Spin Dynamics in Hybrid Halide Perovskites -Effect of Dynamical and Permanent Symmetry Breaking

Congratulations to Kejun Li, Junqing Xu, Mayank Gupta, Jacopo Simoni and Yuan Ping for their work with Uyen N. Huynh, Rikard Bodin, Christian Multunas, Ravishankar Sundararaman and Valy Vardeny on “Spin Dynamics in Hybrid Halide Perovskites -Effect of Dynamical and Permanent Symmetry Breaking”, published in The Journal of Physical Chemistry Letters! Link to the published article.

 

The hybrid organic-inorganic halide perovskite (HOIP), for example MAPbBr3, exhibits extended spin lifetime and apparent spin lifetime anisotropy in experiments. The underlying mechanisms of these phenomena remain elusive. By utilizing our first-principles density matrix dynamics approach with quantum scatterings including electron-phonon and electron-electron interactions and self-consistent spin-orbit coupling, we present temperature- and magnetic field-dependent spin lifetimes in hybrid perovskites, in agreement with experimental observations. For centrosymmetric hybrid perovskite MAPbBr3, the experimentally observed spin lifetime anisotropy is mainly attributed to the dynamical Rashba effect arising from the interaction between organic and inorganic components and the rotation of the organic cation. For noncentrosymmetric perovskite, such as MPSnBr3, we found persistent spin helix texture at the conduction band minimum, which significantly enhances the spin lifetime anisotropy. Our study provides theoretical insight to spin dynamics in HOIP and strategies for controlling and optimizing spin transport.