Scintillation properties and electronic structure of the intrinsic and extrinsic mixed elpasolites Cs2 Na RBr3I3 (R = La, Y)

Wei, Hua; Du, Mao -Hua; Stand, Luis; Zhao, Zhao; Zhuravleva, Mariya; Melcher, Charles L.; Shi, Hongliang

doi:10.1103/PhysRevApplied.5.024008

Title: Scintillation properties and electronic structure of the intrinsic and extrinsic mixed elpasolites Cs₂ Na RBr₃I₃ (R = La, Y)

Journal Article · Fri Feb 19 00:00:00 EST 2016 · Physical Review Applied

DOI:https://doi.org/10.1103/PhysRevApplied.5.024008· OSTI ID:1244201

Wei, Hua ^[1]; Du, Mao -Hua ^[2]; Stand, Luis ^[1]; Zhao, Zhao ^[3]; Zhuravleva, Mariya ^[1]; Melcher, Charles L. ^[1]; Shi, Hongliang ^[2]

Univ. of Tennessee, Knoxville, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Stanford Univ., Stanford, CA (United States)

Scintillators attract wide research interest for their distinct applications in radiation detection. Elpasolite halides are among the most promising scintillators due to their high structural symmetry and good scintillation performance. A better understanding of their underlying scintillation mechanism opens up possibilities in scintillator development. In this work, we employ a variety of experimental techniques to study the two mixed-anion elpasolites Cs₂NaRBr₃I₃ (R = La, Y). The emission of intrinsic Cs₂NaRBr₃I₃ with a light yield ranging from 20 000 to 40 000 ph / MeV is dominant by self-trapped exciton emission. Partial substitution of R with Ce introduces a competing emission, the Ce³⁺ 5d-to-4f radiative transition. Ab initio calculations are performed to investigate the electronic structures as well as the binding energies of polarons in Cs₂NaRBr₆. The calculated large self-trapped exciton binding energies are consistent with the observed high light yield due to self-trapped exciton (STE) emission. The unique electronic structure of halide elpasolites as calculated enhances the STE stability and the STE emission. The highly tunable scintillation properties of mixed-anion elpasolites underscore the role of their complex scintillation mechanism. Furthermore, our study provides guidance for the design of elpasolite scintillators with exceptional energy resolution and light yield desirable for applications.

View Accepted Manuscript (DOE)

View Accepted Manuscript (Publisher)

Cite

Export

Save

Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1244201

Alternate ID(s):: OSTI ID: 1238410

Journal Information:: Physical Review Applied, Vol. 5, Issue 2; ISSN 2331-7019

Publisher:: American Physical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 18 works

Citation information provided by
Web of Science

References (52)

