Photo-induced insulator-metal transition in paramagnetic (V$_{1-x}$Cr$_{x}$)$_2$O$_3$

TL;DR

This study uses advanced simulations to investigate the ultrafast electronic response of Cr-doped V2O3 to laser excitation, revealing rapid thermalization and challenging previous notions of nonthermal metastable states in photo-induced insulator-metal transitions.

Contribution

It combines non-equilibrium dynamical mean-field theory with first-principles modeling to accurately simulate the ultrafast dynamics of Cr-doped V2O3, providing new insights into its thermalization process.

Findings

Electronic system thermalizes within tens of femtoseconds.

No evidence of metastable nonthermal metal state.

Photo-induced gap filling involves charge reshuffling.

Abstract

Pump-probe experiments with femtosecond time resolution allow to disentangle the electronic dynamics from the lattice response and thus provide valuable insights into the non-equilibrium behavior of correlated materials. In Cr-doped V$_2$O$_3$, a multi-orbital Mott-Hubbard material which has been intensively investigated for decades, time-resolved experiments reported a photo-induced insulator-metal transition leading to a transient metal state with nonthermal properties. Here, we combine non-equilibrium dynamical mean-field theory with realistic first principles modeling to simulate the ultrafast response of this material to a laser excitation. Our calculations reproduce the insulating initial state, with orbital occupations in agreement with experiment, and reveal an ultrafast pump-induced gap filling associated with a charge reshuffling between the $e_g^\pi$ and $a_{1g}$ orbitals. However, in contrast to the related compound VO$_2$, the electronic system thermalizes within a few tens of femtoseconds and we find no evidence for the existence of a metastable nonthermal metal. This suggests that the reported nonthermal behavior in the experiments may be associated with the mismatch between the electronic and lattice temperatures.