中国物理B ›› 2022, Vol. 31 ›› Issue (1): 17103-017103.doi: 10.1088/1674-1056/ac3505

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Defect calculations with quasiparticle correction: A revisited study of iodine defects in CH3NH3PbI3

Ling Li(李玲)1 and Wan-Jian Yin(尹万健)1,2,3,†   

  1. 1 College of Energy, Soochow Institute for Energy and Materials Innovations(SIEMIS), and Jiangsu Provincial Key Laboratory for Advanced Carbon Materials and Wearable Energy Technologies, Soochow University, Suzhou 215006, China;
    2 Light Industry Institute of Electrochemical Power Sources, Soochow University, Suzhou 215006, China;
    3 Key Laboratory of Advanced Optical Manufacturing Technologies of Jiangsu Province&Key Laboratory of Modern Optical Technologies of the Education Ministry of China, Soochow University, Suzhou 215006, China
  • 收稿日期:2021-08-23 修回日期:2021-10-14 接受日期:2021-11-01 出版日期:2021-12-03 发布日期:2021-12-28
  • 通讯作者: Wan-Jian Yin E-mail:wjyin@suda.edu.cn
  • 基金资助:
    Project supported by the National Natural Science Foundation of China (Grant No. 11974257), the Distinguished Young Talent Funding of Jiangsu Province, China (Grant No. BK20200003), the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD). DFT calculations were carried out at the National Supercomputer Center in Tianjin [TianHe-1(A)].

Defect calculations with quasiparticle correction: A revisited study of iodine defects in CH3NH3PbI3

Ling Li(李玲)1 and Wan-Jian Yin(尹万健)1,2,3,†   

  1. 1 College of Energy, Soochow Institute for Energy and Materials Innovations(SIEMIS), and Jiangsu Provincial Key Laboratory for Advanced Carbon Materials and Wearable Energy Technologies, Soochow University, Suzhou 215006, China;
    2 Light Industry Institute of Electrochemical Power Sources, Soochow University, Suzhou 215006, China;
    3 Key Laboratory of Advanced Optical Manufacturing Technologies of Jiangsu Province&Key Laboratory of Modern Optical Technologies of the Education Ministry of China, Soochow University, Suzhou 215006, China
  • Received:2021-08-23 Revised:2021-10-14 Accepted:2021-11-01 Online:2021-12-03 Published:2021-12-28
  • Contact: Wan-Jian Yin E-mail:wjyin@suda.edu.cn
  • Supported by:
    Project supported by the National Natural Science Foundation of China (Grant No. 11974257), the Distinguished Young Talent Funding of Jiangsu Province, China (Grant No. BK20200003), the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD). DFT calculations were carried out at the National Supercomputer Center in Tianjin [TianHe-1(A)].

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摘要： Defect levels in semiconductor band gaps play a crucial role in functionalized semiconductors for practical applications in optoelectronics; however, first-principle defect calculations based on exchange-correlation functionals, such as local density approximation, grand gradient approximation (GGA), and hybrid functionals, either underestimate band gaps or misplace defect levels. In this study, we revisited iodine defects in CH3NH3PbI3 by combining the accuracy of total energy calculations of GGA and single-electron level calculation of the GW method. The combined approach predicted neutral Im i to be unstable and the transition level of Im i(+1/-1) to be close to the valence band maximum. Therefore, Im i may not be as detrimental as previously reported. Moreover, Vm I may be unstable in the -1 charged state but could still be detrimental owing to the deep transition level of Vm I(+1/0). These results could facilitate the further understanding of the intrinsic point defect and defect passivation observed in CH3NH3PbI3.

关键词: quasiparticle correction, defect calculation, GW theory, methylammonium lead iodide

Abstract: Defect levels in semiconductor band gaps play a crucial role in functionalized semiconductors for practical applications in optoelectronics; however, first-principle defect calculations based on exchange-correlation functionals, such as local density approximation, grand gradient approximation (GGA), and hybrid functionals, either underestimate band gaps or misplace defect levels. In this study, we revisited iodine defects in CH3NH3PbI3 by combining the accuracy of total energy calculations of GGA and single-electron level calculation of the GW method. The combined approach predicted neutral Im i to be unstable and the transition level of Im i(+1/-1) to be close to the valence band maximum. Therefore, Im i may not be as detrimental as previously reported. Moreover, Vm I may be unstable in the -1 charged state but could still be detrimental owing to the deep transition level of Vm I(+1/0). These results could facilitate the further understanding of the intrinsic point defect and defect passivation observed in CH3NH3PbI3.

Key words: quasiparticle correction, defect calculation, GW theory, methylammonium lead iodide

中图分类号:  (Density functional theory, local density approximation, gradient and other corrections)

  • 71.15.Mb
61.72.Bb (Theories and models of crystal defects) 31.15.xm (Quasiparticle methods)