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

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-liv...

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Autores principales: Nishida, Jun, Johnson, Samuel C., Chang, Peter T. S., Wharton, Dylan M., Dönges, Sven A., Khatib, Omar, Raschke, Markus B.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8885862/
https://www.ncbi.nlm.nih.gov/pubmed/35228517
http://dx.doi.org/10.1038/s41467-022-28224-9
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author Nishida, Jun
Johnson, Samuel C.
Chang, Peter T. S.
Wharton, Dylan M.
Dönges, Sven A.
Khatib, Omar
Raschke, Markus B.
author_facet Nishida, Jun
Johnson, Samuel C.
Chang, Peter T. S.
Wharton, Dylan M.
Dönges, Sven A.
Khatib, Omar
Raschke, Markus B.
author_sort Nishida, Jun
collection PubMed
description 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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spelling pubmed-88858622022-03-17 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. Nat Commun Article 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. Nature Publishing Group UK 2022-02-28 /pmc/articles/PMC8885862/ /pubmed/35228517 http://dx.doi.org/10.1038/s41467-022-28224-9 Text en © The Author(s) 2022 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Nishida, Jun
Johnson, Samuel C.
Chang, Peter T. S.
Wharton, Dylan M.
Dönges, Sven A.
Khatib, Omar
Raschke, Markus B.
Ultrafast infrared nano-imaging of far-from-equilibrium carrier and vibrational dynamics
title Ultrafast infrared nano-imaging of far-from-equilibrium carrier and vibrational dynamics
title_full Ultrafast infrared nano-imaging of far-from-equilibrium carrier and vibrational dynamics
title_fullStr Ultrafast infrared nano-imaging of far-from-equilibrium carrier and vibrational dynamics
title_full_unstemmed Ultrafast infrared nano-imaging of far-from-equilibrium carrier and vibrational dynamics
title_short Ultrafast infrared nano-imaging of far-from-equilibrium carrier and vibrational dynamics
title_sort ultrafast infrared nano-imaging of far-from-equilibrium carrier and vibrational dynamics
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8885862/
https://www.ncbi.nlm.nih.gov/pubmed/35228517
http://dx.doi.org/10.1038/s41467-022-28224-9
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