Cogwheel phase cycling in population-detected optical coherent multidimensional spectroscopy

DOI

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.

Identifier
DOI https://doi.org/10.58160/stAWtPUnpVRsOspy
Related Identifier IsSupplementTo https://doi.org/10.1063/5.0233694
Metadata Access https://www.radar-service.eu/oai/OAIHandler?verb=GetRecord&metadataPrefix=datacite&identifier=10.58160/stAWtPUnpVRsOspy
Provenance
Creator Jayachandran, Ajay ORCID logo; Müller, Stefan ORCID logo
Publisher University of Würzburg
Contributor RADAR
Publication Year 2024
Funding Reference European Research Council https://ror.org/0472cxd90 ROR 101141366 https://cordis.europa.eu/project/id/101141366 Isolating Many-Particle Correlations in Time and Space
Rights Open Access; Creative Commons Attribution 4.0 International; info:eu-repo/semantics/openAccess; https://creativecommons.org/licenses/by/4.0/legalcode
OpenAccess true
Representation
Language English
Resource Type Dataset
Format application/x-tar
Discipline Chemistry; Natural Sciences; Physics