Quasiparticle band gap of organic-inorganic hybrid perovskites: Crystal structure, spin-orbit coupling, and self-energy effects

被引:70
作者
Gao, Weiwei [1 ]
Gao, Xiang [2 ]
Abtew, Tesfaye A. [1 ]
Sun, Yi-Yang [3 ]
Zhang, Shengbai [3 ]
Zhang, Peihong [1 ,2 ]
机构
[1] SUNY Buffalo, Dept Phys, Buffalo, NY 14260 USA
[2] Beijing Computat Sci Res Ctr, Beijing 100084, Peoples R China
[3] Rensselaer Polytech Inst, Dept Phys Appl Phys & Astron, Troy, NY 12180 USA
基金
中国国家自然科学基金; 美国国家科学基金会;
关键词
TIN HALIDE PEROVSKITES; PHASE-TRANSITIONS; OPTICAL-PROPERTIES; HIGH-PERFORMANCE; LEAD IODIDE; SOLAR-CELLS; ELECTRON; SEMICONDUCTORS; CH3NH3PBI3; INSULATORS;
D O I
10.1103/PhysRevB.93.085202
中图分类号
T [工业技术];
学科分类号
08 ;
摘要
The quasiparticle band gap is one of the most important materials properties for photovoltaic applications. Often the band gap of a photovoltaic material is determined (and can be controlled) by various factors, complicating predictive materials optimization. An in-depth understanding of how these factors affect the size of the gap will provide valuable guidance for new materials discovery. Here we report a comprehensive investigation on the band gap formation mechanism in organic-inorganic hybrid perovskites by decoupling various contributing factors which ultimately determine their electronic structure and quasiparticle band gap. Major factors, namely, quasiparticle self-energy, spin-orbit coupling, and structural distortions due to the presence of organic molecules, and their influences on the quasiparticle band structure of organic-inorganic hybrid perovskites are illustrated. We find that although methylammonium cations do not contribute directly to the electronic states near band edges, they play an important role in defining the band gap by introducing structural distortions and controlling the overall lattice constants. The spin-orbit coupling effects drastically reduce the electron and hole effective masses in these systems, which is beneficial for high carrier mobilities and small exciton binding energies.
引用
收藏
页数:7
相关论文
共 61 条
[1]  
[Anonymous], ENERGY ENV SCI
[2]   Synthesis and crystal chemistry of the hybrid perovskite (CH3NH3) PbI3 for solid-state sensitised solar cell applications [J].
Baikie, Tom ;
Fang, Yanan ;
Kadro, Jeannette M. ;
Schreyer, Martin ;
Wei, Fengxia ;
Mhaisalkar, Subodh G. ;
Graetzel, Michael ;
White, Tim J. .
JOURNAL OF MATERIALS CHEMISTRY A, 2013, 1 (18) :5628-5641
[3]   Ab initio investigation of hybrid organic-inorganic perovskites based on tin halides [J].
Borriello, Ivo ;
Cantele, Giovanni ;
Ninno, Domenico .
PHYSICAL REVIEW B, 2008, 77 (23)
[4]   Lattice dynamics and vibrational spectra of the orthorhombic, tetragonal, and cubic phases of methylammonium lead iodide [J].
Brivio, Federico ;
Frost, Jarvist M. ;
Skelton, Jonathan M. ;
Jackson, Adam J. ;
Weber, Oliver J. ;
Weller, Mark T. ;
Goni, Alejandro R. ;
Leguy, Aurelien M. A. ;
Barnes, Piers R. F. ;
Walsh, Aron .
PHYSICAL REVIEW B, 2015, 92 (14)
[5]   Relativistic quasiparticle self-consistent electronic structure of hybrid halide perovskite photovoltaic absorbers [J].
Brivio, Federico ;
Butler, Keith T. ;
Walsh, Aron ;
van Schilfgaarde, Mark .
PHYSICAL REVIEW B, 2014, 89 (15)
[6]   Structural and electronic properties of hybrid perovskites for high-efficiency thin-film photovoltaics from first-principles [J].
Brivio, Federico ;
Walker, Alison B. ;
Walsh, Aron .
APL MATERIALS, 2013, 1 (04)
[7]   Layer-by-Layer Growth of CH3NH3PbI3-xClx for Highly Efficient Planar Heterojunction Perovskite Solar Cells [J].
Chen, Yonghua ;
Chen, Tao ;
Dai, Liming .
ADVANCED MATERIALS, 2015, 27 (06) :1053-1059
[8]   Organometallic Halide Perovskites: Sharp Optical Absorption Edge and Its Relation to Photovoltaic Performance [J].
De Wolf, Stefaan ;
Holovsky, Jakub ;
Moon, Soo-Jin ;
Loeper, Philipp ;
Niesen, Bjoern ;
Ledinsky, Martin ;
Haug, Franz-Josef ;
Yum, Jun-Ho ;
Ballif, Christophe .
JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 2014, 5 (06) :1035-1039
[9]   BerkeleyGW: A massively parallel computer package for the calculation of the quasiparticle and optical properties of materials and nanostructures [J].
Deslippe, Jack ;
Samsonidze, Georgy ;
Strubbe, David A. ;
Jain, Manish ;
Cohen, Marvin L. ;
Louie, Steven G. .
COMPUTER PHYSICS COMMUNICATIONS, 2012, 183 (06) :1269-1289
[10]   Temperature Dependence of the Band Gap of CH3NH3PbI3 Stabilized with PMMA: A Modulated Surface Photovoltage Study [J].
Dittrich, Thomas ;
Awino, Celline ;
Prajongtat, Pongthep ;
Rech, Bernd ;
Lux-Steiner, Martha Ch. .
JOURNAL OF PHYSICAL CHEMISTRY C, 2015, 119 (42) :23968-23972