Nanoscale-femtosecond dielectric response of Mott insulators captured by two-color near-field ultrafast electron microscopy

Abstract

Characterizing and controlling the out-of-equilibrium state of nanostructured Mott insulators hold great promises for emerging quantum technologies while providing an exciting playground for investigating fundamental physics of strongly-correlated systems. Here, we use two-color near-field ultrafast electron microscopy to photo-induce the insulator-to-metal transition in a single VO₂ nanowire and probe the ensuing electronic dynamics with combined nanometer-femtosecond resolution (10⁻²¹ m ∙ s). We take advantage of a femtosecond temporal gating of the electron pulse mediated by an infrared laser pulse, and exploit the sensitivity of inelastic electron-light scattering to changes in the material dielectric function. By spatially mapping the near-field dynamics of an individual nanowire of VO₂, we observe that ultrafast photo-doping drives the system into a metallic state on a timescale of ~150 fs without yet perturbing the crystalline lattice. Due to the high versatility and sensitivity of the electron probe, our method would allow capturing the electronic dynamics of a wide range of nanoscale materials with ultimate spatiotemporal resolution.

The fs control of an insulator-to-metal transition down to a few nanometers and its real-time/real space observation remain a challenge. Here, the authors demonstrate a method based on ultrafast electron microscopy to provide a nm/fs resolved view of the electronic dynamics in a single VO₂ nanowire.