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arXiv:2103.13708 · npj Quantum Materials

High harmonic generation in two-dimensional Mott insulators

Christopher Orthodoxou, A. Zaïr, George H. Booth

Published Sep 9, 2021• 1 citation
arXivHTMLPDF

Abstract

Abstract With a combination of numerical methods, including quantum Monte Carlo, exact diagonalization, and a simplified dynamical mean-field model, we consider the attosecond charge dynamics of electrons induced by strong-field laser pulses in two-dimensional Mott insulators. The necessity to go beyond single-particle approaches in these strongly correlated systems has made the simulation of two-dimensional extended materials challenging, and we contrast their resulting high-harmonic emission with more widely studied one-dimensional analogues. As well as considering the photo-induced breakdown of the Mott insulating state and magnetic order, we also resolve the time and ultra-high-frequency domains of emission, which are used to characterize both the photo-transition, and the sub-cycle structure of the electron dynamics. This extends simulation capabilities and understanding of the photo-melting of these Mott insulators in two dimensions, at the frontier of attosecond non-equilibrium science of correlated materials.

DOI
10.1038/s41535-021-00377-8

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Abstract With a combination of numerical methods, including quantum Monte Carlo, exact diagonalization, and a simplified dynamical mean-field model, we consider the attosecond charge dynamics of electrons induced by strong-field laser pulses in two-dimensional Mott insulators. The necessity to go beyond single-particle approaches in these strongly correlated systems has made the simulation of two-dimensional extended materials challenging, and we contrast their resulting high-harmonic emission with more widely studied one-dimensional analogues. As well as considering the photo-induced breakdown of the Mott insulating state and magnetic order, we also resolve the time and ultra-high-frequency domains of emission, which are used to characterize both the photo-transition, and the sub-cycle structure of the electron dynamics. This extends simulation capabilities and understanding of the photo-melting of these Mott insulators in two dimensions, at the frontier of attosecond non-equilibrium science of correlated materials.
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To study excitonic effects on high-harmonic generation (HHG) in Mott insulators, we investigate pumped nonequilibrium dynamics in the one-dimensional extended Hubbard model. By employing time-dependent calculations based on the exact diagonalization and infinite time-evolving block decimation methods, we find the strong enhancement of the HHG intensity around the exciton energy. The subcycle analysis in the sub-Mott-gap regime shows that the intensity region of the time-resolved spectrum around the exciton energy splits into two levels and oscillates following the driving electric field. This excitonic dynamics is qualitatively different from the dynamics of free doublon and holon but favorably contributes to HHG in the Mott insulator.
We study high-harmonic generation (HHG) in the one-dimensional Hubbard model in order to understand its relation to elementary excitations as well as the similarities and differences to semiconductors. The simulations are based on the infinite time-evolving block decimation (iTEBD) method and exact diagonalization. We clarify that the HHG originates from the doublon-holon recombination, and the scaling of the cutoff frequency is consistent with a linear dependence on the external field. We demonstrate that the subcycle features of the HHG can be reasonably described by a phenomenological three step model for a doublon-holon pair. We argue that the HHG in the one-dimensional Mott insulator is closely related to the dispersion of the doublon-holon pair with respect to its relative momentum, which is not necessarily captured by the single-particle spectrum due to the many-body nature of the elementary excitations. For the comparison to semiconductors, we introduce effective models obtained from the Schrieffer-Wolff transformation, i.e., a strong-coupling expansion, which allows us to disentangle the different processes involved in the Hubbard model: intraband dynamics of doublons and holons, interband dipole excitations, and spin exchanges. These demonstrate the formal similarity of the Mott system to the semiconductor models in the dipole gauge, and reveal that the spin dynamics, which does not directly affect the charge dynamics, can reduce the HHG intensity. We also show that the long-range component of the intraband dipole moment has a substantial effect on the HHG intensity, while the correlated hopping terms for the doublons and holons essentially determine the shape of the HHG spectrum. A new numerical method to evaluate single-particle spectra within the iTEBD method is also introduced.
Solid-state high-harmonic spectroscopy is becoming an emerging tool for probing nonequilibrium many-body dynamics. Yet, direct measurements of strongly driven, sub-optical-cycle dynamics in correlated materials during high-harmonic emission remain largely unexplored. Here, we measure high-harmonic emission chirp in a prototypical one-dimensional Mott insulator, which encodes strongly driven doublon-holon dynamics at sub-optical-cycle timescales. We observe a positive chirp for above band gap harmonics, indicating that high harmonics are dominated by doublon-holon recombinations. We further show a harmonic order-dependent dephasing, which can be understood through different doublon-holon excursion distances associated with each harmonic. These results reveal coherent doublon-holon dynamics and their ultrafast dephasing in Mott insulators, which is relevant to other nonequilibrium light-induced phenomena, such as Floquet engineering.
High harmonic generation (HHG) has emerged as a powerful probe of ultrafast electron dynamics in solids. However, in strongly correlated materials, where electronic excitations arise from many-body interactions rather than single-particle band dispersion, the field remains in its infancy. Here, we report HHG up to the 23rd^{rd}rd order in the prototypical Mott insulator La2_22​CuO4_44​. We observe a robust 4 eV cutoff that is independent of driving field strength, revealing an intrinsic energy scale defined by the Hubbard bands. Using time-resolved high harmonic spectroscopy, we disentangle the distinct contributions of carrier creation, intraband acceleration, and interband recombination to the nonequilibrium radiation spectrum. We demonstrate that photo-doping triggers a fundamental reorganization of the many-body manifolds above a critical excitation density, a process that renormalizes the band curvature and suppresses nonlinear intraband currents, thereby directly imprinting the signature of many-body band reconstruction onto the harmonic emission. These results establish HHG as a sensitive probe of subtle correlation-driven electronic reconstructions and highlight that many-body interactions enable extreme nonlinear optical responses that are highly tunable in nonequilibrium states.
High-harmonic generation (HHG) in strongly correlated Mott insulators is investigated using exact diagonalization and time-dependent density-matrix propagation of a laser-driven one-dimensional Hubbard chain. By projecting onto equilibrium Hubbard bands, we use the doublon population and its dynamics as a diagnostic to analyze intraband (spin-wave-like) and interband (doublon-holon creation) excitation channels. A filling-dependent crossover emerges: Bloch-like intraband response at dilute filling, mixed dynamics at intermediate filling, and interband-dominated HHG with plateau and cutoff near half filling. In the considered parameter range, increasing interaction strength UUU strongly suppresses interband contributions through the enlarged Mott gap and correlation-induced localization. Intra- and interband current decomposition reveals opposing flows below the Mott gap (Δ_{\mathrm{Mott}}) and selective dephasing suppression of interband coherence, enhancing net doublon accumulation. Time-frequency analysis uncovers the filling-dependent features of quantum trajectories, manifesting in distinct below-Δ_{\mathrm{Mott}} emission. This doublon-based analysis provides a transparent link between equilibrium spin-charge separation and nonequilibrium strong-field response, and clarifies how dephasing modifies interband coherence and doublon accumulation.