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arXiv:2609.11858

Sub-cycle doublon-holon dynamics in one-dimensional Mott insulators revealed by two-color high-harmonic spectroscopy

Lance Hatch, Aditya Verma, Eric Schultz, Hanjun Yang, Priscila Rosa, Genda Gu, Igor A. Zaliznyak, Giulio Vampa, Laimei Nie, Hanzhe Liu

Published Sep 10, 2026• 0 citations
arXivHTMLPDF

Abstract

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.

DOI
10.48550/arxiv.2609.11858

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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.
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The key optical and electronic functionalities in condensed materials are determined by the band filling of electrons and their Coulomb correlations. To directly capture how many-body correlations influence the correlated electron dynamics under the driving of laser pulses, the comprehensible quasiparticle picture is desired to distinguish the ultrafast creation and annihilation of doublon-holon pairs in attosecond timescale. Here, we adopt the one-dimensional non-half-filling Hubbard model to study the high-harmonic generation (HHG) in correlated electron systems. As the value of Hubbard UUU increases, the cutoff energy and spectral features in HHG spectra have been revealed and their scaling laws are explained by the characteristic energy gaps obtained from the electronic bands under the quasiparticle picture. The adjustable degree of band filling in correlated systems paves a way to enhance high-harmonic emissions by regulating the creation of doublon-holon pairs. The complex temporal profile of HHG is elucidated in this work by the light-induced evolution of quasiparticle bands in correlated materials. In addition, the dephasing of the HHG spectrum caused by the vibration-induced disorder or lattice temperature is affirmed in the correlated electron systems and this dephasing process is attributed to quasiparticle-lattice scattering during the doublons and holons propagating among the disordered lattice sites.
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 εcutε_{\rm cut}εcut​ scales linearly with the field strength E0E_0E0​ as εcut=Δgap+αE0ε_{\rm cut}=Δ_{\rm gap} + αE_0εcut​=Δgap​+αE0​, where ΔgapΔ_{\rm gap}Δgap​ is the Mott gap. On the other hand, in the stronger-field regime, multiple plateaus emerge and the mmm-th cut-off scales as εcut,m=U+mE0ε_{\rm cut,m}=U + m E_0εcut,m​=U+mE0​. 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.
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.