Ultrafast Quenching of the Exchange Interaction in a Mott Insulator

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.Comment: 8 pages, 4 figure

Second Low Temperature Phase Transition in Frustrated UNi_4B

Hexagonal UNi_4B is magnetically frustrated, yet it orders antiferromagnetically at T_N = 20 K. However, one third of the U-spins remain paramagnetic below this temperature. In order to track these spins to lower temperature, we measured the specific heat C of \unib between 100 mK and 2 K, and in applied fields up to 9 T. For zero field there is a sharp kink in C at $T^\ast\approx$ 330 mK, which we interpret as an indication of a second phase transition involving paramagnetic U. The rise in $\gamma = C/T$ between 7 K and 330 mK and the absence of a large entropy liberated at $T^\ast$ may be due to a combination of Kondo screening effects and frustration that strongly modifies the low T transition.Comment: 4 pages, 4 figure

Kondo Screening and Magnetic Ordering in Frustrated UNi4B

UNi4B exhibits unusual properties and, in particular, a unique antiferromagnetic arrangement involving only 2/3 of the U sites. Based on the low temperature behavior of this compound, we propose that the remaining 1/3 U sites are nonmagnetic due to the Kondo effect. We derive a model in which the coexistence of magnetic and nonmagnetic U sites is the consequence of the competition between frustration of the crystallographic structure and instability of the 5f moments.Comment: 4 pages, 2 figure

Ultrafast and reversible control of the exchange interaction in Mott insulators

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.Comment: 9 pages, 4 figure

Optical control of competing exchange interactions and coherent spin-charge coupling in two-orbital Mott insulators

In order to have a better understanding of ultrafast electrical control of exchange interactions in multi-orbital systems, we study a two-orbital Hubbard model at half filling under the action of a time-periodic electric field. Using suitable projection operators and a generalized time-dependent canonical transformation, we derive an effective Hamiltonian which describes two different regimes. First, for a wide range of non-resonant frequencies, we find a change of the bilinear Heisenberg exchange $J_{\textrm{ex}}$ that is analogous to the single-orbital case. Moreover we demonstrate that also the additional biquadratic exchange interaction $B_{\textrm{ex}}$ can be enhanced, reduced and even change sign depending on the electric field. Second, for special driving frequencies, we demonstrate a novel spin-charge coupling phenomenon enabling coherent transfer between spin and charge degrees of freedom of doubly ionized states. These results are confirmed by an exact time-evolution of the full two-orbital Mott-Hubbard Hamiltonian.Comment: 3 pages, 6 figure

Stable and fast semi-implicit integration of the stochastic Landau-Lifshitz equation

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.Comment: 24 pages, 5 figure

Quantum many-body dynamics of the Einstein-de Haas effect

In 1915, Einstein and de Haas and Barnett demonstrated that changing the magnetization of a magnetic material results in mechanical rotation, and vice versa. At the microscopic level, this effect governs the transfer between electron spin and orbital angular momentum, and lattice degrees of freedom, understanding which is key for molecular magnets, nano-magneto-mechanics, spintronics, and ultrafast magnetism. Until now, the timescales of electron-to-lattice angular momentum transfer remain unclear, since modeling this process on a microscopic level requires addition of an infinite amount of quantum angular momenta. We show that this problem can be solved by reformulating it in terms of the recently discovered angulon quasiparticles, which results in a rotationally invariant quantum many-body theory. In particular, we demonstrate that non-perturbative effects take place even if the electron--phonon coupling is weak and give rise to angular momentum transfer on femtosecond timescales.Comment: 15 pages, 5 figure

Selection rules for ultrafast laser excitation and detection of spin correlations dynamics in a cubic antiferromagnet

Exchange interactions determine the correlations between microscopic spins in magnetic materials. Probing the dynamics of these spin correlations on ultrashort length and time scales is, however rather challenging, since it requires simultaneously high spatial and high temporal resolution. Recent experimental demonstrations of laser-driven two-magnon modes - zone-edge excitations in antiferromagnets governed by exchange coupling - posed questions about the microscopic nature of the observed spin dynamics, the mechanism underlying its excitation, and their macroscopic manifestation enabling detection. Here, on the basis of a simple microscopic model, we derive the selection rules for cubic systems that describe the polarization of pump and probe pulses required to excite and detect dynamics of nearest-neighbor spin correlations, and can be employed to isolate such dynamics from other magnetic excitations and magneto-optical effects. We show that laser-driven spin correlations contribute to optical anisotropy of the antiferromagnet even in the absence of spin-orbit coupling. In addition, we highlight the role of subleading anisotropy in the spin system and demonstrate that the dynamics of the antiferromagnetic order parameter occurs only in next-to-leading order, determined by the smallness of the magnetic anisotropy as compared to the isotropic exchange interactions in the system. We expect that our results will stimulate and support further studies of magnetic correlations on the shortest length and time scale.Comment: 17 pages, 5 figure

Role of stochastic noise and generalization error in the time propagation of neural-network quantum states

Neural-network quantum states (NQS) have been shown to be a suitable variational ansatz to simulate out-of-equilibrium dynamics in two-dimensional systems using time-dependent variational Monte Carlo (t-VMC). In particular, stable and accurate time propagation over long time scales has been observed in the square-lattice Heisenberg model using the Restricted Boltzmann machine architecture. However, achieving similar performance in other systems has proven to be more challenging. In this article, we focus on the two-leg Heisenberg ladder driven out of equilibrium by a pulsed excitation as a benchmark system. We demonstrate that unmitigated noise is strongly amplified by the nonlinear equations of motion for the network parameters, which causes numerical instabilities in the time evolution. As a consequence, the achievable accuracy of the simulated dynamics is a result of the interplay between network expressiveness and measures required to remedy these instabilities. We show that stability can be greatly improved by appropriate choice of regularization. This is particularly useful as tuning of the regularization typically imposes no additional computational cost. Inspired by machine learning practice, we propose a validation-set based diagnostic tool to help determining optimal regularization hyperparameters for t-VMC based propagation schemes. For our benchmark, we show that stable and accurate time propagation can be achieved in regimes of sufficiently regularized variational dynamics