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

Research output: Contribution to journalResearch articleContributedpeer-review

Contributors

  • Nathaniel P. Gallop - , Imperial College London (Author)
  • Dmitry R. Maslennikov - , Imperial College London (Author)
  • Navendu Mondal - , Imperial College London (Author)
  • Katelyn P. Goetz - , Chair of Emerging Electronic Technologies (gB/IFW and cfaed) (Author)
  • Zhenbang Dai - , University of Pennsylvania (Author)
  • Aaron M. Schankler - , University of Pennsylvania (Author)
  • Woongmo Sung - , RIKEN (Author)
  • Satoshi Nihonyanagi - , RIKEN, RIKEN Center for Advanced Photonics (Author)
  • Tahei Tahara - , RIKEN, RIKEN Center for Advanced Photonics (Author)
  • Maryna I. Bodnarchuk - , ETH Zurich, Swiss Federal Laboratories for Materials Science and Technology (Empa) (Author)
  • Maksym V. Kovalenko - , ETH Zurich, Swiss Federal Laboratories for Materials Science and Technology (Empa) (Author)
  • Yana Vaynzof - , Chair of Emerging Electronic Technologies (gB/IFW and cfaed), Leibniz Institute for Solid State and Materials Research Dresden (Author)
  • Andrew M. Rappe - , University of Pennsylvania (Author)
  • Artem A. Bakulin - , Imperial College London (Author)

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.

Details

Original languageEnglish
Pages (from-to)88-94
Number of pages7
JournalNature materials
Volume23
Issue number1
Early online date20 Nov 2023
Publication statusPublished - Jan 2024
Peer-reviewedYes

External IDs

PubMed 37985838