Journal
ACS ENERGY LETTERS
Volume 4, Issue 9, Pages 2205-2212Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.9b01427
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Funding
- Research Foundation -Flanders (FWO) [12Y7218N, G.0197.11, 12Y6418N, 1203719N]
- KU Leuven Research Fund [C14/15/053]
- Flemish government through long term structural funding Methusalem (CASAS2) [Meth/15/04]
- Hercules foundation [HER/11/14]
- Belgian Federal Science Policy Office [IAP-VII/05]
- European Research Council under the European Union [307523]
- Winton Programme for the Physics of Sustainability
- Robinson College, Cambridge
- Cambridge Philosophical Society
- National Natural Science Foundation of China (NFSC) [51802331]
- Guangdong Provincial Key Laboratory of Optical Information Materials and Technology [2017B030301007]
- 111 Project
- Impulsund Vernetzungsfonds der Helmholtz Gemeinschaft via the project PEROSEED
- EPSRC [EP/P020194/1]
- Ministry of Education AcRF Tier 2 Grant [MOE2016-T2-1-034, MOE2017-T2-1-001]
- Singapore National Research Foundation [NRF-NRFI-2018-04]
- EPSRC [EP/P020194/1] Funding Source: UKRI
- European Research Council (ERC) [307523] Funding Source: European Research Council (ERC)
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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 APbBr(3) (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.
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