The DOI matches its Crossref record; 43 of the 43 references it cites were found in a registry or an index.
Fluorescence-detected two-dimensional electronic coherence spectroscopy by acousto-optic phase modulation
Abstract
Two-dimensional electronic coherence spectroscopy (ECS) is an important method to study the coupling between distinct optical modes of a material system. Such studies often involve excitation using a sequence of phased ultrashort laser pulses. In conventional approaches, the delays between pulse temporal envelopes must be precisely monitored or maintained. Here, we introduce a new experimental scheme for phase-selective nonlinear ECS, which combines acousto-optic phase modulation with ultrashort laser excitation to produce intensity modulated nonlinear fluorescence signals. We isolate specific nonlinear signal contributions by synchronous detection, with respect to appropriately constructed references. Our method effectively decouples the relative temporal phases from the pulse envelopes of a collinear train of four sequential pulses. We thus achieve a robust and high signal-to-noise scheme for phase-selective ECS to investigate the resonant nonlinear optical response of photoluminescent systems. We demonstrate the validity of our method using a model quantum three-level system—atomic Rb vapor. Moreover, we show how our measurements determine the resonant complex-valued third-order susceptibility.
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Metadata
- Authors
- Tekavec, P. F., Lott, G. A., & Marcus, A. H.
- Venue
- The Journal of Chemical Physics
- Publisher
- AIP Publishing
- Published
- 2007-12-07
- Volume
- 127
- Issue
- 21
- Pages
- 214307-214307
- ISSN
- 0021-9606 (ISSN-L)
- 1089-7690
- OpenAlex
- W2069852394
- Cited by
- 368
- References
- 43
- FWCI
- 3.46
- Type
- journal article
- Language
- en
- Open access
- closed
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- Tekavec, P. F., Lott, G. A., & Marcus, A. H. (2007). Fluorescence-detected two-dimensional electronic coherence spectroscopy by acousto-optic phase modulation. The Journal of Chemical Physics. https://doi.org/10.1063/1.2800560
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