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Abstract 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)₂AgBiI₈(AE2T: 5,5“‐diylbis(amino‐ethyl)‐(2,2”‐(2)thiophene)), the valence band maximum derived from the [Ag_0.5Bi_0.5I₄]^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. 

Recent successful integration of semiconductors into spintronic THz emitters has demonstrated a new pathway of control over terahertz (THz) radiation through ultrafast demagnetization dynamics. Here, the spintronic THz emission from different ultrawide bandgap (UWBG) semiconductors interfaced with ferromagnets is studied. The authors show that the Schottky barrier in the UWBG semiconductor AlN acts as a spin filter that increases the polarization of the spin current injected from the ferromagnet. Furthermore, the authors show that the two-dimensional electron gas at the interface between Al0.25Ga0.75N and GaN enhances the magnitude of the emitted radiation due to the high spin-to-charge conversion efficiency induced by the Rashba effect that results in a hallmark asymmetry in emission amplitude. The results provide a framework for future engineering of semiconducting/ferromagnet heterostructures for ultrafast communications technologies beyond 5G.