Citation: LI Ru-Song, HE Bin, LI Gang, XU Peng, LU Xin-Cheng, WANG Fei. An Electronic Structure Calculation for 5f States of δ Phase Plutonium Based on the Density Functional Theory Method[J]. Acta Physico-Chimica Sinica, ;2015, 31(S1): 75-80. doi: 10.3866/PKU.WHXB2014Ac03 shu

An Electronic Structure Calculation for 5f States of δ Phase Plutonium Based on the Density Functional Theory Method

LI Ru-Song ^1,, ,
HE Bin ¹ ,
LI Gang ¹ ,
XU Peng ¹ ,
LU Xin-Cheng ² ,
WANG Fei ¹

1.
1 Xi'an Research Institute of High Technology, Xi'an 710025, P. R. China;
2.
2 Navy Research Institute of Nuclear and Chemistry Safety, Beijing 100077, P. R. China

Corresponding author: LI Ru-Song,
Fund Project: 国家自然科学基金(51401237, 51271198, 11474358) (51401237, 51271198, 11474358)第二炮兵工程大学基金(2014QNJJ018, YX2012cxpy06)资助项目 (2014QNJJ018, YX2012cxpy06)

First-principle calculations of 5fⁿ (n=0-7) electronic configurations are performed with several density functional theory (DFT) methods to describe the localized/delocalized states and obtain the precise population of the 5f manifold in delta-plutonium (δ-Pu). The results show that spin polarization clearly reduces the cohesive energies of each electronic configuration, and enhances the cohesion properties. For 5f⁰, 5f¹, 5f³, 5f⁴, and 5f⁶ electronic configurations, the cohesive energies obtained by the spin- polarized local density approximation (SP-LDA)+U method are markedly smaller than that by the SP-LDA method when the lattice constant of δ-Pu exceeds 0.475 nm. The cohesive energies calculated with the spin-polarized generalized gradient approximation (SP-GGA)+U method are smaller than that by SP-GGAmethod, except for 5f⁴ and 5f⁶ electronic configurations, and the former trend to coincide with SP-LDA results when the lattice constants are larger than 0.570 nm. For the SP-LDA(GGA)+Umethod, the cohesive energies of 5f0, 5f1, 5f3, 5f4, and 5f6 (5f0, 5f¹, 5f², 5f³, 5f⁵, and 5f⁷) electronic configurations are all equal, while the cohesive energies of 5f², 5f⁵ (5f⁴) electronic configurations are the same as that of the 5f⁷ (5f⁶) electronic configuration. The cohesive energies of 5fn electronic configurations calculated using the other methods are equal. 5f projected densities of states show that spin polarization results in the exchange split behavior of 5f orbitals. Several 5f states are removed from the Fermi level, which lowers the contribution of 5f states to chemical bonding, and enhances the lattice constant, indicating that strong spin polarization induces partial localization of 5f orbitals. The optimized lattice constants obtained by the SP-LDA method are in good agreement with the experimental values, but the SP-GGA+U method sharply overestimates the lattice constant (by up to about 20%).
- 5f state,
- Electronic structure,
- Localization,
- Spin polarization
1. [1]
  (1) Söderlind, P.; Landa, A.; Sadigh, B. Phys. Rev. B 2002, 66, 205109. doi: 10.1103/PhysRevB.66.205109
2. [2]
