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Spin Berry points as crucial for ultrafast demagnetization

Laser-induced ultrafast demagnetization has puzzled researchers around the world for over two decades. Intrinsic complexity in electronic, magnetic and phononic subsystems is difficult to understand microscopically. So far, it is not possible to explain demagnetization using a single mechanism, which suggests a crucial piece of information still missing. In this paper, we return to a fundamental aspect of physics: spin and its change within each band in the entire Brillouin zone. We employ face-centered cubic (fcc) Ni as an example and use an extremely dense k mesh to map out spin changes for every band close to the Fermi level along all the high symmetry lines. To our surprise, spin angular momentum at some special k points abruptly changes from [Formula: see text] to [Formula: see text] simply by moving from one crystal momentum point to the next. This explains why intraband transitions, which the spin superdiffusion model is based upon, can induce a sharp spin moment reduction, and why electric current can change spin orientation in spintronics. These special k points, which are called spin Berry points [M. V. Berry, Proc. R. Soc. Lond. A 393 (1984) 45], are not random and appear when several bands are close to each other, so the Berry potential of spin majority states is different from that of spin minority states. Although within a single band, spin Berry points jump, when we group several neighboring bands together, they form distinctive smooth spin Berry lines. It is the band structure that disrupts those lines. Spin Berry points are crucial to laser-induced ultrafast demagnetization and spintronics.

Physics↗

Laser-induced forces on atoms during ultrafast demagnetization

Laser-induced femtosecond demagnetization has attracted a broad attention as a possible candidate for information storage technology. However, whether or not lattice vibration directly participates in demagnetization has been highly controversial over a decade. A recent electron diffraction experiment attributed the demagnetization to the polarized phonon effect, but a similar x-ray diffraction experiment attributed it to the Einstein–de Haas effect. Common to both experiments is that neither the angular momentum of the lattice nor the rotation of the sample was directly probed. Here, we report our first first-principles calculation of forces on atoms induced by an ultrafast laser during ultrafast demagnetization. We employ two complementary methods: (i) the frozen lattice with electronic excitation and (ii) frozen excitation but moving the lattice. We find that the forces on atoms start at –50 fs and peak around 30 fs. The magnitude of the force is far smaller than the empirical estimates. Within the limit of our theory, our results suggest that the polarized phonon effect and the Einstein–de Haas effect are unlikely to be the main course of demagnetization. As a result, we expect that our finding has a profound impact on the future direction of laser-induced dynamics in magnetic and quantum materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

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

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.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Laser-Induced Ultrafast Demagnetization and Spin Switching (Final Report)

The information technology revolution demands bigger and faster magnetic storage devices. The funded research focuses on a new frontier - Laser-induced ultrafast all-optical spin switching (AOS), where a single laser pulse can switch spins from one direction to another permanently, without a magnetic field, on a time scale of 1-10 picoseconds, 2-3 orders of magnitude faster than the existing technology. The funded research has successfully resolved a long-standing issue in ultrafast demagnetization whether the lattice contributes to the demagnetization. We developed a high level first-principles theory and employed a massively parallel computer to pin down the details of the physical mechanisms that are inaccessible to other methods. This unique feature allows us to compute the force on each atom in both bulk and monolayer systems. We find that it is indeed true there is a nonzero force on each atom, but the idea of vibration contribution is not crucial to our basic understanding of physics. This paves the way to future experimental, theoretical and technological developments.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Femtosecond photocurrents at the FeRh/Pt interface

