2026-10-11T23:34:27Zhttps://www.radar-service.eu/oai/OAIHandler

10.58160/stAWtPUnpVRsOspy2026-04-24T07:50:14Z

https://dx.doi.org/10.58160/stAWtPUnpVRsOspy Jayachandran, Ajay Müller, Stefan Cogwheel phase cycling in population-detected optical coherent multidimensional spectroscopy University of Würzburg 2024 Physics Chemistry dataset Dataset info:eu-repo/semantics/openAccess https://creativecommons.org/licenses/by/4.0/legalcode Brixner, Tobias 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. Multidimensional spectroscopy Phase cycling Fluorescence Brixner, Tobias eng 10.1063/5.0233694 https://ror.org/0472cxd90 application/x-tar