  (2) Boettger, J. C. Int. J. Quantum Chem. 2003, 95, 380.
3. [3]
  (3) Postnikov, A. V.; Antropov, V. P. Comp. Mat. Sci. 2000, 17, 438. doi: 10.1016/S0927-0256(00)00064-1
4. [4]
  (4) Hecker, S. S.; Harbur, D. R.; Zocco, T. G. Prog. Mater. Sci. 2004, 49, 429. doi: 10.1016/S0079-6425(03)00032-X
5. [5]
  (5) Wang, Y.; Sun, Y. J. Phys.: Condes. Matter 2000, 12, L311.
6. [6]
  (6) Wu, X.; Ray, A. K. Phys. Rev. B 2005, 72, 045115. doi: 10.1103/PhysRevB.72.045115
7. [7]
  (7) Gong, H. R.; Ray, A. K. Surf. Sci. 2006, 600, 2231. doi: 10.1016/j.susc.2006.03.021
8. [8]
  (8) Kutepov, A. L.; Kutepova, S. G. J. Phys. Condes.: Matt. 2003, 15, 2607. doi: 10.1088/0953-8984/15/17/315
9. [9]
  (9) Kollar, J.; Vitos, L.; Skriver, H. L. Phys. Rev. B 1997, 55, 15353. doi: 10.1103/PhysRevB.55.15353
10. [10]
  (10) Hay, P. J.; Martin, R. L. J. Chem. Phys.1998, 109, 3875. doi: 10.1063/1.476988
11. [11]
  (11) Söderlind, P.; Sadigh, B. Phys. Rev. Lett. 2004, 92, 185702. doi: 10.1103/PhysRevLett.92.185702
12. [12]
  (12) Savrasov, S. Y.; Kotliar, G. Phys. Rev. Lett. 2000, 84, 3670. doi: 10.1103/PhysRevLett.84.3670
13. [13]
  (13) Sadigh, B.; Wolfer, W. G. Phys. Rev. B 2005, 72, 205122. doi: 10.1103/PhysRevB.72.205122
14. [14]
  (14) Shorikov, A. O.; Lukoyanov, A. V.; Korotin, M. A.; Anisimov, V. I. Phys. Rev. B 2005, 72, 024458. doi: 10.1103/PhysRevB.72.024458
15. [15]
  (15) Zhu, Z. H.; Meng, D. Q. Acta Phys. Sin. 2011, 60, 040301. [朱正和, 蒙大桥. 物理学报, 2011, 60, 040301]
16. [16]
  (16) Shick, A. B.; Drchal, V.; Havela, L. Europhys. Lett. 2005, 69, 588. doi: 10.1209/epl/i2004-10380-5
17. [17]
  (17) Johansson, B.; Rosengren, A. Phys. Rev. B 1975, 11, 1367. doi: 10.1103/PhysRevB.11.1367
18. [18]
  (18) Savrasov, S. Y.; Kotliar, G.; Abrahams, E. Nature 2001, 410, 793. doi: 10.1038/35071035
19. [19]
  (19) Moore, K. T.; Wall, M. A.; Schwartz, A. J.; Chung, B.W.; Shuh, D. K.; Schulze, R. K.; Tobin, J. G. Phys. Rev. Lett. 2003, 90, 196404. doi: 10.1103/PhysRevLett.90.196404
20. [20]
  (20) van der Laan, G.; Moore, K. T.; Tobin, J. G.; Chung, B.W.; Wall, M. A.; Schwartz, A. J. Phys. Rev. Lett. 2004, 93, 097401. doi: 10.1103/PhysRevLett.93.097401
21. [21]
  (21) Tobin, J. G.; Moore, K. T.; Chung, B.W.; Wall, M. A.; Schwartz, A. J.; van der Laan, G.; Kutepov, A. L. Phys. Rev. B 2005, 72, 085109. doi: 10.1103/PhysRevB.72.085109
22. [22]
  (22) Moore, K. T.; van der Laan, G.; Haire, R. G.; Wall, M. A.; Schwartz, A. J. Phys. Rev. B 2006, 73, 033109. doi: 10.1103/PhysRevB.73.033109
23. [23]
  (23) Kotliar, G.; Vollhardt, D. Phys. Today 2004, 57, 53.
24. [24]
  (24) Dai, X.; Savrasov, S. Y.; Kotliar, G.; Migliori, A.; Ledbetter, H.; Abrahams, E. Science 2003, 300, 953. doi: 10.1126/science.1083428
25. [25]
  (25) Wong, J.; Krisch, M.; Farber, D. L.; Occelli, F.; Schwartz, A. J.; Chiang, T. C.; Wall, M.; Boro, C.; Xu, R. Science 2003, 301, 1078. doi: 10.1126/science.1087179
26. [26]
