Correlation between Spin and Orbital Dynamics during Laser-Induced Femtosecond Demagnetization

Zhang, G. P.; Gu, Mingqiang; Bai, Y. H.; Jenkins, T. L.; George, Thomas F.

doi:10.1021/acs.jpcc.1c03409

Correlation between Spin and Orbital Dynamics during Laser-Induced Femtosecond Demagnetization

Journal Article · Thu Jun 24 00:00:00 EDT 2021 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.1c03409· OSTI ID:1830717

^[1]; Gu, Mingqiang ^[2]; Bai, Y. H. ^[3]; Jenkins, T. L. ^[3]; ^[4]

Indiana State Univ., Terre Haute, IN (United States); Indiana State University
Southern Univ. of Science and Technology, Shenzhen (China)
Indiana State Univ., Terre Haute, IN (United States)
Univ. of Missouri, St. Louis, MO (United States)

Spin and orbital angular momenta are two intrinsic properties of an electron and are responsible for the physics of a solid. How the spin and orbital evolve with respect to each other on several hundred femtoseconds is largely unknown, but it is at the center of laser-induced ultrafast demagnetization. In this paper, we introduce a concept of the spin–orbital correlation diagram, where spin angular momentum is plotted against orbital angular momentum, much like the position-velocity phase diagram in classical mechanics. We use four sets of highly accurate time-resolved X-ray magnetic circular dichroism data to construct four correlation diagrams for iron and cobalt. To our surprise, a pattern emerges. The trace on the correlation diagram for iron is an arc, and at the end of demagnetization, it has a pronounced cusp. The correlation diagram for cobalt is different and appears more linear but with kinks. We carry out first-principles calculations with two different methods: time-dependent density functional theory (TDDFT) and time-dependent Liouville density functional theory. These two methods agree that the experimental findings for both Fe and Co are not due to experimental errors. It is the spin–orbit coupling that correlates the spin dynamics to the orbital dynamics. Microscopically, Fe and Co have different orbital occupations, which leads to distinctive correlation diagrams. We believe that this correlation diagram presents a useful tool to better understand spin and orbital dynamics on an ultrafast time scale. A brief discussion on the magnetic anisotropy energy is also provided.

View Accepted Manuscript (DOE)

Research Organization:: Indiana State Univ., Terre Haute, IN (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC02-05CH11231; FG02-06ER46304

OSTI ID:: 1830717

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 26 Vol. 125; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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