Hyperfine driven spin relaxation of charge carriers in metal-halide perovskites
Abstract
Spin relaxation of localized charge carriers in semiconductors is primarily governed by hyperfine interaction with the surrounding nuclear spin bath. While this mechanism is well-established in III-V bulk materials and quantum dots, its critical role in metal-halide perovskites (MHPs) has only recently emerged. Their inverted band structure induces an unusual hierarchy of hyperfine couplings, with hole interactions dominating electron interactions, particurlaly in Pb-based perovskites. Here, we adapt a spin relaxation model-originally developed for muon spin spectroscopy-to provide an exact description of longitudinal spin relaxation for localized carriers across arbitrary hyperfine correlation times. This approach is motivated by recent experimental evidence in MAPbI 3 , which places carrier spins in an intermediate correlation regime, where conventional monoexponential approximations fail. Our analysis reveals distinct hyperfine relaxation channels: electrons couple primarily to halogen nuclei, whereas hole interactions are governed by metal nuclei. This leads to a key prediction-perovskites with lighter halogens and metal cations exhibit significantly extended spin relaxation times. Applied to time-resolved Faraday rotation data obtained from two perovskite samples, our model extracts key microscopic parameters-including the carrier localization volume and hyperfine correlation time-demonstrating the necessity for the exact dynamical solution over a single-exponential approximation. These findings provide microscopic insight into hyperfine-driven spin relaxation in MHPs and establish a robust framework for characterizing carrier localization and spin dynamics.
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BibTeX
@article{lague2026hyperfine,
title = {{Hyperfine driven spin relaxation of charge carriers in metal-halide perovskites}},
author = {Guillaume Lagüe and Mauricio Calvo and Hernán Miguez and Olfa Selmi and Iván Mora-Seró and Sofia Masi and Frédérick Bernardot and Christophe Testelin and Maria Chamarro},
journal = {Physical Review B},
year = {2026},
month = oct,
doi = {10.1103/z6h4-c83x},
eprint = {2607.15224},
archivePrefix = {arXiv},
url = {https://hal.science/hal-05841409v1},
note = {CC BY 4.0},
}
RIS
TY - JOUR
TI - Hyperfine driven spin relaxation of charge carriers in metal-halide perovskites
AU - Guillaume Lagüe
AU - Mauricio Calvo
AU - Hernán Miguez
AU - Olfa Selmi
AU - Iván Mora-Seró
AU - Sofia Masi
AU - Frédérick Bernardot
AU - Christophe Testelin
AU - Maria Chamarro
PY - 2026
DA - 2026/10/19
JO - Physical Review B
DO - 10.1103/z6h4-c83x
UR - https://hal.science/hal-05841409v1
AB - Spin relaxation of localized charge carriers in semiconductors is primarily governed by hyperfine interaction with the surrounding nuclear spin bath. While this mechanism is well-established in III-V bulk materials and quantum dots, its critical role in metal-halide perovskites (MHPs) has only recently emerged. Their inverted band structure induces an unusual hierarchy of hyperfine couplings, with hole interactions dominating electron interactions, particurlaly in Pb-based perovskites. Here, we adapt a spin relaxation model-originally developed for muon spin spectroscopy-to provide an exact description of longitudinal spin relaxation for localized carriers across arbitrary hyperfine correlation times. This approach is motivated by recent experimental evidence in MAPbI 3 , which places carrier spins in an intermediate correlation regime, where conventional monoexponential approximations fail. Our analysis reveals distinct hyperfine relaxation channels: electrons couple primarily to halogen nuclei, whereas hole interactions are governed by metal nuclei. This leads to a key prediction-perovskites with lighter halogens and metal cations exhibit significantly extended spin relaxation times. Applied to time-resolved Faraday rotation data obtained from two perovskite samples, our model extracts key microscopic parameters-including the carrier localization volume and hyperfine correlation time-demonstrating the necessity for the exact dynamical solution over a single-exponential approximation. These findings provide microscopic insight into hyperfine-driven spin relaxation in MHPs and establish a robust framework for characterizing carrier localization and spin dynamics.
SN - 2469-9950
SN - 2469-9969
ER -