  (26) Pourovskii, L. V.; Katsnelson, M. I.; Lichtenstein, A. I.; Havela, L.; Gouder, T.; Wastin, F.; Shick, A. B.; Drchal, V.; Lander, G. H. Europhys. Lett. 2006, 74, 479. doi: 10.1209/epl/i2005-10548-5
1. [1]
  Zhenming Xu , Mingbo Zheng , Zhenhui Liu , Duo Chen , Qingsheng Liu . Experimental Design of Project-Driven Teaching in Computational Materials Science: First-Principles Calculations of the LiFePO₄ Cathode Material for Lithium-Ion Batteries. University Chemistry, 2024, 39(4): 140-148. doi: 10.3866/PKU.DXHX202307022
2. [2]
  Yonghui ZHOU , Rujun HUANG , Dongchao YAO , Aiwei ZHANG , Yuhang SUN , Zhujun CHEN , Baisong ZHU , Youxuan ZHENG . Synthesis and photoelectric properties of fluorescence materials with electron donor-acceptor structures based on quinoxaline and pyridinopyrazine, carbazole, and diphenylamine derivatives. Chinese Journal of Inorganic Chemistry, 2024, 40(4): 701-712. doi: 10.11862/CJIC.20230373
3. [3]
  Aimin Fu , Chunmei Chen , Qin Li , Nanjin Ding , Jiaxin Dong , Yu Chen , Mengsha Wei , Weiguang Sun , Hucheng Zhu , Yonghui Zhang . Niduenes A−F, six functionalized sesterterpenoids with a pentacyclic 5/5/5/5/6 skeleton from endophytic fungus Aspergillus nidulans. Chinese Chemical Letters, 2024, 35(9): 109100-. doi: 10.1016/j.cclet.2023.109100
4. [4]
  Zhen Liu , Zhi-Yuan Ren , Chen Yang , Xiangyi Shao , Li Chen , Xin Li . Asymmetric alkenylation reaction of benzoxazinones with diarylethylenes catalyzed by B(C₆F₅)₃/chiral phosphoric acid. Chinese Chemical Letters, 2024, 35(5): 108939-. doi: 10.1016/j.cclet.2023.108939
5. [5]
  Runze Xu , Rui Liu . U-Pb Dating in the Age of Dinosaurs. University Chemistry, 2024, 39(9): 243-247. doi: 10.12461/PKU.DXHX202404083
6. [6]
  Xinting XIONG , Zhiqiang XIONG , Panlei XIAO , Xuliang NIE , Xiuying SONG , Xiuguang YI . Synthesis, crystal structures, Hirshfeld surface analysis, and antifungal activity of two complexes Na(Ⅰ)/Cd(Ⅱ) assembled by 5-bromo-2-hydroxybenzoic acid ligands. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1661-1670. doi: 10.11862/CJIC.20240145
7. [7]
  Tengjiao Wang , Tian Cheng , Rongjun Liu , Zeyi Wang , Yuxuan Qiao , An Wang , Peng Li . Conductive Hydrogel-based Flexible Electronic System: Innovative Experimental Design in Flexible Electronics. University Chemistry, 2024, 39(4): 286-295. doi: 10.3866/PKU.DXHX202309094
8. [8]
  Xin Zhou , Zhi Zhang , Yun Yang , Shuijin Yang . A Study on the Enhancement of Photocatalytic Performance in C/Bi/Bi₂MoO₆ Composites by Ferroelectric Polarization: A Recommended Comprehensive Chemical Experiment. University Chemistry, 2024, 39(4): 296-304. doi: 10.3866/PKU.DXHX202310008
9. [9]
  Yuping Wei , Yiting Wang , Jialiang Jiang , Jinxuan Deng , Hong Zhang , Xiaofei Ma , Junjie Li . Interdisciplinary Teaching Practice——Flexible Wearable Electronic Skin for Low-Temperature Environments. University Chemistry, 2024, 39(10): 261-270. doi: 10.12461/PKU.DXHX202404007
10. [10]
