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 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.
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (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)
- OSTI Identifier:
- 1577616
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Journal Article: 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
None, None. 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.
None, None. Revealing angular momentum transfer channels and timescales in the ultrafast demagnetization process of ferromagnetic semiconductors. United States. https://doi.org/10.1073/pnas.1907246116
None, None. 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 = {None, None},
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 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},
url = {https://www.osti.gov/biblio/1577616},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
issn = {0027-8424},
number = 39,
volume = 116,
place = {United States},
year = {2019},
month = {9}
}
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