Lance Hatch | Searcharxiv

arXiv2026

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

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.

cond-mat.str-el↗

arXiv2026

Probing lattice fluctuations using solid-state high-harmonic spectroscopy

Solid-state high-harmonic spectroscopy allows the study of strongly driven ultrafast electron dynamics. Microscopically, high harmonics are generated by strong-laser-field acceleration of electron-hole pairs through the lattice. At finite temperatures, atomic-scale structural fluctuations are ubiquitous and are expected to influence the electron-hole trajectories. Yet, the effect of thermal lattice fluctuations on solid-state high-harmonic generation (HHG) has not been quantified. Here, we demonstrate a profound sensitivity of HHG to thermal lattice fluctuations, by characterizing the temperature dependence of HHG in Re6Se8Cl2, a superatomic semiconductor. As the sample temperature is decreased, the high-harmonic yield exhibits a slow increase, followed by an abrupt increase below 50 K, consistent with the temperature at which lattice vibrations are strongly suppressed. Our calculations show that thermal lattice fluctuations both weaken the harmonic response from individual distorted configurations and induce phase dispersion across the ensemble, leading to a pronounced suppression of the coherently emitted harmonics. We show that this effect can be interpreted in terms of an effective electronic dephasing time that varies with temperature. Our results are relevant to dephasing in broad strong-field phenomena, including lightwave electronics and Floquet engineering. The wide tunability of superatomic crystals further enables materials-controlled strong-field physics.

cond-mat.mtrl-sci↗