Ultrafast vibrational control of organohalide perovskite optoelectronic devices using vibrationally promoted electronic resonance


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Date

2024-01

Publication Type

Journal Article

ETH Bibliography

yes

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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 FAPbBr(3) perovskite solar cells via intramolecular vibrations of the formamidinium cation using spectroscopic techniques based on vibrationally promoted electronic resonance. The observed short (similar to 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.

Publication status

published

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Volume

23 (1)

Pages / Article No.

88 - 94

Publisher

Nature

Event

Edition / version

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Organisational unit

03934 - Kovalenko, Maksym / Kovalenko, Maksym check_circle

Notes

Funding

192308 - Q-Light - Engineered Quantum Light Sources with Nanocrystal Assemblies (SNF)

Related publications and datasets

Is supplemented by: 10.5281/zenodo.8398385