Femtosecond laser excitations of FeRh/Pt bilayers launch an ultrafast pulse of electric photocurrents in the Pt-layer and subsequently result in the emission of electromagnetic radiation in the THz spectral range. Analysis of the THz emission as a function of the polarization of the femtosecond laser pulse, external magnetic field, sample temperature, and sample orientation shows that the photocurrent can emerge due to vertical spin pumping and photo-induced inverse spin–orbit torque at the FeRh/Pt interface. Additionally, the vertical spin pumping from FeRh into Pt does not depend on the polarization of light and originates from ultrafast laser-induced demagnetization of the ferromagnetic phase of FeRh. The photo-induced inverse spin–orbit torque at the FeRh/Pt interface can be described in terms of a helicity-dependent effect of circularly polarized light on the magnetization of the ferromagnetic FeRh and the subsequent generation of a photocurrent.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Nonthermal breaking of magnetic order via photogenerated spin defects in the spin-orbit coupled insulator Sr 3 Ir 2 O 7

In many strongly correlated insulators, antiferromagnetic order competes with exotic and technologically relevant phases, like superconductivity. While control of spin order is critical to stabilize different functional states, elucidating the mechanism of laser-induced demagnetization in complex oxides remains a challenge. It is unknown if the optical pulse can quench magnetization nonthermally or if it instead only acts as a heat source. In this study, we used ultrafast, broadband, optical spectroscopy to track the responses of the electronic, lattice, and spin degrees of freedom and their relation to antiferromagnetism in the strongly spin-orbit coupled insulator Sr 3 Ir 2 O 7 . We find that magnetization can be rapidly and strongly suppressed on a sub-150 fs timescale. At low excitation fluences, the magnetic recovery is fast; however, the recovery time increases dramatically with the magnitude of demagnetization. At the same time, we show that the lattice, evidenced through the A g phonon frequencies, appears to remain below T N , suggesting that the system remains nonthermal during the optical modulation of spin order. We suggest that photogenerated spin defects are responsible for the long-lived demagnetized state and discuss its implications for optical control of solids.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Cavity-assisted magnetization switching in a quantum spin-phonon chain

Néel order switching in antiferromagnets has typically required intense optical driving, leading to substantial heating and limited efficiency. By placing antiferromagnets inside a terahertz-driven optical cavity, we propose a multi-particle mechanism for Néel order switching that benefits from reduced heating. Our analysis reveals that phonons are indispensable to this mechanism. A driven cavity mode couples to a spin-phonon chain, with all excitations dissipating energy through external baths. Mean-field analysis shows that cavity photons induce sublattice spin-density imbalance—an intrinsic symmetry-breaking effect absent without the cavity. Contrary to known (1–10 V/nm) laser fields required to switch the Néel order, our mechanism enables switching at remarkably low laser fields (1–5 V/μm), selectively targeting low-energy and perpendicular magnon modes. By virtue of the suppressed heating, the switching remains highly tunable through laser fluence, damping, and photon loss, establishing a low-dissipation route toward cavity-assisted opto-spintronics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Ultrafast perturbation of magnetic domains by optical pumping in a ferromagnetic multilayer

Ultrafast optical pumping of spatially nonuniform magnetic textures is known to induce far-from-equilibrium spin transport effects. Here, we use ultrafast x-ray diffraction with unprecedented dynamic range to study the laser-induced dynamics of labyrinth domain networks in ferromagnetic CoFe/Ni multilayers. We detected azimuthally isotropic, odd order, magnetic diffraction rings up to fifth order. The amplitudes of all three diffraction rings quench to different degrees within 1.6 ps. In addition, all three of the detected diffraction rings both broaden by 15% and radially contract by 6% during the quench process. We are able to rigorously quantify a 31% ultrafast broadening of the domain walls via Fourier analysis of the order-dependent quenching of the three detected diffraction rings. Here, the broadening of the diffraction rings is interpreted as a reduction in the domain coherence length, but the shift in the ring radius, while unambiguous in its occurrence, remains unexplained. In particular, we demonstrate that a radial shift explained by domain-wall broadening can be ruled out. With the unprecedented dynamic range of our data, our results provide convincing evidence that labyrinth domain structures are spatially perturbed at ultrafast speeds under far-from-equilibrium conditions, albeit the mechanism inducing the perturbations remains yet to be clarified.

36 MATERIALS SCIENCE↗