The Role of PET Scan in Diagnosis, Staging, and Management of Non‐Small Cell Lung Cancer Schrevens, Liesbet; Lorent, Natalie; Dooms, Christophe The Oncologist, Vol. 9, Issue 6 https://doi.org/10.1634/theoncologist.9-6-633	journal	November 2004
Role of ${Ce}^{4 +}$ in the Scintillation Mechanism of Codoped ${Gd}_{3} {Ga}_{3} {Al}_{2} O_{12} ∶ Ce$ Wu, Yuntao; Meng, Fang; Li, Qi Physical Review Applied, Vol. 2, Issue 4 https://doi.org/10.1103/PhysRevApplied.2.044009	journal	October 2014
Cerium-doped lutetium oxyorthosilicate: a fast, efficient new scintillator Melcher, C. L.; Schweitzer, J. S. IEEE Transactions on Nuclear Science, Vol. 39, Issue 4 https://doi.org/10.1109/23.159655	journal	January 1992
Scintillator developments for high energy physics and medical imaging Lecoq, P.; Korzhik, M. IEEE Transactions on Nuclear Science, Vol. 47, Issue 4 https://doi.org/10.1109/23.872969	journal	January 2000
Applications of single crystals in oil well logging Melcher, C. L.; Schweitzer, J. S.; Manente, R. A. Journal of Crystal Growth, Vol. 109, Issue 1-4 https://doi.org/10.1016/0022-0248(91)90155-X	journal	February 1991
Scintillation: mechanisms and new crystals Weber, M. J. Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 527, Issue 1-2 https://doi.org/10.1016/j.nima.2004.03.009	journal	July 2004
The quest for the ideal inorganic scintillator Derenzo, S. E.; Weber, M. J.; Bourret-Courchesne, E. Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 505, Issue 1-2, p. 111-117 https://doi.org/10.1016/S0168-9002(03)01031-3	journal	June 2003
Light output and energy resolution of Ce3+-doped scintillators Dorenbos, Pieter Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 486, Issue 1-2 https://doi.org/10.1016/S0168-9002(02)00704-0	journal	June 2002
LaBr ₃ :Ce and SiPMs for time-of-flight PET: achieving 100 ps coincidence resolving time Schaart, Dennis R.; Seifert, Stefan; Vinke, Ruud Physics in Medicine and Biology, Vol. 55, Issue 7 https://doi.org/10.1088/0031-9155/55/7/N02	journal	March 2010
Crystal growth and scintillation properties of potassium strontium bromide Stand, L.; Zhuravleva, M.; Wei, H. Optical Materials, Vol. 46 https://doi.org/10.1016/j.optmat.2015.04.002	journal	August 2015
Characterization of the CLYC detector for neutron and photon detection Bourne, M. M.; Mussi, C.; Miller, E. C. Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 736 https://doi.org/10.1016/j.nima.2013.10.030	journal	February 2014
Optical and scintillation properties of pure and Ce3+-doped Cs2LiYCl6 and Li3YCl6:Ce3+ crystals Combes, C. M.; Dorenbos, P.; van Eijk, C. W. E. Journal of Luminescence, Vol. 82, Issue 4 https://doi.org/10.1016/S0022-2313(99)00047-2	journal	October 1999
f–d Luminescence of Pr3+ and Ce3+ in the chloro-elpasolite Cs2NaYCl6 Laroche, Mathieu; Bettinelli, Marco; Girard, Sylvain Chemical Physics Letters, Vol. 311, Issue 3-4 https://doi.org/10.1016/S0009-2614(99)00853-2	journal	September 1999
Luminescence properties of Ce-doped Cs2LiLaCl6 crystals Rodnyi, P. A.; Mikhailik, V. B.; Stryganyuk, G. B. Journal of Luminescence, Vol. 86, Issue 2 https://doi.org/10.1016/S0022-2313(99)00181-7	journal	March 2000
Crystal structure of dipotassium sodium fluoroaluminate (elpasolite) Moras, Lester R. Journal of Inorganic and Nuclear Chemistry, Vol. 36, Issue 12 https://doi.org/10.1016/0022-1902(74)80190-9	journal	December 1974
Phase transitions in elpasolites (ordered perovskites) Flerov, I. N.; Gorev, M. V.; Aleksandrov, K. S. Materials Science and Engineering: R: Reports, Vol. 24, Issue 3 https://doi.org/10.1016/S0927-796X(98)00015-1	journal	November 1998
