Accelerating ab initio spin-phonon relaxation simulation of single-ion magnets by quantum embedding and spatial truncation
Abstract
Single-ion magnets (SIMs) show promise for high-density storage and quantum computing, but predicting spin-phonon coupling (SPC) and magnetic relaxation remains challenging due to the need for numerous non-equilibrium multiconfigurational calculations. Recent advances in quantum embedding methods offer a potential route to address this issue. In this work, density matrix embedding theory (DMET) combined with complete active space self-consistent field (CASSCF) is benchmarked for the static magnetic properties and spin-phonon coupling (SPC) parameters of Dy3+-based SIMs. The method is further combined with spatial truncation to calculate SPC parameters for these SIMs. It is found that truncating the space near the first coordination sphere reduces the computational cost dramatically while keeping the errors in the effective energy barrier and relaxation time-scale negligible. This study provides a practical calculation framework for accurate and efficient spin dynamics prediction, laying the foundation for the rational design of high-performance single-molecule magnets.
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BibTeX
@misc{deng2026accelerating,
title = {{Accelerating ab initio spin-phonon relaxation simulation of single-ion magnets by quantum embedding and spatial truncation}},
author = {Yifan Deng and Zhe-Bin Guan and Zilong Zou and Zheng Sun and Ze-Wei Li and Bingwu Wang and Hong Jiang},
howpublished = {arXiv},
year = {2026},
month = sep,
doi = {10.48550/arxiv.2609.14371},
eprint = {2609.14371},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2609.14371},
}
RIS
TY - UNPB
TI - Accelerating ab initio spin-phonon relaxation simulation of single-ion magnets by quantum embedding and spatial truncation
AU - Yifan Deng
AU - Zhe-Bin Guan
AU - Zilong Zou
AU - Zheng Sun
AU - Ze-Wei Li
AU - Bingwu Wang
AU - Hong Jiang
PY - 2026
DA - 2026/09/13
PB - arXiv
DO - 10.48550/arxiv.2609.14371
UR - https://arxiv.org/abs/2609.14371
AB - Single-ion magnets (SIMs) show promise for high-density storage and quantum computing, but predicting spin-phonon coupling (SPC) and magnetic relaxation remains challenging due to the need for numerous non-equilibrium multiconfigurational calculations. Recent advances in quantum embedding methods offer a potential route to address this issue. In this work, density matrix embedding theory (DMET) combined with complete active space self-consistent field (CASSCF) is benchmarked for the static magnetic properties and spin-phonon coupling (SPC) parameters of Dy^3+-based SIMs. The method is further combined with spatial truncation to calculate SPC parameters for these SIMs. It is found that truncating the space near the first coordination sphere reduces the computational cost dramatically while keeping the errors in the effective energy barrier and relaxation time-scale negligible. This study provides a practical calculation framework for accurate and efficient spin dynamics prediction, laying the foundation for the rational design of high-performance single-molecule magnets.
ER -