Unexpected Anisotropy of the Electron and Hole Landé g-Factors in Perovskite CH3NH3PbI3 Polycrystalline Films.

In this work, we studied, at low temperature, the coherent evolution of the localized electron and hole spins in a polycrystalline film of CH3NH3PbI3 (MAPI) by using a picosecond-photo-induced Faraday rotation technique in an oblique magnetic field. We observed an unexpected anisotropy for the electron and hole spin. We determined the electron and hole Landé factors when the magnetic field was applied in the plane of the film and perpendicular to the exciting light, denoted as transverse ⟂ factors, and when the magnetic field was applied perpendicular to the film and parallel to the exciting light, denoted as parallel ∥ factors. We obtained |ge,⟂|=2.600 ± 0.004, |ge,∥|=1.604 ± 0.033 for the electron and |gh,⟂|=0.406 ± 0.002, |gh,∥|=0.299 ± 0.007 for the hole. Possible origins of this anisotropy are discussed herein.

Energy Tuning of Electronic Spin Coherent Evolution in Methylammonium Lead Iodide Perovskites.

We investigated the coherent evolution of the electronic spin at low temperature in high-quality CH3NH3PbI3 polycrystalline films by picosecond-resolved photoinduced Faraday rotation. We show that this coherent evolution can be tuned by choosing the pump-probe energy within the lowest optical-absorption band, and we explain it as the result of two main contributions: the localized electron and the localized hole. Their corresponding amplitude ratios are not constant across the lowest absorption band-an observation which disqualifies a free exciton from being at the origin of the electronic spin coherent evolution. We measured a spin coherence time of localized electrons (holes) of 4.4 ns (3.7 ns) at 1.635 eV, which evolves to about 7 ns at 1.612 eV (the hole coherence time remains almost constant at lower energies). Finally, we provide a global image of the spin coherent evolution in bulk metal halide perovskite, which overcomes recent controversies.