We employ real-time time-dependent density functional theory (rt-TDDFT) and ab initio nonadiabatic molecular dynamics (NAMD) to systematically investigate the ultrafast laser pulses induced spin transfer and relaxation dynamics of two-dimensional (2D) antiferromagnetic-ferromagnetic (AFM/FM) MnPS3/MnSe2 van der Waals heterostructures. We demonstrate that laser pulses can induce a ferrimagnetic (FiM) state in the AFM MnPS3 layer within tens of femtoseconds and maintain it for subpicosecond time scale before reverting to the AFM state. We identify the mechanism in which the asymmetric optical intersite spin transfer (OISTR) effect occurring within the sublattices of the AFM and FM layers drives the interlayer spin-selective charge transfer, leading to the transition from AFM to FiM state. Furthermore, the unequal electron-phonon coupling of spin-up and spin-down channels of AFM spin sublattice causes an inequivalent spin relaxation, in turn extending the time scale of the FiM state. These findings are essential for designing novel optical-driven ultrafast 2D magnetic switches.

• Klíčová slova
• 2D magnetism, antiferromagnetism, nonadiabatic MD, real-time TDDFT, spin dynamics, spin relaxation,
• Publikační typ
• časopisecké články MeSH

Spin injection stands out as a crucial method employed for initializing, manipulating, and measuring the spin states of electrons, which are fundamental to the creation of qubits in quantum computing. However, ensuring efficient spin injection while maintaining compatibility with standard semiconductor processing techniques is a significant challenge. Herein, we demonstrate the capability of inducing an ultrafast spin injection into a WSe2 layer from a magnetic CrI3 layer on a femtosecond time scale, achieved through real-time time-dependent density functional theory calculations upon a laser pulse. Following the peak of the magnetic moment in the CrI3 sublayer, the magnetic moment of the WSe2 layer reaches a maximum of 0.89 μB (per unit cell containing 4 WSe2 and 1 CrI3 units). During the spin dynamics, spin-polarized excited electrons transfer from the WSe2 layer to the CrI3 layer via type-II band alignment. The large spin splitting in conduction bands and the difference in the number of spin-polarized local unoccupied states available in the CrI3 layer lead to a net spin in the WSe2 layer. Furthermore, we confirmed that the number of available states, the spin-flip process, and the laser pulse parameters play important roles during the spin injection process. This work highlights the dynamic and rapid nature of spin manipulation in layered all-semiconductor systems, offering significant implications for the development and enhancement of quantum information processing technologies.

• Klíčová slova
• all-semiconductor magnetic heterobilayer, laser-driven spin dynamics, out-of-equilibrium spin populations, real-time density functional theory, spin injection,
• Publikační typ
• časopisecké články MeSH

Invar-behavior occurring in many magnetic materials has long been of interest to materials science. Here, we show not only invar behavior of a continuous film of FePt but also even negative thermal expansion of FePt nanograins upon equilibrium heating. Yet, both samples exhibit pronounced transient expansion upon laser heating in femtosecond x-ray diffraction experiments. We show that the granular microstructure is essential to support the contractive out-of-plane stresses originating from in-plane expansion via the Poisson effect that add to the uniaxial contractive stress driven by spin disorder. We prove the spin contribution by saturating the magnetic excitations with a first laser pulse and then detecting the purely expansive response to a second pulse. The contractive spin stress is reestablished on the same 100-ps time scale that we observe for the recovery of the ferromagnetic order. Finite-element modeling of the mechanical response of FePt nanosystems confirms the morphology dependence of the dynamics.

• Publikační typ
• časopisecké články MeSH

Ultrafast demagnetization of rare-earth metals is distinct from that of 3d ferromagnets, as rare-earth magnetism is dominated by localized 4f electrons that cannot be directly excited by an optical laser pulse. Their demagnetization must involve excitation of magnons, driven either through exchange coupling between the 5d6s-itinerant and 4f-localized electrons or by coupling of 4f spins to lattice excitations. Here, we disentangle the ultrafast dynamics of 5d6s and 4f magnetic moments in terbium metal by time-resolved photoemission spectroscopy. We show that the demagnetization time of the Tb 4f magnetic moments of 400 fs is set by 4f spin-lattice coupling. This is experimentally evidenced by a comparison to ferromagnetic gadolinium and supported by orbital-resolved spin dynamics simulations. Our findings establish coupling of the 4f spins to the lattice via the orbital momentum as an essential mechanism driving magnetization dynamics via ultrafast magnon generation in technically relevant materials with strong magnetic anisotropy.

• Publikační typ
• časopisecké články MeSH