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  2. Cogwheel phase cycling in population-detected optical coherent multidimensional spectroscopy
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    Datenpaket: Cogwheel phase cycling in population-detected optical coherent multidimensional spectroscopy

    Alternativer Identifier:
    -
    Verwandter Identifier:
    (Is Supplement To) 10.1063/5.0233694 - DOI
    Ersteller/in:
    Jayachandran, Ajay https://orcid.org/0000-0002-5265-0502 [University of Würzburg]

    Müller, Stefan https://orcid.org/0009-0002-6384-9282 [University of Würzburg]
    Beitragende:
    (Project Leader)
    Brixner, Tobias https://orcid.org/0000-0002-6529-704X [University of Würzburg]
    Titel:
    Cogwheel phase cycling in population-detected optical coherent multidimensional spectroscopy
    Weitere Titel:
    -
    Beschreibung:
    (Abstract) An integral procedure in every coherent multidimensional spectroscopy experiment is to suppress undesired background signals. For that purpose, one can employ a particular phase-matching geometry or phase cycling, a procedure that was adapted from nuclear magnetic resonance (NMR) spectroscopy. In optical multidimensional spectroscopy, phase cycling has been usually carried out in a “nested” fashion, where pulse phases are incremented sequentially with linearly spaced increments. Another phase-cycling approach which was developed for NMR spectroscopy is “cogwheel phase cycling,” where all pulse phases are varied simultaneously in increments defined by so-called “winding numbers”. Here we explore the concept of cogwheel phase cycling in the context of population-based coherent multidimensional spectroscopy. We derive selection rules for resolving and extracting fourth-order and higher-order nonlinear signals by cogwheel phase cycling and describe how to perform a numerical search for the winding numbers for various population-detected 2D spectroscopy experiments. We also provide an expression for a numerical search for nested phase-cycling schemes and predict the most economical schemes of both approaches for a wide range of nonlinear signals. The signal selectivity of the technique is demonstrated experimentally by acquiring rephasing and nonrephasing fourth-order signals of a laser dye by both phase-cycling approaches. We find that individual nonlinear signal contributions are, in most cases, captured with fewer steps by cogwheel phase cycling compared to nested phase cycling.
    Schlagworte:
    Multidimensional spectroscopy
    Phase cycling
    Fluorescence
    Zugehörige Informationen:
    -
    Sprache:
    Englisch
    Herausgeber/in:
    University of Würzburg
    Erstellungsjahr:
    Fachgebiet:
    Physics
    Chemistry
    Objekttyp:
    Dataset
    Datenquelle:
    -
    Verwendete Software:
    Software für Datenbearbeitung
    Software:
    Matlab - 9.14.0.2206163
    Alternative Software:
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    Datenverarbeitung:
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    Erscheinungsjahr:
    Rechteinhaber/in:
    Förderung:
    European Research Council - (Isolating Many-Particle Correlations in Time and Space) 101141366
    Name Speichervolumen Metadaten Upload Aktion
    Status:
    Publiziert
    Eingestellt von:
    696b272337bbae795272b68d9b435eb0
    Erstellt am:
    Archivierungsdatum:
    2024-11-14
    Archivgröße:
    3,4 MB
    Archiversteller:
    dd7b509482ad0a11773b217cbbcdf32f
    Archiv-Prüfsumme:
    203486718c86d6b5cdff9c080208dffa (MD5)
    Embargo-Zeitraum:
    -