Separation of experimental 2D IR frequency-frequency correlation functions into structural and reorientation-induced contributions Article Swipe
Patrick L. Kramer
,
Jun Nishida
,
M. D. Fayer
·
YOU?
·
· 2015
· Open Access
·
· DOI: https://doi.org/10.1063/1.4931402
YOU?
·
· 2015
· Open Access
·
· DOI: https://doi.org/10.1063/1.4931402
A vibrational transition frequency can couple to its environment through a directional vector interaction. In such cases, reorientation of the vibrational transition dipole (molecular orientational relaxation) and its frequency fluctuations can be strongly coupled. It was recently shown [Kramer et al., J. Chem. Phys. 142, 184505 (2015)] that differing frequency-frequency correlation function (FFCF) decays, due to reorientation-induced spectral diffusion (RISD), are observed with different two-dimensional infrared polarization configurations when such strong coupling is present. The FFC functional forms were derived for the situation in which all spectral diffusion is due to reorientational motion. We extend the previous theory to include vibrational frequency evolution (spectral diffusion) caused by structural fluctuations of the medium. Model systems with diffusive reorientation and several regimes of structural spectral diffusion rates are analyzed for first order Stark effect interactions. Additionally, the transition dipole reorientational motion in complex environments is frequently not completely diffusive. Several periods of restricted angular motion (wobbling-in-a-cone) may precede the final diffusive orientational randomization. The polarization-weighted FFCF decays are presented in this case of restricted transition dipole wobbling. With these extensions to the polarization-dependent FFCF expressions, the structural spectral diffusion dynamics of methanol in the room temperature ionic liquid 1-hexyl-3-methylimidazolium hexafluorophosphate can be separated quantitatively from RISD using the experimental center line slope data. In addition, prior results on the spectral diffusion of water, methanol, and ethanol in 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide are re-examined to elucidate the influence of reorientation on the data, which were interpreted in terms of structural fluctuations.
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- Type
- article
- Language
- en
- Landing Page
- https://doi.org/10.1063/1.4931402
- OA Status
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- Cited By
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- References
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https://openalex.org/W1912811808Canonical identifier for this work in OpenAlex
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https://doi.org/10.1063/1.4931402Digital Object Identifier
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Separation of experimental 2D IR frequency-frequency correlation functions into structural and reorientation-induced contributionsWork title
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articleOpenAlex work type
- Language
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enPrimary language
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2015Year of publication
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2015-09-28Full publication date if available
- Authors
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Patrick L. Kramer, Jun Nishida, M. D. FayerList of authors in order
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https://doi.org/10.1063/1.4931402Publisher landing page
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YesWhether a free full text is available
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greenOpen access status per OpenAlex
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https://www.osti.gov/biblio/1229678Direct OA link when available
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Dipole, Rotational diffusion, Chemistry, Polarization (electrochemistry), Diffusion, Relaxation (psychology), Molecular vibration, Molecular physics, Chemical physics, Physics, Molecule, Physical chemistry, Thermodynamics, Psychology, Social psychology, Organic chemistryTop concepts (fields/topics) attached by OpenAlex
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49Total citation count in OpenAlex
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2024: 4, 2023: 1, 2022: 3, 2021: 7, 2020: 7Per-year citation counts (last 5 years)
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10Other works algorithmically related by OpenAlex
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| publication_date | 2015-09-28 |
| publication_year | 2015 |
| referenced_works | https://openalex.org/W2127577365, https://openalex.org/W2123453296, https://openalex.org/W1998643104, https://openalex.org/W2118522276, https://openalex.org/W2073968024, https://openalex.org/W2087322664, https://openalex.org/W2312672170, https://openalex.org/W2057124482, https://openalex.org/W2040871466, https://openalex.org/W331729359, https://openalex.org/W2323004863, https://openalex.org/W2109467211, https://openalex.org/W2170317460, https://openalex.org/W2050410865, https://openalex.org/W2027186143, https://openalex.org/W1985515789, https://openalex.org/W2165357882, https://openalex.org/W2313154154, https://openalex.org/W1987998850, https://openalex.org/W1982219464, https://openalex.org/W2029799575, https://openalex.org/W2087872396, https://openalex.org/W2120571018, https://openalex.org/W2064141166, https://openalex.org/W2008556254, https://openalex.org/W2075187353, https://openalex.org/W2077894462, https://openalex.org/W1974292841, https://openalex.org/W2025717854, https://openalex.org/W1971409383, https://openalex.org/W1988137457, https://openalex.org/W2067051784, https://openalex.org/W2025381545, https://openalex.org/W2170062453, https://openalex.org/W2330884986, https://openalex.org/W1996619573, https://openalex.org/W2128097747, https://openalex.org/W2335324453, https://openalex.org/W2047376058, https://openalex.org/W2043438870, https://openalex.org/W641544850, https://openalex.org/W1564993719, https://openalex.org/W3022806437, https://openalex.org/W2494402508 |
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