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Experimental Methods for Spin- and Angle-Resolved Photoemission Spectroscopy Combined with Polarization-Variable Laser
Published on: June 28, 2018
Spin Polarization Dynamics of Free Charge Carriers in CsPbI3 Nanocrystals
Simone Strohmair1, Amrita Dey1, Yu Tong1
1Chair for Photonics and Optoelectronics, Nano-Institute Munich, Department of Physics, Ludwig-Maximilians-Universität (LMU), Königinstr. 10, 80539 Munich, Germany.
Abstract:
Lead halide perovskites (LHPs) exhibit large spin-orbit coupling (SOC), leading to only twofold-degenerate valence and conduction bands and therefore allowing for efficient optical orientation. This makes them ideal materials to study charge carrier spins. With this study 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). We find that the photoinduced spin polarization significantly diminishes during thermalization and cooling toward the energetically favorable band edge. 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). 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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