Journal
ADVANCED FUNCTIONAL MATERIALS
Volume 33, Issue 21, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.202213021
Keywords
coherent phonons; charge transfer; hybrid perovskites; density functional theory
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Electron-phonon interactions are shown to manipulate charge transfer in hybrid perovskites, using coherent phonon modes. The energy offset at the organic-inorganic interface oscillates periodically, providing a unique opportunity for the modulation of interfacial charge transfer. These observations demonstrate how electron-phonon interactions can be used to manipulate fundamental charge and energy transfer processes in hybrid perovskites.
Electron-phonon interactions play an essential role in charge transport and transfer processes in semiconductors. For most structures, tailoring electron-phonon interactions for specific functionality remains elusive. Here, it is shown that, in hybrid perovskites, coherent phonon modes can be used to manipulate charge transfer. In the 2D double perovskite, (AE2T)(2)AgBiI8 (AE2T: 5,5-diylbis(amino-ethyl)-(2,2-(2)thiophene)), the valence band maximum derived from the [Ag0.5Bi0.5I4](2-) framework lies in close proximity to the AE2T-derived HOMO level, thereby forming a type-II heterostructure. During transient absorption spectroscopy, pulsed excitation creates sustained coherent phonon modes, which periodically modulate the associated electronic levels. Thus, the energy offset at the organic-inorganic interface also oscillates periodically, providing a unique opportunity for modulation of interfacial charge transfer. Density-functional theory corroborates the mechanism and identifies specific phonon modes as likely drivers of the coherent charge transfer. These observations are a striking example of how electron-phonon interactions can be used to manipulate fundamentally important charge and energy transfer processes in hybrid perovskites.
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