1. Uncovering the Electron‐Phonon Interplay and Dynamical Energy‐Dissipation Mechanisms of Hot Carriers in Hybrid Lead Halide Perovskites
- Author
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Keyou Yan, Jianbin Xu, Han Wang, Kam Sing Wong, Wallace C. H. Choy, Christopher C. S. Chan, Dino Novko, Ivor Lončarić, Zhanfeng Huang, and Kezhou Fan
- Subjects
Materials science ,Renewable Energy, Sustainability and the Environment ,business.industry ,Physics ,electron phonon coupling ,density functional theory ,02 engineering and technology ,Dissipation ,010402 general chemistry ,021001 nanoscience & nanotechnology ,Polaron ,01 natural sciences ,7. Clean energy ,0104 chemical sciences ,Condensed Matter::Materials Science ,Semiconductor ,Chemical physics ,Ultrafast laser spectroscopy ,General Materials Science ,Density functional theory ,0210 nano-technology ,business ,Spectroscopy ,Excitation ,Perovskite (structure) - Abstract
The discovery of slow hot carrier cooling in hybrid organic–inorganic lead halide perovskites (HOIPs) has provided exciting prospects for efficient solar cells that can overcome the Shockley–Queisser limit. Questions still loom over how electron‐phonon interactions differ from traditional polar semiconductors. Herein, the electron‐phonon coupling (EPC) strength of common perovskite films (MAPbBr3, MAPbI3, CsPbI3, and FAPbBr3) is obtained using transient absorption spectroscopy by analyzing the hot carrier cooling thermodynamics via a simplified two‐temperature model. Density function theory calculations are numerically performed at relevant electron‐temperatures to confirm experiments. Further, the variation of carrier‐temperature over a large range of carrier‐densities in HOIPs is analyzed, and an “S‐shaped” dependence of the initial carrier‐temperature to carrier‐density is reported. The phenomenon is attributed to the dominance of the large polaron screening and the destabilization effect which causes an increasing‐decreasing fluctuation in temperature at low excitation powers ; and a hot‐phonon bottleneck which effectively increases the carrier temperature at higher carrier‐densities. The turning point in the relationship is indicative of the critical Mott density related to the nonmetal‐metal transition. The EPC analysis provides a novel perspective to quantify the energy transfer in HOIPs, electron‐lattice subsystem, and the complicated screening‐bottleneck interplay is comprehensively described, resolving the existing experimental contradictions.
- Published
- 2021