Coherent response of the electronic system driven by non-interfering laser pulses

  • The strength of light–matter interaction in condensed matter is fundamentally linked to the orientation and oscillation strength of the materials’ optical transition dipoles. Structurally anisotropic materials, e.g., elongated molecules, exhibit optical transition dipoles with fixed orientations that govern the angular-dependent light–matter interaction. Contrary, free electron-like metals should exhibit isotropic light–matter interaction with the light fields dictating the orientation of the optical transition dipoles. Here, we demonstrate that an anisotropic direction of the optical transition dipoles even exists in highly free electron-like noble metal surfaces. Our time- and phase-resolved photoemission experiment reveals coherent interference effects on the (110)-oriented silver surface after optical excitation with two non-interfering cross-polarized pulses. We explain this coherent material response within the density matrix formalism by an intrinsic coupling of theThe strength of light–matter interaction in condensed matter is fundamentally linked to the orientation and oscillation strength of the materials’ optical transition dipoles. Structurally anisotropic materials, e.g., elongated molecules, exhibit optical transition dipoles with fixed orientations that govern the angular-dependent light–matter interaction. Contrary, free electron-like metals should exhibit isotropic light–matter interaction with the light fields dictating the orientation of the optical transition dipoles. Here, we demonstrate that an anisotropic direction of the optical transition dipoles even exists in highly free electron-like noble metal surfaces. Our time- and phase-resolved photoemission experiment reveals coherent interference effects on the (110)-oriented silver surface after optical excitation with two non-interfering cross-polarized pulses. We explain this coherent material response within the density matrix formalism by an intrinsic coupling of the non-interfering light fields mediated by optical transition dipoles with fixed orientations in silver.show moreshow less

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Metadaten
Author:Tobias Eul, Eva Prinz, Michael Hartelt, Benjamin Frisch, Martin Aeschlimann, Benjamin StadtmüllerGND
URN:urn:nbn:de:bvb:384-opus4-1129956
Frontdoor URLhttps://opus.bibliothek.uni-augsburg.de/opus4/112995
ISSN:2041-1723OPAC
Parent Title (English):Nature Communications
Publisher:Springer Science and Business Media LLC
Type:Article
Language:English
Year of first Publication:2022
Publishing Institution:Universität Augsburg
Release Date:2024/05/14
Volume:13
Issue:1
First Page:3324
DOI:https://doi.org/10.1038/s41467-022-30768-9
Institutes:Mathematisch-Naturwissenschaftlich-Technische Fakultät
Mathematisch-Naturwissenschaftlich-Technische Fakultät / Institut für Physik
Mathematisch-Naturwissenschaftlich-Technische Fakultät / Institut für Physik / Lehrstuhl für Experimentalphysik II
Dewey Decimal Classification:5 Naturwissenschaften und Mathematik / 53 Physik / 530 Physik
Licence (German):CC-BY 4.0: Creative Commons: Namensnennung (mit Print on Demand)