Role of Electron–Phonon Coupling in the Thermal Evolution of Bulk Rashba-Like Spin-Split Lead Halide Perovskites Exhibiting Dual-Band Photoluminescence,ACS Energy Letters

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Role of Electron–Phonon Coupling in the Thermal Evolution of Bulk Rashba-Like Spin-Split Lead Halide Perovskites Exhibiting Dual-Band Photoluminescence
ACS Energy Letters ( IF 19.3 ) Pub Date : 2019-08-19 00:00:00 , DOI: 10.1021/acsenergylett.9b01427
Julian A. Steele ₁ , Pascal Puech ₂ , Bartomeu Monserrat ₃ , Bo Wu ₄ , Ruo Xi Yang ₅ , Thomas Kirchartz _{6,

7} , Haifeng Yuan ₈ , Guillaume Fleury ₁ , David Giovanni ₉ , Eduard Fron ₈ , Masoumeh Keshavarz ₈ , Elke Debroye ₈ , Guofu Zhou ₄ , Tze Chien Sum ₉ , Aron Walsh _{10,

11} , Johan Hofkens ₈ , Maarten B. J. Roeffaers ₁

Affiliation

cMACS, Department of Microbial and Molecular Systems, KU Leuven, Celestijnenlaan 200F, 3001 Leuven, Belgium
CEMES/CNRS, Université de Toulouse, 29, rue Jeanne Marvig, 31055 Toulouse, France
TCM Group, Cavendish Laboratory, University of Cambridge, J. J. Thomson Avenue, Cambridge CB3 0HE, United Kingdom
Guangdong Provincial Key Laboratory of Optical Information Materials and Technology & Institute of Electronic Paper Displays, South China Academy of Advanced Optoelectronics, South China Normal University, Guangzhou 510006, People’s Republic of China
Molecular Foundry, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, California 94720, United States
IEK5-Photovoltaics, Forschungszentrum Jülich, 52425 Jülich, Germany
Faculty of Engineering and CENIDE, University of Duisburg−Essen, Carl-Benz-Straße 199, 47057 Duisburg, Germany
Department of Chemistry, KU Leuven, Celestijnenlaan 200F, 3001 Leuven, Belgium
Division of Physics and Applied Physics, School of Physical and Mathematical Sciences, Nanyang Technological University, 21 Nanyang Link, Singapore 637371, Singapore
Department of Materials, Imperial College London, Exhibition Road, London SW7 2AZ, United Kingdom
Global E3 Institute and Department of Materials Science and Engineering, Yonsei University, Seoul 120-749, Korea

The optoelectronic properties of lead halide perovskites strongly depend on their underlying crystal symmetries and dynamics, sometimes exhibiting a dual photoluminescence (PL) emission via Rashba-like effects. Here we exploit spin- and temperature-dependent PL to study single-crystal APbBr₃ (A = Cs and methylammonium; CH₃NH₃) and evaluate the peak energy, intensity, and line width evolutions of their dual emission. Both perovskites exhibit temperature trends governed by two temperature regimes—above and below approximately 100 K—which impose different carrier scattering and radiative recombination dynamics. With increasing temperature, high-energy optical phonons activate near 100 K to drive energy splitting of the dual bands and induce line width broadening via electron–phonon coupling, with a stronger coupling constant inferred for carriers recombining by the spin-split indirect bands, compared to the direct ones. We find that the unusual thermal evolutions of all-inorganic and hybrid bulk lead bromide perovskites are comparable, suggesting A-site independence and the dominance of dynamic effects, and are best understood within a framework that accounts for Rashba-like effects.

中文翻译：

电子-声子耦合在大体积Rashba样自旋分裂卤化钙钛矿中的热演化过程中的作用，具有双带光致发光

卤化钙钛矿的光电性能在很大程度上取决于其潜在的晶体对称性和动力学，有时通过类Rashba效应表现出双重光致发光（PL）发射。在这里，我们利用自旋和温度相关的PL研究单晶APbBr ₃（A = Cs和甲基铵； CH ₃ NH ₃），并评估其双重发射的峰值能量，强度和线宽演变。两种钙钛矿均显示出受两个温度范围（约100 K以上和以下）控制的温度趋势，这两种情况强加了不同的载流子散射和辐射复合动力学。随着温度的升高，高能光学声子在100 K附近激活，以驱动双带分裂，并通过电子-声子耦合引起线宽加宽，与自旋分裂间接带重组的载流子相比，耦合常数更强。到直接的。我们发现，全无机和杂化散装溴化铅钙钛矿的异常热演化具有可比性，表明A位独立性和动态效应占主导地位，

更新日期：2019-08-19

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