New quadruple perovskites Ln ₂ Ba ₂ Ti _x Sn _2–x Cu ₂ O ₁₁ , (0⩽x⩽2): controlling copper–oxygen distances in potential superconducting parent phases Gormezano, Anne; Weller, Mark T. J. Mater. Chem., Vol. 3, Issue 9 https://doi.org/10.1039/jm9930300979	journal	January 1993
Neutron Scattering Studies on Phase Transition and Phonon Dispersion in Cs2NaBiCl6 Prokert, F.; Aleksandrov, K. S. physica status solidi (b), Vol. 124, Issue 2 https://doi.org/10.1002/pssb.2221240208	journal	August 1984
Selected Properties of Cs$_{2}$LiYCl$_{6}$, Cs$_{2}$LiLaCl$_{6}$, and Cs$_{2}$LiLaBr$_{6}$ Scintillators Glodo, Jarek; van Loef, Edgar; Hawrami, Rastgo IEEE Transactions on Nuclear Science, Vol. 58, Issue 1, p. 333-338 https://doi.org/10.1109/TNS.2010.2098045	journal	February 2011
Scintillation and spectroscopy of the pure and Ce ³ -doped elpasolites: Cs ₂ LiYX ₆ (X Cl, Br) Loef, E. V. D. van; Dorenbos, P.; Eijk, C. W. E. van Journal of Physics: Condensed Matter, Vol. 14, Issue 36 https://doi.org/10.1088/0953-8984/14/36/307	journal	August 2002
Scintillation and anomalous emission in elpasolite Cs₂LiLuCl₆:Ce³⁺ Bessière, A; Dorenbos, P; van Eijk, C. W. E. Journal of Luminescence, Vol. 117, Issue 2, p. 187-198 https://doi.org/10.1016/j.jlumin.2005.05.005	journal	April 2006
Scintillation characteristics of Cs2LiCeBr6 crystal Cheon, Jong Kyu; Kim, Sunghwan; Rooh, Gul Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 652, Issue 1 https://doi.org/10.1016/j.nima.2011.02.038	journal	October 2011
Scintillation Properties of a Cs2NaCeBr6 Crystal under X-ray, $gamma$-ray and Proton Irradiations Kim, Sunghwan; Moon, Jinho; Kim, H. J. Journal of the Korean Physical Society, Vol. 54, Issue 5(2) https://doi.org/10.3938/jkps.54.2098	journal	May 2009
Luminescence and Scintillation Characterization of Cs2NaGdBr6: Ce3+ Single Crystal Rooh, Gul; Kim, H. J.; Park, H. Journal of Luminescence, Vol. 132, Issue 3 https://doi.org/10.1016/j.jlumin.2011.10.015	journal	March 2012
Scintillation properties of Cs2LiLaBr6 (CLLB) crystals with varying Ce3+ concentration Shirwadkar, Urmila; Glodo, Jarek; van Loef, Edgar V. Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 652, Issue 1 https://doi.org/10.1016/j.nima.2010.08.050	journal	October 2011
Discrete Electronic Bands in Semiconductors and Insulators: Potential High-Light-Yield Scintillators Shi, Hongliang; Du, Mao-Hua Physical Review Applied, Vol. 3, Issue 5 https://doi.org/10.1103/PhysRevApplied.3.054005	journal	May 2015
Embedded-ion method: An analytical energy-conserving charge-transfer interatomic potential and its application to the La-Br system Zhou, X. W.; Doty, F. P. Physical Review B, Vol. 78, Issue 22 https://doi.org/10.1103/PhysRevB.78.224307	journal	December 2008
Two new cerium-doped mixed-anion elpasolite scintillators: Cs2NaYBr3I3 and Cs2NaLaBr3I3 Wei, Hua; Stand, Luis; Zhuravleva, Mariya Optical Materials, Vol. 38 https://doi.org/10.1016/j.optmat.2014.09.038	journal	December 2014
Scintillation Properties of Cs$_{3}$LaCl$_{6}$:Ce$^{3+}$ and Cs$_{3}$LaBr$_{6}$:Ce$^{3+}$ Wei, Hua; Zhuravleva, Mariya; Tyagi, Mohit IEEE Transactions on Nuclear Science, Vol. 61, Issue 1 https://doi.org/10.1109/TNS.2013.2282818	journal	February 2014
The scintillation properties of CeBr 3−x Cl x single crystals Wei, Hua; Martin, Victoria; Lindsey, Adam Journal of Luminescence, Vol. 156 https://doi.org/10.1016/j.jlumin.2014.08.015	journal	December 2014
Temperature dependence spectroscopic study of Ce-doped Cs3LaCl6 and Cs3LaBr6 scintillators Wei, Hua; Zhuravleva, Mariya; Meng, Fang Journal of Luminescence, Vol. 160 https://doi.org/10.1016/j.jlumin.2014.11.050	journal	April 2015
VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data Momma, Koichi; Izumi, Fujio Journal of Applied Crystallography, Vol. 44, Issue 6 https://doi.org/10.1107/S0021889811038970	journal	October 2011
