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Understanding how fast short-range interactions build up long-range order is one of the most intriguing topics in condensed matter physics. FeRh is a test specimen for studying this problem in magnetism, where the microscopic spin-spin exchange interaction is ultimately responsible for either ferro- or antiferromagnetic macroscopic order. Femtosecond laser excitation can induce ferromagnetism in antiferromagnetic FeRh, but the mechanism and dynamics of this transition are topics of intense debates. Employing double-pump THz emission spectroscopy has enabled us to dramatically increase the temporal detection window of THz emission probes of transient states without sacrificing any loss of resolution or sensitivity. It allows us to study the kinetics of emergent ferromagnetism from the femtosecond up to the nanosecond timescales in FeRh/Pt bilayers. Our results strongly suggest a latency period between the initial pump-excitation and the emission of THz radiation by ferromagnetic nuclei.
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We investigate the propagation of magnons after ultrashort perturbations of the exchange interaction in the prototype two-dimensional Heisenberg antiferromagnet. Using the recently proposed neural quantum states, we predict highly anisotropic spreading in space constrained by the symmetry of the perturbation. Interestingly, the propagation speed at the shortest length scale and timescale is up to 40% higher than the highest magnon velocity. We argue that the enhancement stems from extraordinary strong magnon-magnon interactions, suggesting new avenues for manipulating information transfer on ultrashort length scales and timescales.
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In recent years, the optical control of exchange interactions has emerged as an exciting new direction in the study of the ultrafast optical control of magnetic order. Here we review recent theoretical works on antiferromagnetic systems, devoted to (i) simulating the ultrafast control of exchange interactions, (ii) modeling the strongly nonequilibrium response of the magnetic order and (iii) the relation with relevant experimental works developed in parallel. In addition to the excitation of spin precession, we discuss examples of rapid cooling and the control of ultrafast coherent longitudinal spin dynamics in response to femtosecond optically induced perturbations of exchange interactions. These elucidate the potential for exploiting the control of exchange interactions to find new scenarios for both faster and more energy-efficient manipulation of magnetism.
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Terahertz magnetic fields with amplitudes of up to 0.4 Tesla drive magnon resonances in nickel oxide while the induced dynamics is recorded by femtosecond magneto-optical probing. We observe distinct spin-mediated optical nonlinearities, including oscillations at the second harmonic of the 1 THz magnon mode. The latter originate from coherent dynamics of the longitudinal component of the antiferromagnetic order parameter, which are probed by magneto-optical effects of second order in the spin deflection. These observations allow us to dynamically disentangle electronic from lattice-related contributions to magnetic linear birefringence and dichroism-information so far only accessible by ultrafast THz spin control. The nonlinearities discussed here foreshadow physics that will become essential in future subcycle spin switching.
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Ultrafast non-thermal manipulation of magnetization by light relies on either indirect coupling of the electric field component of the light with spins via spin-orbit interaction or direct coupling between the magnetic field component and spins. Here we propose a scenario for coupling between the electric field of light and spins via optical modification of the exchange interaction, one of the strongest quantum effects with strength of 10(3) Tesla. We demonstrate that this isotropic opto-magnetic effect, which can be called inverse magneto-refraction, is allowed in a material of any symmetry. Its existence is corroborated by the experimental observation of terahertz emission by spin resonances optically excited in a broad class of iron oxides with a canted spin configuration. From its strength we estimate that a sub-picosecond modification of the exchange interaction by laser pulses with fluence of about 1 mJ cm(-2) acts as a pulsed effective magnetic field of 0.01 Tesla.
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The strongest interaction between microscopic spins in magnetic materials is the exchange interaction Jex. Therefore, ultrafast control of Jex holds the promise to control spins on ultimately fast timescales. We demonstrate that time-periodic modulation of the electronic structure by electric fields can be used to reversibly control Jex on ultrafast timescales in extended antiferromagnetic Mott insulators. In the regime of weak driving strength, we find that Jex can be enhanced and reduced for frequencies below and above the Mott gap, respectively. Moreover, for strong driving strength, even the sign of Jex can be reversed and we show that this causes time reversal of the associated quantum spin dynamics. These results suggest wide applications, not only to control magnetism in condensed matter systems, for example, via the excitation of spin resonances, but also to assess fundamental questions concerning the reversibility of the quantum many-body dynamics in cold atom systems.
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We investigate how fast and how effective photocarrier excitation can modify the exchange interaction J_{ex} in the prototype Mott-Hubbard insulator. We demonstrate an ultrafast quenching of J_{ex} both by evaluating exchange integrals from a time-dependent response formalism and by explicitly simulating laser-induced spin precession in an antiferromagnet that is canted by an external magnetic field. In both cases, the electron dynamics is obtained from nonequilibrium dynamical mean-field theory. We find that the modified J_{ex} emerges already within a few electron hopping times after the pulse, with a reduction that is comparable to the effect of chemical doping.
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Ultrafast laser techniques have revealed extraordinary spin dynamics in magnetic materials that equilibrium descriptions of magnetism cannot explain. Particularly important for future applications is understanding non-equilibrium spin dynamics following laser excitation on the nanoscale, yet the limited spatial resolution of optical laser techniques has impeded such nanoscale studies. Here we present ultrafast diffraction experiments with an X-ray laser that probes the nanoscale spin dynamics following optical laser excitation in the ferrimagnetic alloy GdFeCo, which exhibits macroscopic all-optical switching. Our study reveals that GdFeCo displays nanoscale chemical and magnetic inhomogeneities that affect the spin dynamics. In particular, we observe Gd spin reversal in Gd-rich nanoregions within the first picosecond driven by the non-local transfer of angular momentum from larger adjacent Fe-rich nanoregions. These results suggest that a magnetic material's microstructure can be engineered to control transient laser-excited spins, potentially allowing faster (~ 1 ps) spin reversal than in present technologies.
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We propose a general theoretical framework for ultrafast laser-induced spin dynamics in multisublattice magnets. We distinguish relaxation of relativistic and exchange origin and show that when the former dominates, nonequivalent sublattices have distinct dynamics despite their strong exchange coupling. Even more interesting, in the exchange dominated regime sublattices can show highly counterintuitive transitions between parallel and antiparallel alignment. This allows us to explain recent experiments with antiferromagnetically coupled sublattices, and predict that such transitions are possible with ferromagnetic coupling as well. In addition, we predict that exchange relaxation enhances the demagnetization speed of both sublattices only when they are antiferromagnetically coupled.
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We propose new semi-implicit numerical methods for the integration of the stochastic Landau-Lifshitz equation with built-in angular momentum conservation. The performance of the proposed integrators is tested on the 1D Heisenberg chain. For this system, our schemes show better stability properties and allow us to use considerably larger time steps than standard explicit methods. At the same time, these semi-implicit schemes are also of comparable accuracy to and computationally much cheaper than the standard midpoint implicit method. The results are of key importance for atomistic spin dynamics simulations and the study of spin dynamics beyond the macro spin approximation.