First-principles calculation of the electronic structure, chemical bonding, and thermodynamic properties of β-US2

doi:10.1088/1674-1056/24/12/127101

中国物理B ›› 2015, Vol. 24 ›› Issue (12): 127101-127101.doi: 10.1088/1674-1056/24/12/127101

• CONDENSED MATTER: ELECTRONIC STRUCTURE, ELECTRICAL, MAGNETIC, AND OPTICAL PROPERTIES • 上一篇下一篇

First-principles calculation of the electronic structure, chemical bonding, and thermodynamic properties of β-US₂

李世长^a, 郑远蕾^a, 马生贵^a, 高涛^a, 敖冰云^b

a Institute of Atomic and Molecular Physics, Sichuan University, Chengdu 610065, China;
b Science and Technology on Surface Physics and Chemistry Laboratory, P. O. Box 9071-35, Jiangyou 621907, China

收稿日期:2015-07-07 修回日期:2015-08-05 出版日期:2015-12-05 发布日期:2015-12-05
通讯作者: Gao Tao, Ao Bing-Yun E-mail:gaotao@scu.edu.cn;aobingyun@caep.cn
基金资助:
Project supported by the National Natural Science Foundation of China (Grant Nos. 21371160 and 21401173).

First-principles calculation of the electronic structure, chemical bonding, and thermodynamic properties of β-US₂

Li Shi-Chang (李世长)^a, Zheng Yuan-Lei (郑远蕾)^a, Ma Sheng-Gui (马生贵)^a, Gao Tao (高涛)^a, Ao Bing-Yun (敖冰云)^b

a Institute of Atomic and Molecular Physics, Sichuan University, Chengdu 610065, China;
b Science and Technology on Surface Physics and Chemistry Laboratory, P. O. Box 9071-35, Jiangyou 621907, China

Received:2015-07-07 Revised:2015-08-05 Online:2015-12-05 Published:2015-12-05
Contact: Gao Tao, Ao Bing-Yun E-mail:gaotao@scu.edu.cn;aobingyun@caep.cn
Supported by:
Project supported by the National Natural Science Foundation of China (Grant Nos. 21371160 and 21401173).

摘要/Abstract

摘要： The electronic structure, magnetic states, chemical bonding, and thermodynamic properties of β-US₂ are investigated by using first-principles calculation through the density functional theory (DFT)+U approach. The obtained band structure exhibits a direct band gap semiconductor at Γ point with a band gap of 0.9 eV for β-US₂, which is in good agreement with the recent experimental data. The charge-density differences, the Bader charge analysis, and the Born effective charges suggest that the U-S bonds of the β-US₂ have a mixture of covalent and ionic characters, but the ionic character is stronger than covalent character. The Raman-active, infrared-active, and silent modes at the Γ point are further assigned and discussed. The obtained optical-mode frequencies indicate that the three apparent LO-TO (longitudinal optical-transverse optical) splittings occur in B_1u, B_2u, and B_3u modes, respectively. Furthermore, the Helmholtz free energy ΔF, the specific heat ΔE, vibrational entropy SM, and constant volume C_V are studied over a range from 0 K～100 K. We expect that our work can provide some valuable information for further experimental investigation of the dielectric properties and the infrared reflectivity spectrum of uranium chalcogenide.

关键词: β-US₂, magnetization, chemical bonding, thermodynamic properties

Abstract: The electronic structure, magnetic states, chemical bonding, and thermodynamic properties of β-US₂ are investigated by using first-principles calculation through the density functional theory (DFT)+U approach. The obtained band structure exhibits a direct band gap semiconductor at Γ point with a band gap of 0.9 eV for β-US₂, which is in good agreement with the recent experimental data. The charge-density differences, the Bader charge analysis, and the Born effective charges suggest that the U-S bonds of the β-US₂ have a mixture of covalent and ionic characters, but the ionic character is stronger than covalent character. The Raman-active, infrared-active, and silent modes at the Γ point are further assigned and discussed. The obtained optical-mode frequencies indicate that the three apparent LO-TO (longitudinal optical-transverse optical) splittings occur in B_1u, B_2u, and B_3u modes, respectively. Furthermore, the Helmholtz free energy ΔF, the specific heat ΔE, vibrational entropy SM, and constant volume C_V are studied over a range from 0 K～100 K. We expect that our work can provide some valuable information for further experimental investigation of the dielectric properties and the infrared reflectivity spectrum of uranium chalcogenide.

Key words: β-US₂, magnetization, chemical bonding, thermodynamic properties

中图分类号: (Strongly correlated electron systems; heavy fermions)

71.27.+a

31.15.ae (Electronic structure and bonding characteristics) 74.25.Bt (Thermodynamic properties)

李世长, 郑远蕾, 马生贵, 高涛, 敖冰云. First-principles calculation of the electronic structure, chemical bonding, and thermodynamic properties of β-US₂[J]. 中国物理B, 2015, 24(12): 127101-127101.

Li Shi-Chang (李世长), Zheng Yuan-Lei (郑远蕾), Ma Sheng-Gui (马生贵), Gao Tao (高涛), Ao Bing-Yun (敖冰云). First-principles calculation of the electronic structure, chemical bonding, and thermodynamic properties of β-US₂[J]. Chin. Phys. B, 2015, 24(12): 127101-127101.

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First-principles calculation of the electronic structure, chemical bonding, and thermodynamic properties of β-US₂

First-principles calculation of the electronic structure, chemical bonding, and thermodynamic properties of β-US₂

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