Ultrafast infrared nano-imaging of far-from-equilibrium carrier and vibrational dynamics

Jun Nishida, Samuel C. Johnson, Peter T. S. Chang, Dylan M. Wharton, Sven A. Dönges, Omar Khatib and Markus B. Raschke ()
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Jun Nishida: University of Colorado
Samuel C. Johnson: University of Colorado
Peter T. S. Chang: University of Colorado
Dylan M. Wharton: University of Colorado
Sven A. Dönges: University of Colorado
Omar Khatib: University of Colorado
Markus B. Raschke: University of Colorado

Nature Communications, 2022, vol. 13, issue 1, 1-9

Abstract: Abstract Ultrafast infrared nano-imaging has demonstrated access to ultrafast carrier dynamics on the nanoscale in semiconductor, correlated-electron, or polaritonic materials. However, mostly limited to short-lived transient states, the contrast obtained has remained insufficient to probe important long-lived excitations, which arise from many-body interactions induced by strong perturbation among carriers, lattice phonons, or molecular vibrations. Here, we demonstrate ultrafast infrared nano-imaging based on excitation modulation and sideband detection to characterize electron and vibration dynamics with nano- to micro-second lifetimes. As an exemplary application to quantum materials, in phase-resolved ultrafast nano-imaging of the photoinduced insulator-to-metal transition in vanadium dioxide, a distinct transient nano-domain behavior is quantified. In another application to lead halide perovskites, transient vibrational nano-FTIR spatially resolves the excited-state polaron-cation coupling underlying the photovoltaic response. These examples show how heterodyne pump-probe nano-spectroscopy with low-repetition excitation extends ultrafast infrared nano-imaging to probe elementary processes in quantum and molecular materials in space and time.

Date: 2022
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DOI: 10.1038/s41467-022-28224-9

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