High harmonic generation reflecting the sub-cycle evolution of the Mott transition under a mid-infrared electric field

TL;DR

This study demonstrates that high-harmonic generation spectroscopy can reveal the sub-cycle electronic dynamics during a Mott insulator-metal transition induced by a mid-infrared laser in a strongly correlated material.

Contribution

It provides the first experimental evidence linking HHG spectral features to ultrafast electronic-structure changes during a Mott transition, supported by dynamical mean-field theory.

Findings

HHG spectra show redshifts at high field amplitudes

Carrier generation is efficient above 6 MV/cm

Spectral features reflect sub-cycle electronic reconstructions

Abstract

Solids in an intense laser field show high-harmonic generation (HHG), which can provide information on carrier dynamics and band structures in weakly correlated systems. In strongly correlated systems, a laser field can induce a transition between the various electronic phases formed by the entanglement of charge, spin, and orbital degrees of freedom via carrier generation. The HHG accompanying this process should contain information on the nonequilibrium electronic-state dynamics along the oscillating field - an aspect that remains unresolved to date. Here, we show that an intense mid-infrared (MIR) pulse induces a Mott insulator-metal transition in a one-dimensional cuprate, Sr2CuO3, the evolution of which is reflected by the spectral features of HHs. When the electric-field amplitude exceeds 6 MV/cm, carriers are efficiently generated and each harmonic frequency decreases from odd multiples of the MIR frequency. Dynamical mean-field theory indicates that these redshifts originate from a series of electronic-structure reconstructions in each electric-field cycle during the melting of the Mott-insulator state, which modifies the radiation phase from carrier recombination cycle-by-cycle. This phenomenon is negligible in rigid-band systems. This experimental-theoretical study confirms that HH spectroscopy research can potentially unravel the sub-cycle dynamics of nonequilibrium phase transitions in correlated materials.