Revealing angular momentum transfer channels and timescales in the ultrafast demagnetization process of ferromagnetic semiconductors
Abstract
Ultrafast control of magnetic order by light provides a promising realization for spintronic devices beyond Moore’s Law and has stimulated intense research interest in recent years. Yet, despite 2 decades of debates, the key question of how the spin angular momentum flows on the femtosecond timescale remains open. The lack of direct first-principle methods and pictures for such process exacerbates the issue. Here, we unravel the laser-induced demagnetization mechanism of ferromagnetic semiconductor GaMnAs, using an efficient time-dependent density functional theory approach that enables the direct real-time snapshot of the demagnetization process. Our results show a clear spin-transfer trajectory from the localized Mn-d electrons to itinerant carriers within 20 fs, illustrating the dominant role of $$\textit{sp–d}$$ interaction. We find that the total spin of localized electrons and itinerant carriers is not conserved in the presence of spin-orbit coupling (SOC). Immediately after laser excitation, a growing percentage of spin-angular momentum is quickly transferred to the electron orbital via SOC in about 1 ps, then slowly to the lattice via electron–phonon coupling in a few picoseconds, responsible for the 2-stage process observed experimentally. The spin-relaxation time via SOC is about 300 fs for itinerant carriers and about 700 fs for Mn-d electrons. These results provide a quantum-mechanical microscopic picture for the long-standing questions regarding the channels and timescales of spin transfer, as well as the roles of different interactions underlying the GaMnAs demagnetization process.
- Authors:
-
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Chinese Academy of Sciences (CAS), Beijing (China)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; National Natural Science Foundation of China (NSFC)
- OSTI Identifier:
- 1577616
- Grant/Contract Number:
- AC02-05CH11231; 61888102
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Proceedings of the National Academy of Sciences of the United States of America
- Additional Journal Information:
- Journal Volume: 116; Journal Issue: 39; Journal ID: ISSN 0027-8424
- Publisher:
- National Academy of Sciences
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; science & technology; semiconductor magnetism; ultrafast; quantum simulation; angular momentum
Citation Formats
Chen, Zhanghui, Luo, Jun-Wei, and Wang, Lin-Wang. Revealing angular momentum transfer channels and timescales in the ultrafast demagnetization process of ferromagnetic semiconductors. United States: N. p., 2019.
Web. doi:10.1073/pnas.1907246116.
Chen, Zhanghui, Luo, Jun-Wei, & Wang, Lin-Wang. Revealing angular momentum transfer channels and timescales in the ultrafast demagnetization process of ferromagnetic semiconductors. United States. https://doi.org/10.1073/pnas.1907246116
Chen, Zhanghui, Luo, Jun-Wei, and Wang, Lin-Wang. Mon .
"Revealing angular momentum transfer channels and timescales in the ultrafast demagnetization process of ferromagnetic semiconductors". United States. https://doi.org/10.1073/pnas.1907246116. https://www.osti.gov/servlets/purl/1577616.
@article{osti_1577616,
title = {Revealing angular momentum transfer channels and timescales in the ultrafast demagnetization process of ferromagnetic semiconductors},
author = {Chen, Zhanghui and Luo, Jun-Wei and Wang, Lin-Wang},
abstractNote = {Ultrafast control of magnetic order by light provides a promising realization for spintronic devices beyond Moore’s Law and has stimulated intense research interest in recent years. Yet, despite 2 decades of debates, the key question of how the spin angular momentum flows on the femtosecond timescale remains open. The lack of direct first-principle methods and pictures for such process exacerbates the issue. Here, we unravel the laser-induced demagnetization mechanism of ferromagnetic semiconductor GaMnAs, using an efficient time-dependent density functional theory approach that enables the direct real-time snapshot of the demagnetization process. Our results show a clear spin-transfer trajectory from the localized Mn-d electrons to itinerant carriers within 20 fs, illustrating the dominant role of $\textit{sp–d}$ interaction. We find that the total spin of localized electrons and itinerant carriers is not conserved in the presence of spin-orbit coupling (SOC). Immediately after laser excitation, a growing percentage of spin-angular momentum is quickly transferred to the electron orbital via SOC in about 1 ps, then slowly to the lattice via electron–phonon coupling in a few picoseconds, responsible for the 2-stage process observed experimentally. The spin-relaxation time via SOC is about 300 fs for itinerant carriers and about 700 fs for Mn-d electrons. These results provide a quantum-mechanical microscopic picture for the long-standing questions regarding the channels and timescales of spin transfer, as well as the roles of different interactions underlying the GaMnAs demagnetization process.},
doi = {10.1073/pnas.1907246116},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 39,
volume = 116,
place = {United States},
year = {Mon Sep 09 00:00:00 EDT 2019},
month = {Mon Sep 09 00:00:00 EDT 2019}
}
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