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Title: Role of electron-phonon coupling in the thermal evolution of bulk Rashba-like spin-split lead halide perovskites exhibiting dual-band photoluminescence
Authors: Steele, Julian A.
Puech, Pascal
Monserrat, Bartomeu
Wu, Bo
Yang, Ruo Xi
Kirchartz, Thomas
Yuan, Haifeng
Fleury, Guillaume
Giovanni, David
Fron, Eduard
Keshavarz, Masoumeh
Debroye, Elke
Zhou, Guofu
Sum, Tze Chien
Walsh, Aron
Hofkens, Johan
Roeffaers, Maarten B. J.
Keywords: Science::Physics::Optics and light
Issue Date: 2019
Source: Steele, J. A., Puech, P., Monserrat, B., Wu., B., Yang, R. X., Kirchartz, T., . . . Roeffaers, M. B. J. (2019). 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, 4(9), 2205-2212. doi:10.1021/acsenergylett.9b01427
Journal: ACS Energy Letters
Abstract: 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.
ISSN: 2380-8195
DOI: 10.1021/acsenergylett.9b01427
DOI (Related Dataset):
Schools: School of Physical and Mathematical Sciences 
Rights: This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Energy Letters, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see
Fulltext Permission: open
Fulltext Availability: With Fulltext
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