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Multidimensional infrared spectroscopy of water. II. Hydrogen bond switching dynamics
Abstract
We use multidimensional infrared spectroscopy of the OH stretch of HOD in D2O to measure the interconversion of different hydrogen bonding environments. The OH stretching frequency distinguishes hydrogen bonded (HB) and non-hydrogen-bonded (NHB) configurations by their absorption on the low (red) and high (blue) sides of the line shape. Measured asymmetries in the two dimensional infrared OH line shapes are manifestations of the fundamentally different spectral relaxations of HB and NHB. HB oscillators exhibit coherent oscillations within the hydrogen-bonded free energy well before undergoing activated barrier crossing, resulting in the exchange of hydrogen bonded partners. Conversely, NHB oscillators rapidly return to HB frequencies within 150fs. These results support a picture where NHB configurations are only visited transiently during large fluctuations about a hydrogen bond or during the switching of hydrogen bonding partners. The results are not consistent with the presence of entropically stabilized dangling hydrogen bonds or a conceptual picture of water as a mixture of environments with varying hydrogen bond strength separated by barriers >kT.
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Cites
Computer Simulation of Liquids
Allen, M. P., & Tildesley, D. J. (2017) · doi:10.1093/oso/9780198803195.001.0001 · Cited by 20,945
Large local energy fluctuations in water. II. Cooperative motions and fluctuations
Ohmine, I., Tanaka, H., & Wolynes, P. G. (1988) · The Journal of Chemical Physics · doi:10.1063/1.455536 · Cited by 216
Cited by
Coherent Two-Dimensional Optical Spectroscopy
Cho, M. (2008) · Chemical Reviews · doi:10.1021/cr078377b · Cited by 835
On the Molecular Mechanism of Water Reorientation
Laage, D., & Hynes, J. T. (2008) · The Journal of Physical Chemistry B · doi:10.1021/jp805217u · Cited by 438
Structure, Dynamics, and Spectral Diffusion of Water from First-Principles Molecular Dynamics
Bankura, A., Karmakar, A., Carnevale, V., Chandra, A., & Klein, M. L. (2014) · The Journal of Physical Chemistry C · doi:10.1021/jp506120t · Cited by 166
Metadata
- Authors
- Loparo, J. J., Roberts, S. T., & Tokmakoff, A.
- Venue
- The Journal of Chemical Physics
- Publisher
- AIP Publishing
- Published
- 2006-11-21
- Volume
- 125
- Issue
- 19
- Pages
- 194522-194522
- ISSN
- 0021-9606 (ISSN-L)
- 1089-7690
- OpenAlex
- W1966035771
- Cited by
- 186
- References
- 2
- FWCI
- 9.67
- Type
- journal article
- Language
- en
- Open access
- closed
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