by spark plasma sintering (SPS) under sintering temperature of 1200℃ and the applied pressure of 80 MPa starting from fabricated A-type LSO:Ce spherical powder. Relative density of the sintered LSO:Ce ceramics can be attained to 99.7%. The pressureless sintered ceramics with relative density of 98.6% was obtained through pressureless sintering at 1650℃ for 4 h in air starting from the green compact dry-pressured from an A-type LSO:Ce spherical powder. The average grain size of the pressureless sintered ceramics is 1.6 μm. After HIPing at 1650℃ under an argon atmosphere for 1 h, a translucent LSO:Ce ceramics with clear grain boundary was achieved. The relative density of the HIPed ceramics is 99.9% and its average grain size is 1.7 μm. The light yield of the HIPed LSO:Ce ceramics reaches 28600 photons/MeV and its luminescence decay time is 25 ns.

Key words: lutetium oxyorthosilicate, fabrication, SPS, HIP, scintillation ceramics

CLC Number:

TQ174

FAN Ling-Cong, SHI Ying, XIE Jian-Jun. Fabrication and Luminescent Property of Polycrystalline Cerium-doped Lutetium Oxyorthsilicate Scintillation Ceramics[J]. Journal of Inorganic Materials, 2018, 33(2): 237-244.

Figures/Tables 11

Fig. 1 TG-DSC curves of the LSO:Ce precursor derived from spray drying

Fig. 2 XRD patterns of the precursors calcined at (a) 1000℃ and (b) 1100℃

Fig. 3 SEM images of the precursors (a, b) and precursors calcined at (c) 1000℃, (d) 1100℃, (e) 1200℃ and (f) 1300℃

Fig. 4 SEM images of fracture surfaces of LSO:Ce ceramics SPS-sintered at (a) 1150℃, (b) 1200℃, (c) 1250℃, (d) 1300℃ and (e) 1350℃ for 5 min from micrometer-sized spherical powders

Fig. 5 Dependence of the grain size and the porosity of SPS- sintered LSO:Ce ceramics on the sintering temperature

Fig. 6 Polished surface morphologies of LSO:Ce ceramics (a) before and (b) after HIPing

Fig. 7 PL and PLE spectra of the HIPed LSO:Ce ceramics

Fig. 8 CL spectra of the HIPed LSO:Ce ceramics Insets are the morphologies of the respective coarse-grained and fine- grained area

Fig. 9 In-line transmittance curve of the HIPed LSO:Ce ceramics Inset is photograph of the HIPed ceramics

Fig. 10 137Cs spectra of the HIPed LSO:Ce ceramics and BGO single crystal

Fig. 11 Luminescence decay curve of the HIPed LSO:Ce ceramics (λex=360 nm, λem=406 nm)

