dorsal/arxiv
View SchemaEnergy-level diagrams and their contribution to fifth-order Raman and second-order infrared responses: Distinction between relaxation mechanisms by two-dimensional spectroscopy
| Authors | Ko Okumura, Yoshitaka Tanimura |
|---|---|
| Categories | |
| ArXiv ID | physics/0211122 |
| URL | https://arxiv.org/abs/physics/0211122 |
| DOI | 10.1021/jp027360o |
Abstract
We develop a Feynman rule for energy-level diagrams emphasizing their connections to the double-sided Feynman diagrams and physical processes in the Liouville space. Thereby we completely identify such diagrams and processes contributing to the two-dimensional response function in the Brownian oscillator model. We classify such diagrams or processes in quartet and numerically present signals separately from each quartet of diagrams or Liouville-space processes. We find that the signal from each quartet is distinctly different from the others; we can identify each peaks in frequency domain with a certain quartet. This offers the basis for analyzing and assigning actual two-dimensional peaks and suggests the possibility of Liouville-space-path selective spectroscopy. As an application we demonstrate an example in which two familiar homogeneous mechanisms of relaxation are distinguished by existence or non-existence of certain peaks on the two-dimensional map; appearance or disappearance of certain peak is sensitive to the coupling mechanism. We also point out some confusion in the literature with regard to inclusion of relaxation effects.
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"abstract": "We develop a Feynman rule for energy-level diagrams emphasizing their\nconnections to the double-sided Feynman diagrams and physical processes in the\nLiouville space. Thereby we completely identify such diagrams and processes\ncontributing to the two-dimensional response function in the Brownian\noscillator model. We classify such diagrams or processes in quartet and\nnumerically present signals separately from each quartet of diagrams or\nLiouville-space processes. We find that the signal from each quartet is\ndistinctly different from the others; we can identify each peaks in frequency\ndomain with a certain quartet. This offers the basis for analyzing and\nassigning actual two-dimensional peaks and suggests the possibility of\nLiouville-space-path selective spectroscopy. As an application we demonstrate\nan example in which two familiar homogeneous mechanisms of relaxation are\ndistinguished by existence or non-existence of certain peaks on the\ntwo-dimensional map; appearance or disappearance of certain peak is sensitive\nto the coupling mechanism. We also point out some confusion in the literature\nwith regard to inclusion of relaxation effects.",
"arxiv_id": "physics/0211122",
"authors": [
"Ko Okumura",
"Yoshitaka Tanimura"
],
"categories": [
"physics.chem-ph"
],
"doi": "10.1021/jp027360o",
"title": "Energy-level diagrams and their contribution to fifth-order Raman and second-order infrared responses: Distinction between relaxation mechanisms by two-dimensional spectroscopy",
"url": "https://arxiv.org/abs/physics/0211122"
},
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