Optically accessible long-lived electronic biexcitons at room temperature in strongly coupled H- aggregates

Sohoni, Siddhartha; Ghosh, Indranil; Nash, Geoffrey T.; Jones, Claire A.; Lloyd, Lawson T.; Li, Beiye C.; Ji, Karen L.; Wang, Zitong; Lin, Wenbin; Engel, Gregory S.

doi:10.1038/s41467-024-52341-2

Nat Commun

2024

DOI: 10.1038/s41467-024-52341-2

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Optically accessible long-lived electronic biexcitons at room temperature in strongly coupled H- aggregates

Siddhartha Sohoni,

Indranil Ghosh,

Geoffrey T. Nash

et al.

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2024

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Cogwheel phase cycling in population-detected optical coherent multidimensional spectroscopy

Jayachandran,

Mueller,

Brixner

2024

The Journal of Chemical Physics

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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 that 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.

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Cogwheel phase cycling in population-detected optical coherent multidimensional spectroscopy

Jayachandran,

Mueller,

Brixner

2024

The Journal of Chemical Physics

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show abstract

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Optically accessible long-lived electronic biexcitons at room temperature in strongly coupled H- aggregates

Cited by 1 publication

References 69 publications

Cogwheel phase cycling in population-detected optical coherent multidimensional spectroscopy

Cogwheel phase cycling in population-detected optical coherent multidimensional spectroscopy

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