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

Nishida, Jun; Johnson, Samuel C.; Chang, Peter T. S.; Wharton, Dylan M.; Dönges, Sven A.; Khatib, Omar; Raschke, Markus B.

doi:10.1038/s41467-022-28224-9

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

Journal Article · Mon Feb 28 00:00:00 EST 2022 · Nature Communications

DOI:https://doi.org/10.1038/s41467-022-28224-9· OSTI ID:1904494

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^[1]; Chang, Peter T. S. ^[1];

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Univ. of Colorado, Boulder, CO (United States)

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.

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Research Organization:: Univ. of Colorado, Boulder, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); National Science Foundation (NSF)

Grant/Contract Number:: SC0008807; DMR-1548924

OSTI ID:: 1904494

Journal Information:: Nature Communications, Vol. 13, Issue 1; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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