Investigation of Light-induced Ultrafast Magnetization Dynamics Using Ab Initio Methods
| Author | : Philippe Scheid |
| Publisher | : |
| Total Pages | : 0 |
| Release | : 2020 |
| Genre | : |
| ISBN | : |
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This thesis begins with a review of the current experimental and theoretical state of the art related to the light-induced ultrafast demagnetization and the all-optical helicity-dependent switching. This is followed by an overview of density functional theory, upon which relies most of the work reported thereafter. The first set of results concerns the ab initio study of the effect of a rise in the electronic temperature on the magnetized matter properties, and more specifically Fe, Co, Ni and FePt. We show that the magnetic moment carried by each atom disappears at the so-called Stoner temperature, and that this phenomenon impacts the electronic energy and specific heat, even at low electronic temperature. Then, we show that upon an increase in the electronic temperature, the interatomic Heisenberg exchange, which is responsible for the magnetic ordering, decreases. Using the atomistic Langevin Landau-Lifshitz-Gilbert equation, we demonstrate that this decrease is enough to induce a large reduction of the average magnetization by creating transversal excitations. The second set of results regards the origin of the helicity-dependent light-induced dynamics. While the literature attributes it mainly to the inverse Faraday effect, we argue that another and novel phenomenon, which occurs during the absorption of the light, may be more suited to account for the experimental dynamics. Indeed, using the Fermi golden rule and ground state density functional theory calculations in Fe, Co, Ni and FePt, we show that, as the light is absorbed and electrons are excited, concurrently to the increase of the electronic energy, the spin-state is also changed in presence of spin-orbit coupling. This results in a difference in the value of the atomic magnetic moments, persisting even after the light is gone, as opposed to the inverse Faraday effect. Then, using real-time time-dependent density functional theory, we compute the magnetization dynamics induced by real optical and XUV femtosecond circularly polarized pulses. We show that, in both cases the dynamics is helicity-dependent and that this characteristic is largely amplified in the XUV regime involving the semi-core 3p states. Finally, we compare the relative role of the inverse Faraday effect and the magnetization induced during the absorption of the light and show that the latter plays a prominent role, especially after the light has gone, and in the XUV regime.
