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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.
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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.
Femtosecond time-resolved core-level photoemission spectroscopy with a free-electron laser is used to measure the atomic-site specific charge-order dynamics in the charge-density-wave/Mott insulator 1T-TaS2. After strong photoexcitation, a prompt loss of charge order and subsequent fast equilibration dynamics of the electron-lattice system are observed. On the time scale of electron-phonon thermalization, about 1 ps, the system is driven across a phase transition from a long-range charge ordered state to a quasi-equilibrium state with domain-like short-range charge and lattice order. The experiment opens the way to study the nonequilibrium dynamics of condensed matter systems with full elemental, chemical, and atomic site selectivity.
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.
We report strong instantaneous photoinduced absorption (PA) in the quasi-one-dimensional Mott insulator ${rm Sr_2CuO_3}$ in the IR spectral region. The observed PA is to an even-parity two-photon state that occurs immediately above the absorption edge. Theoretical calculations based on a two-band extended Hubbard model explains the experimental features and indicates that the strong two-photon absorption is due to a very large dipole-coupling between nearly degenerate one- and two-photon states. Room temperature picosecond recovery of the optical transparency suggests the strong potential of ${rm Sr_2CuO_3}$ for all-optical switching.
We have observed the characteristic temperature dependence of the intermolecular phonon spectrum in the organic dimer Mott insulator kappa-(ET)2Cu2(CN)3 exhibiting a dielectric anomaly at 30 K. The anomalous spectral narrowing of the 55 cm-1 phonon peak at 30 K was analyzed in terms of motional narrowing within the framework of a stationary Gaussian process, i. e., the phonon frequency is modulated by the ultrafast charge fluctuation. The spectral narrowing occurs because the time constant of the correlation time tau_c and the amplitude of the frequency modulation delta satisfy the relation tau_c<delta at 30 K. At temperatures below 30 K, the motional narrowing is disturbed by the increasing of tau_c, near the charge-glass or the short-range order at 6 K. On the other hand, for temperatures above 30 K, the motional narrowing is disturbed by the increase of delta with increasing temperature.
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