Coherent Phonon‐Induced Modulation of Charge Transfer in 2D Hybrid Perovskites

Electron–phonon interactions play an essential role in charge transport and transfer processes semiconductors. For most structures, tailoring electron–phonon for specific functionality remains elusive. Here, it is shown that, hybrid perovskites, coherent phonon modes can be used to manipulate transfer. In the 2D double perovskite, (AE2T)2AgBiI8 (AE2T: 5,5“-diylbis(amino-ethyl)-(2,2”-(2)thiophene)), valence band maximum derived from [Ag0.5Bi0.5I4]2– framework lies close proximity AE2T-derived HOMO level, thereby forming a type-II heterostructure. During transient absorption spectroscopy, pulsed excitation creates sustained modes, which periodically modulate associated electronic levels. Thus, energy offset at organic–inorganic interface also oscillates periodically, providing unique opportunity modulation of interfacial Density-functional theory corroborates mechanism identifies as likely drivers These observations are striking example how fundamentally important perovskites.