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Register a new userManipulating magnetism by ultrafast control of the exchange interaction
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Johan. H. Mentink
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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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The strongest interaction between microscopic spins in magnetic materials is the exchange interaction $J_text{ex}$. Therefore, ultrafast control of $J_text{ex}$ 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 $J_text{ex}$ on ultrafast timescales in extended antiferromagnetic Mott insulators. In the regime of weak driving strength, we find that $J_text{ex}$ can be enhanced and reduced for frequencies below and above the Mott gap, respectively. Moreover, for strong driving strength, even the sign of $J_text{ex}$ 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.
We investigate how fast and how effective photocarrier excitation can modify the exchange interaction $J_mathrm{ex}$ in the prototype Mott-Hubbard insulator. We demonstrate an ultrafast quenching of $J_mathrm{ex}$ 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 $J_mathrm{ex}$ emerges already within a few electron hopping times after the pulse, with a reduction that is comparable to the effect of chemical doping.
We report a detailed study of the magnetization modulus as a function of temperature and applied magnetic field under varying angle in Sr$_{4}$Ru$_{3}$O$_{10}$ close to the metamagnetic transition at $H_{c}backsimeq 2.5,$T for $H perp c$. We confirm that the double-feature at $H_{c}$ is robust without further splitting for temperatures below 1.8 K down to 0.48 K. The metamagnetism in Sr$_{4}$Ru$_{3}$O$_{10}$ is accompanied by a reduction of the magnetic moment in the plane of rotation and large field-hysteretic behavior. The double anomaly shifts to higher fields by rotating the field from $H,perp ,c$ to $H,parallel,c$. We compare our experimental findings with numerical simulations based on spin reorientation models caused by intrinsic magnetocrystalline anisotropy and Zeeman effect. Crystal anisotropy is able to explain a metamagnetic transition in the ferromagnetic ordered system Sr$_{4}$Ru$_{3}$O$_{10}$, but a Dzyaloshinskii-Moriya term is crucial to account for a reduction of the magnetic moment as discovered in the experiments.
Directly modifying spin exchange energies in a magnetic material with light can enable ultrafast control of its magnetic states. Current approaches rely on tuning charge hopping amplitudes that mediate exchange by optically exciting either virtual or real charge-transfer transitions (CT) between magnetic sites. Here we show that when exchange is mediated by a non-magnetic ligand, it can be substantially enhanced by optically exciting a real CT transition from the ligand to magnetic site, introducing lower order virtual hopping contributions. We demonstrate sub-picosecond enhancement in a superexchange dominated ferromagnet CrSiTe3 through this mechanism using phase-resolved coherent phonon spectroscopy. This technique can also be applied in the paramagnetic phase to disentangle light induced exchange modification from other ultrafast effects that alter the magnetization. This protocol can potentially be broadly applied to engineer thermally inaccessible spin Hamiltonians in superexchange dominated magnets.
Femtosecond time-resolved x-ray diffraction is employed to study the dynamics of the periodic lattice distortion (PLD) associated with the charge-density-wave (CDW) in K0.3MoO3. Using a multi-pulse scheme we show the ability to extend the lifetime of coherent oscillations of the PLD about the undistorted structure through re-excitation of the electronic states. This suggests that it is possible to enter a regime where the symmetry of the potential energy landscape corresponds to the high symmetry phase but the scattering pathways that lead to the damping of coherent dynamics are still controllable by altering the electronic state population. The demonstrated control over the coherence time offers new routes for manipulation of coherent lattice states.
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