How spin relaxes and dephases in bulk halide perovskites

Junqing Xu, Kejun Li, Uyen N. Huynh, Mayada Fadel, Jinsong Huang, Ravishankar Sundararaman (), Valy Vardeny () and Yuan Ping ()
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Junqing Xu: Hefei University of Technology
Kejun Li: University of California
Uyen N. Huynh: University of Utah
Mayada Fadel: Rensselaer Polytechnic Institute
Jinsong Huang: University of North Carolina
Ravishankar Sundararaman: Rensselaer Polytechnic Institute
Valy Vardeny: University of Utah
Yuan Ping: University of California

Nature Communications, 2024, vol. 15, issue 1, 1-13

Abstract: Abstract Spintronics in halide perovskites has drawn significant attention in recent years, due to their highly tunable spin-orbit fields and intriguing interplay with lattice symmetry. Here, we perform first-principles calculations to determine the spin relaxation time (T1) and ensemble spin dephasing time ( $${T}_{2}^{*}$$ T 2 * ) in a prototype halide perovskite, CsPbBr3. To accurately capture spin dephasing in external magnetic fields we determine the Landé g-factor from first principles and take it into account in our calculations. These allow us to predict intrinsic spin lifetimes as an upper bound for experiments, identify the dominant spin relaxation pathways, and evaluate the dependence on temperature, external fields, carrier density, and impurities. We find that the Fröhlich interaction that dominates carrier relaxation contributes negligibly to spin relaxation, consistent with the spin-conserving nature of this interaction. Our theoretical approach may lead to new strategies to optimize spin and carrier transport properties.

Date: 2024
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DOI: 10.1038/s41467-023-42835-w

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