Ultrafast vibrational control of organohalide perovskite optoelectronic devices using vibrationally promoted electronic resonance
Author(s)
Type
Journal Article
Abstract
Vibrational control (VC) of photochemistry through the optical stimulation of structural dynamics is a nascent concept only recently demonstrated for model molecules in solution. Extending VC to state-of-the-art materials may lead to new applications and improved performance for optoelectronic devices. Metal halide perovskites are promising targets for VC due to their mechanical softness and the rich array of vibrational motions of both their inorganic and organic sublattices. Here, we demonstrate the ultrafast VC of FAPbBr3 perovskite solar cells via intramolecular vibrations of the formamidinium cation using spectroscopic techniques based on vibrationally promoted electronic resonance. The observed short (~300 fs) time window of VC highlights the fast dynamics of coupling between the cation and inorganic sublattice. First-principles modelling reveals that this coupling is mediated by hydrogen bonds that modulate both lead halide lattice and electronic states. Cation dynamics modulating this coupling may suppress non-radiative recombination in perovskites, leading to photovoltaics with reduced voltage losses.
Date Issued
2024-01
Date Acceptance
2023-10-12
Citation
Nature Materials, 2024, 23 (1), pp.88-94
ISSN
1476-1122
Publisher
Nature Research
Start Page
88
End Page
94
Journal / Book Title
Nature Materials
Volume
23
Issue
1
Copyright Statement
© The Author(s) 2023 Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.
License URL
Identifier
https://www.nature.com/articles/s41563-023-01723-w
Subjects
Chemistry
Chemistry, Physical
HALIDE PEROVSKITES
LEAD IODIDE PEROVSKITES
Materials Science
Materials Science, Multidisciplinary
MOLECULAR-DYNAMICS
ORGANIC CATION
Physical Sciences
Physics
Physics, Applied
Physics, Condensed Matter
ROTATION
Science & Technology
SPECTROSCOPY
Technology
Publication Status
Published
Date Publish Online
2023-11-20