| CONDENSED MATTER: STRUCTURAL, MECHANICAL, AND THERMAL PROPERTIES |
Prev
Next
|
|
|
Site occupation of Al doping in Lu2SiO5: The role of ionic radius versus chemical valence |
| Xuejiao Sun(孙雪娇)1,2, Yu Cui(崔宇)1,2, Feng Gao(高峰)1,†, Zhongjun Xue(薛中军)2, Shuwen Zhao(赵书文)2, Dongzhou Ding(丁栋舟)2, Fan Yang(杨帆)3, and Yi-Yang Sun(孙宜阳)2,‡ |
1 School of Physics, Changchun Normal University, Changchun 130032, China;
2 State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 201899, China;
3 Key Laboratory of Weak-Light Nonlinear Photonics, Ministry of Education, School of Physics, Nankai University, Tianjin 300071, China |
|
|
|
|
Abstract Lu$_{2}$SiO$_{5}$:Ce (LSO:Ce) serving as a core material for radiation detectors, plays a crucial role in the design and development of positron emission tomography (PET) devices. Experiment has confirmed that low concentration of Al doping can significantly enhance the light yield, decay time, rise time, energy resolution, and afterglow level of the LSO:Ce crystals. The mechanisms regarding the lattice site occupancy of Al in LSO, while closely associated with the performance improvements, are not yet fully understood. Particularly, it is unclear either the ionic radius or the chemical valence plays a more critical role in determining the site occupancy. In this study, we utilized first-principles calculations based on density functional theory (DFT) to study the lattice site occupancy of Al in LSO crystals and to explore their impact on the electronic structure. Our results indicate that with changes in the growth environment, as reflected by the atomic chemical potentials, Al can occupy either the Si sites or the Lu$_2$ sites, and it is not inclined to occupy the Lu$_1$ sites. The doping of Al at the Si site introduces a shallow acceptor level, which may contribute to the suppression of trap concentration and affect the ratio of Ce$^{3+}$ to Ce$^{4+}$ within the crystal, thereby influencing its scintillation properties.
|
Received: 12 January 2025
Revised: 08 April 2025
Accepted manuscript online: 09 May 2025
|
|
PACS:
|
61.72.-y
|
(Defects and impurities in crystals; microstructure)
|
| |
31.15.es
|
(Applications of density-functional theory (e.g., to electronic structure and stability; defect formation; dielectric properties, susceptibilities; viscoelastic coefficients; Rydberg transition frequencies))
|
| |
29.40.Mc
|
(Scintillation detectors)
|
|
| Fund: Project supported by the National Key Research and Development Program of China (Grant No. 2022YFB3503900) and the National Natural Science Foundation of China (Grant No. 12305212). |
Corresponding Authors:
Feng Gao, Yi-Yang Sun
E-mail: 5234110@qq.com;yysun@mail.sic.ac.cn
|
Cite this article:
Xuejiao Sun(孙雪娇), Yu Cui(崔宇), Feng Gao(高峰), Zhongjun Xue(薛中军), Shuwen Zhao(赵书文), Dongzhou Ding(丁栋舟), Fan Yang(杨帆), and Yi-Yang Sun(孙宜阳) Site occupation of Al doping in Lu2SiO5: The role of ionic radius versus chemical valence 2025 Chin. Phys. B 34 096101
|
[1] Melcher C and Schweitzer J 1992 IEEE Trans. Nucl. Sci. 39 502
[2] Doshi N K, Shao Y, Silverman R W and Cherry S R 2000 Med. Phys. 27 1535
[3] Lecoq P 2016 Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment 809 130
[4] Weber M J 2002 Journal of Luminescence 100 35
[5] Di Francesco A, Bugalho R, Oliveira L, Pacher L, Rivetti A, Rolo M, Silva J, Silva R and Varela J 2016 Journal of Instrumentation 11 C03042
[6] Surti S and Karp J S 2016 Physica Medica 32 12
[7] Melcher C, Koschan M, Zhuravleva M, Wu Y, Rothfuss H, Meng F, Tyagi M, Donnald S, Yang K, Hayward J et al. 2016 Scintillator design via codoping Proceedings of International Symposium on Radiation Detectors and Their Uses p. 020001
