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   

  1. 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   

  1. 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: 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 B1u, B2u, and B3u modes, respectively. Furthermore, the Helmholtz free energy ΔF, the specific heat ΔE, vibrational entropy SM, and constant volume CV 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 B1u, B2u, and B3u modes, respectively. Furthermore, the Helmholtz free energy ΔF, the specific heat ΔE, vibrational entropy SM, and constant volume CV 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)