Spin Dynamics of Electrons and Holes Interacting with Nuclei in MAPbI3 Perovskite Single Crystals

E. Kirstein, D. Yakovlev, E. Zhukov, J. Höcker, V. Dyakonov, and M. Bayer


Methylammonium lead triiodine (MAPbI3) is a material representative of the hybrid organic–inorganic lead halide perovskites which currently attract great attention due to their photovoltaic efficiency and bright optoelectronic properties. Here, the coherent spin dynamics of charge carriers and spin-dependent phenomena induced by the carrier interaction with nuclear spins are studied in MAPbI3 single crystals, using time-resolved Kerr rotation at cryogenic temperatures in magnetic fields up to 3 T. Spin dephasing times up to a few nanoseconds and a longitudinal spin relaxation time of 37 ns are measured. The Larmor spin precession of both resident electrons and holes is identified in the Kerr rotation signals. The Landé factors (g-factors) in the orthorhombic crystal phase show a strong anisotropy, ranging for the holes from −0.28 to −0.71 and for the electrons from +2.46 to +2.98, while the g-factor dispersion of about 1% is rather small. An exciton g-factor of +2.3 is measured by magnetoreflectivity. A dynamic nuclear polarization by means of spin-polarized electrons and holes is achieved in tilted magnetic fields giving access to the carrier–nuclei exchange interaction and the nuclear spin relaxation time exceeding 16 min.

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