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Title: Picosecond charge localization dynamics in CH₃NH₃PbI₃ perovskite probed by infrared-activated vibrations
Authors: Stallhofer, Klara
Nuber, Matthias
Cortecchia, Daniele
Bruno, Annalisa
Kienberger, Reinhard
Deschler, Felix
Soci, Cesare
Iglev, Hristo
Keywords: Science::Physics
Issue Date: 2021
Source: Stallhofer, K., Nuber, M., Cortecchia, D., Bruno, A., Kienberger, R., Deschler, F., Soci, C. & Iglev, H. (2021). Picosecond charge localization dynamics in CH₃NH₃PbI₃ perovskite probed by infrared-activated vibrations. Journal of Physical Chemistry Letters, 12(18), 4428-4433.
Project: NRF-CRP14-2014-03 
Journal: Journal of Physical Chemistry Letters 
Abstract: Hybrid metal halide perovskites exhibit well-defined semiconducting properties and efficient optoelectronic performance considering their soft crystal structure and low-energy lattice motions. The response of such a crystal lattice to light-induced charges is a fundamental question, for which experimental insight into ultrafast time scales is still sought. Here, we use infrared-activated vibrations (IRAV) of the organic components within the hybrid perovskite lattice as a sensitive probe for local structural reorganizations after photoexcitation, with femtosecond resolution. We find that the IRAV signal response shows a delayed rise of about 3 ps and subsequent decay of pronounced monomolecular character, distinguishing it from absorption associated with free carriers. We interpret our results as a two-step carrier localization process. Initially, carriers localize transiently in local energy minima formed by lattice fluctuations. A subpopulation of these can then fall into deeper trapped states over picoseconds, likely due to local reorganization of the organic molecules surrounding the carriers.
ISSN: 1948-7185
DOI: 10.1021/acs.jpclett.1c00935
Schools: Interdisciplinary Graduate School (IGS) 
School of Physical and Mathematical Sciences 
Research Centres: Energy Research Institute @ NTU (ERI@N) 
Rights: This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of Physical Chemistry Letters, copyright © 2021 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
Appears in Collections:ERI@N Journal Articles
IGS Journal Articles
SPMS Journal Articles

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