  Yan Liu , Yuexiang Zhu , Luhua Lai . Introduction to Blended and Small-Class Teaching in Structural Chemistry: Exploring the Structure and Properties of Crystals. University Chemistry, 2024, 39(3): 1-4. doi: 10.3866/PKU.DXHX202306084
11. [11]
  Jinfu Ma , Hui Lu , Jiandong Wu , Zhongli Zou . Teaching Design of Electrochemical Principles Course Based on “Cognitive Laws”: Kinetics of Electron Transfer Steps. University Chemistry, 2024, 39(3): 174-177. doi: 10.3866/PKU.DXHX202309052
12. [12]
  Zitong Chen , Zipei Su , Jiangfeng Qian . Aromatic Alkali Metal Reagents: Structures, Properties and Applications. University Chemistry, 2024, 39(8): 149-162. doi: 10.3866/PKU.DXHX202311054
13. [13]
  Donghui PAN , Yuping XU , Xinyu WANG , Lizhen WANG , Junjie YAN , Dongjian SHI , Min YANG , Mingqing CHEN . Preparation and in vivo tracing of ⁶⁸Ga-labeled PM_2.5 mimetic particles for positron emission tomography imaging. Chinese Journal of Inorganic Chemistry, 2024, 40(4): 669-676. doi: 10.11862/CJIC.20230468
14. [14]
  Jizhou Liu , Chenbin Ai , Chenrui Hu , Bei Cheng , Jianjun Zhang . 六氯锡酸铵促进钙钛矿太阳能电池界面电子转移及其飞秒瞬态吸收光谱研究. Acta Physico-Chimica Sinica, 2024, 40(11): 2402006-. doi: 10.3866/PKU.WHXB202402006
15. [15]
  Qin Hu , Liuyun Chen , Xinling Xie , Zuzeng Qin , Hongbing Ji , Tongming Su . Ni掺杂构建电子桥及激活MoS₂惰性基面增强光催化分解水产氢. Acta Physico-Chimica Sinica, 2024, 40(11): 2406024-. doi: 10.3866/PKU.WHXB202406024
16. [16]
  Xiangchun Li , Wei Xue , Xu Liu , Wenyong Lai . Research and Practice on the Cultivation of Innovation Ability of Chemistry Graduate Students in Electronic Information Universities: A Case Study of Nanjing University of Posts and Telecommunications. University Chemistry, 2024, 39(6): 55-62. doi: 10.3866/PKU.DXHX202310018
17. [17]
  Yi Zhang , Biao Wang , Chao Hu , Muhammad Humayun , Yaping Huang , Yulin Cao , Mosaad Negem , Yigang Ding , Chundong Wang . Fe–Ni–F electrocatalyst for enhancing reaction kinetics of water oxidation. Chinese Journal of Structural Chemistry, 2024, 43(2): 100243-100243. doi: 10.1016/j.cjsc.2024.100243
18. [18]
  Xinyu Yin , Haiyang Shi , Yu Wang , Xuefei Wang , Ping Wang , Huogen Yu . Spontaneously Improved Adsorption of H₂O and Its Intermediates on Electron-Deficient Mn^(3+δ)+ for Efficient Photocatalytic H₂O₂ Production. Acta Physico-Chimica Sinica, 2024, 40(10): 2312007-. doi: 10.3866/PKU.WHXB202312007
19. [19]
  Kun WANG , Wenrui LIU , Peng JIANG , Yuhang SONG , Lihua CHEN , Zhao DENG . Hierarchical hollow structured BiOBr-Pt catalysts for photocatalytic CO₂ reduction. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1270-1278. doi: 10.11862/CJIC.20240037
20. [20]
  Haitang WANG , Yanni LING , Xiaqing MA , Yuxin CHEN , Rui ZHANG , Keyi WANG , Ying ZHANG , Wenmin WANG . Construction, crystal structures, and biological activities of two Ln^Ⅲ₃ complexes. Chinese Journal of Inorganic Chemistry, 2024, 40(8): 1474-1482. doi: 10.11862/CJIC.20240188

Get Citation

PDF

XML

Metrics

PDF Downloads(249)
Abstract views(915)
HTML views(32)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142