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arXiv:1911.04183 · International Conference on Strongly Correlated Electron Systems (SCES)

Floquet DMFT Analysis of High Harmonic Generation in Mott Insulators

Yuta Murakami, Martin Eckstein, Philipp Werner

Published Mar 18, 2020• 1 citation
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Abstract

We study the high harmonic generation (HHG) in Mott insulators using Floquet dynamical mean-field theory (DMFT). We show that the main origin of the HHG in Mott insulators is the doublon-holon recombination, and that the character of the HHG spectrum differs depending on the field strength. In the weaker-field regime, the HHG spectrum shows a single plateau as in the HHG from gases, and its cut-off energy $ε_{\rm cut}$ scales linearly with the field strength $E_0$ as $ε_{\rm cut}=Δ_{\rm gap} + αE_0$, where $Δ_{\rm gap}$ is the Mott gap. On the other hand, in the stronger-field regime, multiple plateaus emerge and the $m$-th cut-off scales as $ε_{\rm cut,m}=U + m E_0$. We show that this difference originates from the different dynamics of the doublons and holons in the weak- and strong-field regimes. We also comment on the similarities and differences between HHG from Mott insulators and from semiconductors. This proceedings paper complements our recent work, Phys. Rev. Lett. 121, 057405 (2018), with additional results and analyses.

DOI
10.7566/jpscp.30.011183

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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.
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.
In recent years, the study of phenomena pertaining to non-linear properties of materials has seen a major upswing - especially in the context of High Harmonic Generation (HHG). In this thesis, an account of the current state of research in this area will be given. In addition, we seek to combine two seemingly disparate areas of research, both of which have been the subject of numerous years of intense research - namely those of HHG in solid state materials, and the optical response of strongly correlated quantum systems. To this end we will rely on solving the Fermi-Hubbard model coupled to an electromagnetic field under time propagation. With the aid of both numerical work and simple energy level analyses, we are able to explain most of the characteristics of our calculated spectra. High field strength will induce a Mott insulator to metal phase transition whose imprints will be established through time resolved high harmonic emission and doublon and spin correlation functions. The various HHG spectra, together with said correlation functions will be studied through an Exact diagonalization algorithm in conjunction with an Arnoldi-Lanczos time propagator. The parameter space considered is comprised of the electron-electron repulsion energy, U, and peak electric field strength. Additionally, the study is not restricted to half-filling, and results for doped materials will be presented. We find that the high U-induced energy gap in the Fermi-Hubbard model plays the same role as the valence-conduction bandgap in models like for instance the Semiconductor Bloch Equations when it comes to generating high harmonic radiation through multiphoton processes. The central part of this thesis aims at providing insight to and making further contributions to an article published in Nature Photonics in March 2018. [1]
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.