How spin relaxes and dephases in bulk halide perovskites

Xu, Junqing; Li, Kejun; Huynh, Uyen N.; Fadel, Mayada; Huang, Jinsong; Sundararaman, Ravishankar; Vardeny, Valy; Ping, Yuan

doi:10.1038/s41467-023-42835-w

Title: How spin relaxes and dephases in bulk halide perovskites

Journal Article · 01 January 2024 · Nature Communications

DOI: https://doi.org/10.1038/s41467-023-42835-w · OSTI ID:2274847

Xu, Junqing;

; Huynh, Uyen N.;

;

; Sundararaman, Ravishankar; Vardeny, Valy;

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 ( T ₁ ) and ensemble spin dephasing time ( $$$${T}_{2}^{*}$$$$ $T_{2}^{*}$ ) in a prototype halide perovskite, CsPbBr ₃ . 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.

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Research Organization:: Board of Regents of the University of Wisconsin System, operating as University of Wisconsin-Madison; Brookhaven National Laboratory (BNL), Upton, NY (United States); University of California, Oakland, CA (United States); University of California, Santa Cruz, CA (United States)

Sponsoring Organization:: DOE | SC | Basic Energy Sciences; National Science Foundation (NSF); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; SC0012704; SC0023301; SC0024891

OSTI ID:: 2274847

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 15; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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Title: How spin relaxes and dephases in bulk halide perovskites

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