[8] Cooke D, Mcclellan K J, Bennett B L, Roper J, Whittaker M T, Muenchausen R E and Sze R 2000 J. Appl. Phys. 88 7360
[9] Kimble T, ChouMand Chai B H 2002 Scintillation properties of LYSO crystals IEEE Nuclear Science Symposium Conference Record, Vol. 3 (IEEE) pp. 1434-1437
[10] Spurrier M A, Szupryczynski P, Yang K, Carey A A and Melcher C L 2008 IEEE Trans. Nucl. Sci. 55 1178
[11] Blahuta S, Bessiere A, Viana B, Dorenbos P and Ouspenski V 2013 IEEE Trans. Nucl. Sci. 60 3134
[12] Yang K, Melcher C L, Rack P D and Eriksson L A 2009 IEEE Trans. Nucl. Sci. 56 2960
[13] Wu Y, Koschan M, Li Q, Greeley I and Melcher C L 2018 Journal of Crystal Growth 498 362
[14] Cai J and Yeung Y y 2023 Phys. Rev. B 107 085149
[15] Xue Z, Chen L, Zhao S, Yang F, An R, Wang L, Sun Y Y, Feng H and Ding D 2023 Crystal Growth & Design 23 4562
[16] Syntfeld-Kazuch A, Moszynski M, Swiderski L, Szczesniak T, Nassalski A, Melcher C L and Spurrier M A 2008 Energy resolution of calcium co-doped LSO:Ce scintillators IEEE Nuclear Science Symposium Conference Record (IEEE) pp. 2744-2750
[17] Shannon R D 1976 Foundations of Crystallography 32 751
[18] Kresse G and Furthmüller J 1996 Comput. Mater. Sci. 6 15
[19] Blöchl P E 1994 Phys. Rev. B 50 17953
[20] Kresse G and Joubert D 1999 Phys. Rev. B 59 1758
[21] Perdew J P, Ruzsinszky A, Csonka G I, Vydrov O A, Scuseria G E, Constantin L A, Zhou X and Burke K 2008 Phys. Rev. Lett. 100 136406
[22] Paier J, Marsman M, Hummer K, Kresse G, Gerber I C and Ańgyań J G 2006 J. Chem. Phys. 124 154709
[23] Freysoldt C, Grabowski B, Hickel T, Neugebauer J, Kresse G, Janotti A and Van de Walle C G 2014 Rev. Mod. Phys. 86 253
[24] Zhang S and Northrup J E 1991 Phys. Rev. Lett. 67 2339
[25] Freysoldt C, Grabowski B, Hickel T, Neugebauer J, Kresse G, Janotti A and Van de Walle C G 2014 Rev. Mod. Phys. 86 253
[26] Lu L, Zhang H, Wu X, Shi J and Sun Y Y 2021 Chin. Phys. B 30 096806
[27] Wu X, Ming C, Shi J, Wang H, West D, Zhang S and Sun Y Y 2022 Chin. Phys. Lett. 39 046101
[28] Kobayashi M, Ishii M and Melcher C L 1993 Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment 335 509
[29] Kamenskikh I, Mikhailin V, Munro I, Petrovykh D, Shaw D, Studenikin P, Vasil’ev A, Zagumennyi I and Zavartsev Y D 1995 Radiation Effects and Defects in Solids 135 391
[30] Lempicki A and Glodo J 1998 Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment 416 333
[31] Blahuta S, Bessière A, Viana B, Ouspenski V, Mattmann E, Lejay J and Gourier D 2011 Materials 4 1224
[32] Ding D, Feng H, Ren G, Nikl M, Qin L, Pan S and Yang F 2010 IEEE Trans. Nucl. Sci. 57 1272
[33] Melcher C L, Friedrich S, Cramer S P, Spurrier M A, Szupryczynski P and Nutt R 2005 IEEE Trans. Nucl. Sci. 52 1809 |
| No Suggested Reading articles found! |
|
|
Viewed |
|
|
|
Full text
|
|
|
|
|
Abstract
|
|
|
|
|
Cited |
|
|
|
|
Altmetric
|
|
blogs
Facebook pages
Wikipedia page
Google+ users
|
Online attention
Altmetric calculates a score based on the online attention an article receives. Each coloured thread in the circle represents a different type of online attention. The number in the centre is the Altmetric score. Social media and mainstream news media are the main sources that calculate the score. Reference managers such as Mendeley are also tracked but do not contribute to the score. Older articles often score higher because they have had more time to get noticed. To account for this, Altmetric has included the context data for other articles of a similar age.
View more on Altmetrics
|
|
|