Sample-to-Sample Variation in Single Crystal YAP:Ce Non-Proportionality Donnald, Samuel B.; Tyagi, Mohit; Rothfuss, Harold E. IEEE Transactions on Nuclear Science, Vol. 61, Issue 1 https://doi.org/10.1109/TNS.2013.2277860	journal	February 2014
Stepless Variable Resistor for High Currents Yokley, C. R.; Shumaker, J. B. Review of Scientific Instruments, Vol. 32, Issue 1 https://doi.org/10.1063/1.1717150	journal	January 1961
Effect of Ba substitution in CsSrI3:Eu2+ Wei, H.; Zhuravleva, M.; Yang, K. Journal of Crystal Growth, Vol. 384 https://doi.org/10.1016/j.jcrysgro.2013.09.007	journal	December 2013
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
First-principles calculations to describe zirconia pseudopolymorphs Jomard, G.; Petit, T.; Pasturel, A. Physical Review B, Vol. 59, Issue 6 https://doi.org/10.1103/PhysRevB.59.4044	journal	February 1999
Screened hybrid density functionals applied to solids Paier, J.; Marsman, M.; Hummer, K. The Journal of Chemical Physics, Vol. 124, Issue 15 https://doi.org/10.1063/1.2187006	journal	April 2006
First principles study of native defects in InI Biswas, Koushik; Du, Mao-Hua Journal of Applied Physics, Vol. 109, Issue 11 https://doi.org/10.1063/1.3592231	journal	June 2011
First-principles study of native defects in TlBr: Carrier trapping, compensation, and polarization phemomenon Du, Mao-Hua Journal of Applied Physics, Vol. 108, Issue 5 https://doi.org/10.1063/1.3476564	journal	September 2010
Impurity-bound small polarons in ZnO: Hybrid density functional calculations Du, Mao-Hua; Zhang, S. B. Physical Review B, Vol. 80, Issue 11 https://doi.org/10.1103/PhysRevB.80.115217	journal	September 2009
Linear optical properties in the projector-augmented wave methodology Gajdoš, M.; Hummer, K.; Kresse, G. Physical Review B, Vol. 73, Issue 4 https://doi.org/10.1103/PhysRevB.73.045112	journal	January 2006
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
Scintillation properties and anomalous Ce ³⁺ emission of Cs ₂ NaREBr ₆ :Ce ³⁺ (RE = La,Y,Lu) Birowosuto, M. D.; Dorenbos, P.; Eijk, C. W. E. van Journal of Physics: Condensed Matter, Vol. 18, Issue 26 https://doi.org/10.1088/0953-8984/18/26/031	journal	June 2006
Level location and spectroscopy of , , , and in Dorenbos, P.; van Loef, E. V. D.; Vink, A. P. Journal of Luminescence, Vol. 117, Issue 2 https://doi.org/10.1016/j.jlumin.2005.04.016	journal	April 2006
Low-Temperature Luminescence of Lu ₂ O ₃ :Eu Ceramics upon Excitation with Synchrotron Radiation in the Vicinity of Band Gap Energy Zych, Eugeniusz; Trojan-Piegza, Joanna Chemistry of Materials, Vol. 18, Issue 8 https://doi.org/10.1021/cm052774q	journal	April 2006
Small polarons in real crystals: concepts and problems Shluger, A. L.; Stoneham, A. M. Journal of Physics: Condensed Matter, Vol. 5, Issue 19 https://doi.org/10.1088/0953-8984/5/19/007	journal	May 1993
Trapping, self-trapping and the polaron family Stoneham, A. M.; Gavartin, J.; Shluger, A. L. Journal of Physics: Condensed Matter, Vol. 19, Issue 25 https://doi.org/10.1088/0953-8984/19/25/255208	journal	May 2007
Properties of the YAP : Ce scintillator Moszyński, M.; Kapusta, M.; Wolski, D. Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 404, Issue 1 https://doi.org/10.1016/S0168-9002(97)01115-7	journal	February 1998
Energy transport and scintillation of cerium-doped elpasolite Cs $_{2}$ LiYCl $_{6}$ : Hybrid density functional calculations Biswas, Koushik; Du, Mao-Hua Physical Review B, Vol. 86, Issue 1 https://doi.org/10.1103/PhysRevB.86.014102	journal	July 2012
Electronic structure engineering of elpasolites: Case of Cs2AgYCl6 Du, Mao-Hua; Biswas, Koushik Journal of Luminescence, Vol. 143 https://doi.org/10.1016/j.jlumin.2013.05.033	journal	November 2013