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Spin-Canting-Controlled Hole Spin Relaxation in Two-Dimensional Magnet CrSBr.
Chenxi Ma1, Haoran Lu1, Run Long1
1College of Chemistry, Key Laboratory of Theoretical & Computational Photochemistry of Ministry of Education, Beijing Normal University, Beijing 100875, People's Republic of China.
The Journal of Physical Chemistry Letters
|January 15, 2026
Summary
Controlling spin dynamics in nanoscale spintronics is key. This study reveals how magnetic-field-induced spin orientation in CrSBr influences hole spin relaxation, showing distinct ultrafast depolarization mechanisms.
Area of Science:
- Condensed Matter Physics
- Quantum Technology
- Materials Science
Background:
- Controlling spin dynamics is crucial for advancing nanoscale spintronics and quantum technologies.
- Understanding hole spin relaxation mechanisms is essential for developing new spintronic devices.
Purpose of the Study:
- To investigate the influence of spin-canting angles on hole spin relaxation in CrSBr.
- To elucidate the mechanistic transition of spin relaxation governed by magnetic-field-induced spin orientation.
Main Methods:
- Utilized interlayer spin-canting angles as a proxy for magnetic-field-induced spin reorientation.
- Employed noncollinear time-dependent density functional theory (TDDFT) combined with nonadiabatic molecular dynamics.
Main Results:
- Hole energy relaxation rates varied with spin-canting angles (90° > 60° ≈ 0° > 30°), influenced by nonadiabatic coupling.
- A mechanistic transition in spin relaxation was observed: ultrafast depolarization via adiabatic spin flips at 0°, and nonadiabatic spin flips at finite angles.
- The 90° configuration exhibited the fastest spin flips due to aligned spin character in valence bands.
Conclusions:
- Magnetic-field-controlled spin orientation significantly governs ultrafast spin dynamics in magnets.
- The findings provide insights into manipulating spin relaxation for spintronic applications.
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