Publication date: 3rd July 2020
Lead halide perovskites (LHPs) demonstrate great potential for optoelectronic applications such as light emitting devices, solar energy harvesting and spintronics. Understanding the spin dynamics of charge carriers in this material could help improving the efficiencies of those applications. Perovskites inhibit large spin-orbit coupling, leading to a significant fine structure splitting, which makes both, the conduction and valence band two-fold degenerate. This allows for efficient optical orientation of charge carriers, making perovskites an ideal material to investigate the spin dynamics of photoinduced charge carriers.
We elucidate the spin dynamics of photoexcited charge carriers and the underlying spin relaxation mechanisms in CsPbI3 nanocrystals by employing time-resolved differential transmission spectroscopy (DTS) [1]. We find that the photoinduced spin polarization significantly diminishes during thermalization and cooling of charge carriers toward the respective band edges. Temperature-dependent DTS reveals a decay in spin polarization that is more than 1 order of magnitude faster at room temperature (3 ps) than at cryogenic temperatures (32 ps). As a result of comparing our experimental data to theoretical models, we propose that spin relaxation of free charge carriers in large-SOC materials like LHPs occurs as a result of carrier−phonon scattering, as described by the Elliott−Yafet mechanism.
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