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arXiv:1905.03921 · Physical review. B./Physical review. B

Orbital Floquet engineering of exchange interactions in magnetic materials

Swati Chaudhary, David Hsieh, Gil Refael

Published Dec 9, 2019• 34 citations
arXivHTMLPDF

Abstract

We present a scheme to control the spin-exchange interactions by manipulating the orbital degrees of freedom using a periodic drive. We discuss two different protocols for orbital Floquet engineering. In one case, a periodic drive modifies the properties of the ligand orbitals which mediate magnetic interactions between transition-metal ions. In the other case, we consider drive-induced mixing of $d$ orbitals on each magnetic ion. We first find that an AC Stark shift of orbitals induces a change comparable to that induced from photoinduced hopping schemes, but expands the applicable frequency ranges. Next, we find that radiatively induced coherent vibrations provide a realistic path for Floquet orbital engineering with short pulses of electric fields weaker than 0.5 V/\AA{} producing $5%--10%$ changes in the magnetic coupling of Mott insulators such as the rare-earth titanates.

DOI
10.1103/physrevb.100.220403

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We present a scheme to control the spin-exchange interactions by manipulating the orbital degrees of freedom using a periodic drive. We discuss two different protocols for orbital Floquet engineering. In one case, a periodic drive modifies the properties of the ligand orbitals which mediate magnetic interactions between transition-metal ions. In the other case, we consider drive-induced mixing of ddd orbitals on each magnetic ion. We first find that an AC Stark shift of orbitals induces a change comparable to that induced from photoinduced hopping schemes, but expands the applicable frequency ranges. Next, we find that radiatively induced coherent vibrations provide a realistic path for Floquet orbital engineering with short pulses of electric fields weaker than 0.5 V/\AA{} producing 55%--10%5 changes in the magnetic coupling of Mott insulators such as the rare-earth titanates.
We consider driving multiorbital Mott insulators using laser radiation. We derive general expressions for periodically driven spin-orbital models using time-dependent perturbation theory in the strong interaction limit. We show that the effective exchange interactions of the Floquet spin-orbital Hamiltonian are highly tunable via variations of the frequency, amplitude, and polarization of the laser. We also take the effect of a finite bandwidth of excitations into account and study possible heating effects. We further apply our formalism to orthorhombic titanates YTiO_{3} and LaTiO_{3} based on first-principles calculations, and we find that the spin exchange interactions in these compounds can be engineered to a large extent by tuning the frequency and electric-field amplitude of the laser.
Intense light can alter the electronic properties of materials through its oscillating electric field. The effects on magnetic excitations in insulators, however, are indirect, since these are neutral and do not see the electric field directly. This study reports on how exchange interactions in single- and multiorbital Mott insulators are modified by electromagnetic radiation, whose frequency is assumed to be on the order of the Mott-Hubbard gap. The latter condition results in a nonvanishing creation rate of doubly occupied sites (doublons), which necessitates taking into account the finite bandwidth of the doublon excitations, a feature which goes beyond the na\"{\i}ve leading order strong correlation expansion. This ultimately leads to a complex-valued exchange parameter, where the real part represents the ``Floquet'' spin-exchange interaction, while the imaginary part reflects the creation rate of doublons.
Coherent control of interacting spin systems under time-periodic driving is a central challenge in spin-based quantum technologies. Here we demonstrate the applicability of a full Floquet-space formalism, adapted from Nuclear Magnetic Resonance (NMR) methodologies, to model the dynamics of driven coupled electron spins in the presence of a static magnetic field B0 and a transverse oscillating field B1. The framework explicitly includes isotropic exchange coupling J and the chiral Dzyaloshinskii-Moriya antisymmetric exchange interaction (DMI), and its numerical convergence is systematically validated with respect to Fourier-space truncation. In the non-interacting limit, the expected driven-spin dynamics is recovered, with the oscillation periodicity governed by B1. Exchange coupling alone does not modify the collective spin expectation values under the chosen initial condition, consistent with symmetry considerations. In contrast, increasing DMI generates a finite Sy component, suppresses Sz, and produces tilted, elliptical Bloch-sphere trajectories, reflecting the emergence of chiral spin-spin correlations. These effects are pronounced for open boundary conditions, while remaining nearly negligible in the periodic boundary case. When exchange coupling and DMI coexist, the dynamics becomes strongly perturbed and multi-frequency in nature. Together, these results demonstrate that full Floquet-space modeling provides a robust and predictive framework for analyzing and engineering coherent dynamics in driven interacting spin systems beyond simple coherent-rotation regimes.
Non-equilibrium control of electronic properties in condensed matter systems can result in novel phenomena. In this work, we provide a novel non-equilibrium route to realize half-metallic phases. We explore the periodically driven Hubbard model on a bipartite lattice and demonstrate that a specially designed sublattice dependent drive can transform a weakly interacting metal or insulator into a ferrimagnetic half-metal (HM). We consider a Fermi-Hubbard model with only nearest-neighbour hopping and Floquet engineer the elusive half-metal phase by driving the site potentials periodically. The drive induces staggered higher range hoppings and a staggered potential between two sublattices in the Floquet Hamiltonian. Close to the dynamical localization point, due to the suppression of nearest neighbor hopping in the driven system, an effective enhancement of various terms in the Floquet Hamiltonian, including the e-e interactions, occurs. This helps in stabilizing a broad ferrimagnetic HM phase for a wide range of drive parameters. This dynamically stabilized HM phase is a pristine platform for next-generation spintronics, topological quantum computing (specifically for engineering Majorana zero modes in hybrid nanowires) and ultrafast magnetic memory architectures.
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}} J ex that is analogous to the single-orbital case. Moreover we demonstrate that also the additional biquadratic exchange interaction B_{\textrm{ex}} B 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.
Floquet engineering is a powerful tool that drives materials with periodic light. Traditionally, the light is monochromatic, with amplitude, frequency, and polarization varied. We introduce Floquet engineering via unpolarized light built from quasimonochromatic light and show how it can modify strongly correlated systems, while preserving the original symmetries. Different types of unpolarized light can realize different strongly correlated phases As an example, we treat insulating magnetic materials on a triangular lattice and show how unpolarized light can induce a Dirac spin liquid.