Spin dynamics of electrons and holes interacting with nuclei in MAPbI${}_3$ perovskite single crystals

Abstract

Methylammonium lead triiodine (MAPbI${}_3$) is a material representative of the hybrid organic-inorganic lead halide perovskites which attract currently 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 MAPbI${}_3$ 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 magneto-reflectivity. 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 nuclei spin relaxation time exceeding 16 minutes.

References in corpus (7)

• Pump-Probe Faraday Rotation and Ellipticity in an Ensemble of Singly Charged Quantum Dots
• Coherent Spin Precession and Lifetime-Limited Spin Dephasing in CsPbBr3 Perovskite Nanocrystals
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Cited by in corpus (4)

• Coherent Spin Dynamics of Electrons in Two-Dimensional (PEA)${}_2$PbI${}_4$ Perovskites
• Spin Coherence and Spin Relaxation in Hybrid Organic-Inorganic Lead and Mixed Lead-Tin Perovskites
• Rapid spin depolarization in the layered 2D Ruddlesden Popper perovskite (BA)(MA)PbI
• Hyperfine interaction of electrons and holes with nuclei probed by optical orientation in MAPbI${}_3$ perovskite crystals