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

Xuewen Fu (), Francesco Barantani, Simone Gargiulo, Ivan Madan, Gabriele Berruto, Thomas LaGrange, Lei Jin, Junqiao Wu, Giovanni Maria Vanacore, Fabrizio Carbone () and Yimei Zhu ()
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Xuewen Fu: Nankai University
Francesco Barantani: École Polytechnique Fédérale de Lausanne
Simone Gargiulo: École Polytechnique Fédérale de Lausanne
Ivan Madan: École Polytechnique Fédérale de Lausanne
Gabriele Berruto: École Polytechnique Fédérale de Lausanne
Thomas LaGrange: École Polytechnique Fédérale de Lausanne
Lei Jin: University of California
Junqiao Wu: University of California
Giovanni Maria Vanacore: University of Milano-Bicocca
Fabrizio Carbone: École Polytechnique Fédérale de Lausanne
Yimei Zhu: Brookhaven National Laboratory

Nature Communications, 2020, vol. 11, issue 1, 1-11

Abstract: 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.

Date: 2020
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DOI: 10.1038/s41467-020-19636-6

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