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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, we show that, in hybrid perovskites, coherent phonon modes can be used to manipulate charge transfer. In the two-dimensional double perovskite, (AE2T)2AgBiI8 (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.
Acknowledgments: D.S., K.G., X.Q., V.B., M.K.J., D.B.M., S.J., and W.Y., acknowledge support from the NSF DMREF program under grant numbers DMR-1729297, DMR-1728921, and DMR-1729383. The authors acknowledge the NCSU Imaging and Kinetic Spectroscopy facility. S.M.J. thanks the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) for a postdoctoral fellowship, Grant No. 393196393.... [Read More]
Total Size
3 files (1.81 GB)
Data Citation
Qin, X., Blum, V. (2023). Phonon and Raman caculation data from: Coherent Phonon‐Induced Modulation of Charge Transfer in 2D Hybrid Perovskites. Duke Research Data Repository. https://doi.org/10.7924/r4mc93m7j
Seyitliyev, D., Qin, X., Jana, M. K., Janke, S. M., Zhong, X., You, W., Mitzi, D. B., Blum, V. & Gundogdu, K. (2023). Coherent Phonon-Induced Modulation of Charge Transfer in 2D Hybrid Perovskites. Advanced Functional Materials 33(21). https://doi.org/10.1002/adfm.202213021
