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

Publikation: Beitrag in FachzeitschriftForschungsartikelBeigetragenBegutachtung


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


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.


Seiten (von - bis)88-94
FachzeitschriftNature materials
PublikationsstatusVeröffentlicht - 20 Nov. 2023

Externe IDs

PubMed 37985838