References 27

[1]	ZHU R Y Quality of Long LSO/LYSO Crystals.Journal of Physics: Conference Series, 2012, 404(1): 012026.
[2]	MELCHER C L, SCHWEITZER J S.Cerium-doped lutetium oxyorthosilicate: a fast, efficient new scintillator.IEEE Transactions on Nuclear Science, 1992, 39(4): 502-505.
[3]	MELCHER C L, SCHMAND M, ERIKSSON M, et al.Scintillation properties of LSO:Ce boules.IEEE Transactions on Nuclear Science, 2000, 47(3): 965-968.
[4]	BLAHUTA S, BESSI RE A, VIANA B, et al.Evidence and consequences of Ce in LYSO Ce, Ca and LYSO Ce, Mg single crystals for medical imaging applications.IEEE Transactions on Nuclear Science, 2013, 60(4): 3134-3141.
[5]	MAO R, WU C, DAI L E, et al.Crystal growth and scintillation properties of LSO and LYSO crystals.Journal of Crystal Growth, 2013, 368: 97-100.
[6]	YAN C, ZHAO G, HANG Y, et al.Comparison of cerium-doped Lu2Si2O7 and Lu2SiO5 scintillators.Journal of Crystal Growth, 2005, 281(2/3/4): 411-415.
[7]	REN G, QIN L, LU S, et al.Scintillation characteristics of lutetium oxyorthosilicate (Lu2SiO5:Ce) crystals doped with cerium ions. Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment. 2004, 531(3): 560-565.
[8]	FARHI H, LEBBOU K, BELKAHLA S, et al.Fiber single crystal growth by LHPG technique and optical characterization of Ce3+-doped Lu2SiO5.Optical Materials. 2008, 30(9): 1461-1467.
[9]	REN G, QIN L, LI H, et al.Investigation on defects in Lu2SiO5 : Ce crystals grown by Czochralski method.Crystal Research and Technology, 2006, 41(2): 163-167.
[10]	QIN L, REN G, LI H, et al.Main problems in the growth of Lu2SiO5:Ce scintillation crystals.Journal of The Chinese Ceramic Society, 2004, 32(11): 1361-1366.
[11]	LOUTTS G B, ZAGUMENNYI A I, LAVRISHCHEV S V, et al.Czochralski growth and characterization of (Lu1-xGdx)2SiO5 single crystals for scintillators.Journal of Crystal Growth, 1997, 174: 331-336.
[12]	LEMPICKI A, BRECHER C, LINGERTAT H, et al.A ceramic version of the LSO scintillator.IEEE Transactions on Nuclear Science, 2008, 55(3): 1148-1151.
[13]	WANG Y, LOEF E V, RHODES W H, et al.Lu2SiO5:Ce optical ceramic scintillator for PET.IEEE Transactions on Nuclear Science, 2009, 56(3): 887-891.
[14]	XIE J, SHI Y, FAN L, et al.Microstructure and luminescent properties of Ce:Lu2SiO5 ceramic scintillator by spark plasma sintering.Optical Materials, 2013, 35(4): 744-747.
[15]	XIE J, LIN T, SHI Y, et al.Luminescence properties of nano-sized Lu2SiO5:Ce phosphors prepared by Sol-Gel method.Journal of the Chinese Ceramic Society, 2010, 38(10): 1931-1936.
[16]	FAN L, SHI Y, XU J, et al.Consolidation of translucent Ce3+- doped Lu2SiO5 scintillation ceramics by pressureless sintering.Journal of Materials Research, 2014, 29(19): 2252-2259.
[17]	LIN T, XU Z B, DENG L Y, et al.Spark plasma sintering of Ce3+:Lu2SiO5 scintillation ceramics and its luminescent characteristics.Journal of Inorganic Materials, 2011, 26(11): 1210-1214.
[18]	LLER-BUNZ H M, SCHLEID T. On the oxide silicates M2O[SiO4] of the heavy lanthanides (M = Dy-Lu) with the A-type structure.Zeitschrift für Anorganische und Allgemeine Chemie. 1999, 625(4): 613-618.
[19]	ZHU J, GU M, LIU X, et al.Phase transition and elastic and optical properties of Lu2SiO5.Optical Materials, 2013, 35(9): 1659-1663.
[20]	FAN L, SHI Y, WU Y, et al.Crystal structure dependence of luminescence properties of Ce-doped lutetium oxyorthosilicate powder.Journal of Luminescence, 2017, 190: 504-510.
[21]	GUSTAFSSON T, KLINTENBERG M, DERENZO S E, et al.Lu2SiO5 by single-crystal X-ray and neutron diffraction.Acta Crystallographica Section C: Crystal Structure Communications, 2001, 57(6): 668-669.
[22]	WANG Y, HE Q, CHU B.Synthesis and characterization of Ce-doped Lu2SiO5 powders by the solid-state reaction with Li2SO4 flux.Journal of Alloys and Compounds, 2009, 479(1/2): 704-706.
[23]	MANSUY C, MAHIOU R, NEDELEC J M.A new Sol-Gel route to Lu2SiO5 (LSO) scintillator: powders and thin films.Chemistry of Materials, 2003, 15(17): 3242-3244.
[24]	ZYCH E, BRECHER C, WOJTOWICZ A J, et al.Luminescence properties of Ce-activated YAG optical ceramic scintillator materials.Journal of Luminescence, 1997, 75(3): 193-203.
[25]	FAN L, JIANG M, LIN D, et al.Densification of cerium-doped lutetium oxyorthosilicate scintillation ceramics by hot isostatic pressing.Journal of Alloys and Compounds, 2017, 720: 161-168.
[26]	ROY S, LINGERTAT H, BRECHER C, et al.Optical properties of anisotropic polycrystalline Ce3+ activated LSO.Optical Materials, 2012, 35(5): 827-832.
[27]	CHEN J, MAO R, ZHANG L, et al.Large size LSO and LYSO crystals for future high energy physics experiments.IEEE Transactions on Nuclear Science, 2007, 54(3): 718-724.