Optically controlling the competition between spin flips and intersite spin transfer in a Heusler half-metal on sub-100 fs timescales

The direct manipulation of spins via light may provide a path toward ultrafast energy-efficient devices. However, distinguishing the microscopic processes that can occur during ultrafast laser excitation in magnetic alloys is challenging. Here, we study the Heusler compound Co2MnGa, a material that exhibits very strong light-induced spin transfers across the entire M-edge. By combining the element-specificity of extreme ultraviolet high harmonic probes with time-dependent density functional theory, we disentangle the competition between three ultrafast light-induced processes that occur in Co2MnGa: same-site Co-Co spin transfer, intersite Co-Mn spin transfer, and ultrafast spin-flips mediated by spin-orbit coupling. By measuring the dynamic magnetic asymmetry across the entire M-edges of the two magnetic sublattices involved, we uncover the relative dominance of these processes at different probe energy regions and times during the laser pulse. Our combined approach enables a comprehensive microscopic interpretation of laser-induced magnetization dynamics on timescales shorter than 100 fs.Comment: 31 pages, 12 figure

Element-selective ultrafast magnetization dynamics of hybrid Stoner-Heisenberg magnets

Stoner and Heisenberg excitations in magnetic materials are inherently different. The first involves an effective reduction of the exchange splitting, whereas the second comprises excitation of spin waves. In this work, we test the impact of these two excitations in the hybrid Stoner-Heisenberg system of FePd. We present a microscopic picture of ultrafast demagnetization dynamics in this alloy, which represents both components of strong local exchange splitting in Fe and induced polarization in Pd. We identify the spin-orbit coupling (SOC) and the optical intersite spin transfer (OISTR) as the two dominant factors for demagnetization at ultrashort timescales. Remarkably, the drastic difference in the origin of the magnetic moment of the Fe and Pd species is not deciding the initial magnetization dynamics in this alloy. By tuning the external laser pulse, the extrinsic OISTR can be manipulated for site-selective demagnetization on femtosecond timescales providing the fastest way for optical and selective control of the magnetization dynamics in alloys. Saliently, our results signify why various experiments demonstrating OISTR might obtain conflicting results

Optically controlling the competition between spin flips and intersite spin transfer in a Heusler half-metal on sub-100-fs time scales

The direct manipulation of spins via light may provide a path toward ultrafast energy-efficient devices. However, distinguishing the microscopic processes that can occur during ultrafast laser excitation in magnetic alloys is challenging. Here, we study the Heusler compound Co2MnGa, a material that exhibits very strong light-induced spin transfers across the entire M-edge. By combining the element specificity of extreme ultraviolet high-harmonic probes with time-dependent density functional theory, we disentangle the competition between three ultrafast light-induced processes that occur in Co2MnGa: same-site Co-Co spin transfer, intersite Co-Mn spin transfer, and ultrafast spin flips mediated by spin-orbit coupling. By measuring the dynamic magnetic asymmetry across the entire M-edges of the two magnetic sublattices involved, we uncover the relative dominance of these processes at different probe energy regions and times during the laser pulse. Our combined approach enables a comprehensive microscopic interpretation of laser-induced magnetization dynamics on time scales shorter than 100 femtoseconds

The interplay of local electron correlations and ultrafast spin dynamics in fcc Ni

The complex electronic structure of metallic ferromagnets is determined by a balance between exchange interaction, electron hopping leading to band formation, and local Coulomb repulsion. By combining high energy and temporal resolution in femtosecond time-resolved X-ray absorption spectroscopy with ab initio time-dependent density functional theory we analyze the electronic structure in fcc Ni on the time scale of these interactions in a pump-probe experiment. We distinguish transient broadening and energy shifts in the absorption spectra, which we demonstrate to be captured by electron repopulation respectively correlation-induced modifications of the electronic structure, requiring to take the local Coulomb interaction into account.ISSN:2166-383

The interplay of local electron correlations and ultrafast spin dynamics in fcc Ni

The complex electronic structure of metallic ferromagnets is determined by a balance between exchange interaction, electron hopping leading to band formation, and local Coulomb repulsion. By combining high energy and temporal resolution in femtosecond time-resolved X-ray absorption spectroscopy with ab initio time-dependent density functional theory we analyze the electronic structure in fcc Ni on the time scale of these interactions in a pump-probe experiment. We distinguish transient broadening and energy shifts in the absorption spectra, which we demonstrate to be captured by electron repopulation respectively correlation-induced modifications of the electronic structure, requiring to take the local Coulomb interaction into account