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Uncovering the Electron‐Phonon Interplay and Dynamical Energy‐Dissipation Mechanisms of Hot Carriers in Hybrid Lead Halide Perovskites

Chan, Christopher C. S.; Fan, Kezhou; Wang, Han; Huang, Zhanfeng; Novko, Dino; Yan, Keyou; Xu, Jianbin; Choy, Wallace C. H.; Lončarić, Ivor; Wong, Kam Sing (2021) Uncovering the Electron‐Phonon Interplay and Dynamical Energy‐Dissipation Mechanisms of Hot Carriers in Hybrid Lead Halide Perovskites. Advanced Energy Materials, 11 (9). ISSN 1614-6832

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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.

Item Type: Article
Uncontrolled Keywords: electron phonon coupling ; density functional theory
Subjects: NATURAL SCIENCES > Physics
Divisions: Theoretical Physics Division
Project titleProject leaderProject codeProject type
2D i kvazi-2D perovskiti: od ciljanog strukturnog dizajna do poboljšane učinkovitosti i stabilnostiPopović, JasminkaPZS-2019-02-2068HRZZ
Istraživanje fononski posredovanih procesa u kvazi-dvodimenzionalnim materijalimaNovko, DinoUIP-2019-04-6869HRZZ
Potpora vrhunskim istraživanjima Centra izvrsnosti za napredne materijale i senzoreIvanda, Mile; Jakšić, Milko; Stipčević, Mario; Kralj, MarkoKK.
Sinergijom do uspjeha: RBI-T-WINNING i ESIF udruženi u jačanju izvrsnosti Zavoda za teorijsku fiziku Instituta Ruđer BoškovićMelic, BlazenkaKK.
Depositing User: Ivor Lončarić
Date Deposited: 16 Mar 2021 10:28
DOI: 10.1002/aenm.202003071

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