Spintronic Terahertz Emission by Ultrafast Spin-Charge Current Conversion in Reduced Dimensional Organic-Inorganic Hybrid Perovskites*

Reduced Dimensional Hybrid Metal Halides (RD-HMHs) are a new class of synthetic semiconductor prepared via low-temperature solution processing with a wide array of possible chemical and structural arrangements enabled by the versatility of their molecular cations. RD-HMHs have already been shown to possess remarkable photovoltaic, excitonic, and optoelectronic properties, but their rich spintronic functionalities have yet to be utilized. We report the successful observation of the inverse Rashba-Edelstein Effect (IREE) in a 2D HMH (BA)₂(MA)_n-1Pb_nI_3n+1 driven by spin pumping from an adjacent ferromagnetic Ni₈₁Fe₁₉ layer using femtosecond laser pulses. We observed spin-dependent THz radiation at room temperature. The phase of the THz field can be controlled by means of an external magnetic field. Circular polarization dependence of the THz radiation confirms the helicity-dependent directional THz radiation and reveals the Rashba states in the RD-HMH materials. This work opens the door for next generation, low-cost THz emitters with tunable functionalities.