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Oscillatory Magnetic Circular Dichroism of Free-Carrier Absorption and Determination of the Rashba Dispersions in Hybrid Organic-Inorganic Perovskites

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AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.7b02902

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  1. US Army Research Office [W911NF-17-1-0511]

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Free-carrier absorption (FCA) in a semiconductor provides information about the band on which the free carriers reside, and in the classical limit, follows the omega(-2) law with omega being the photon frequency. In hybrid organic inorganic perovskites (HOIPs), the colossal Rashba effect (RE) results in a new band dispersion, characterized by wavevector vertical bar k vertical bar = k(0) of band extremum and effective mass m*. Here we show that the colossal RE in two-dimensional HOIPs greatly enhances phonon-assisted FCA with a modified frequency dependence and induces a direct transition between the subbands with a resonance at h omega = 4R 2h(2)k(0)(2)/m*, which, under a magnetic field, exhibits a strong oscillatory magnetic circular dichroism (MCD). The MCD spectrum allows a complete and reliable determination of k(0) and m* for conduction and valence bands in HOIPs and helps reveal the microscopic mechanism of their outstanding photovoltaic performance.

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