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Double proton transfer dynamics of model DNA base pairs in the condensed phase
Open accessAbstract
The dynamics of excited-state double proton transfer of model DNA base pairs, 7-azaindole dimers, is reported using femtosecond fluorescence spectroscopy. To elucidate the nature of the transfer in the condensed phase, here we examine variation of solvent polarity and viscosity, solute concentration, and isotopic fractionation. The rate of proton transfer is found to be significantly dependent on polarity and on the isotopic composition in the pair. Consistent with a stepwise mechanism, the results support the presence of an ionic intermediate species which forms on the femtosecond time scale and decays to the final tautomeric form on the picosecond time scale. We discuss the results in relation to the molecular motions involved and comment on recent claims of concerted transfer in the condensed phase. The nonconcerted mechanism is in agreement with previous isolated-molecule femtosecond dynamics and is also consistent with the most-recent high-level theoretical study on the same pair.
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Femtosecond molecular dynamics of tautomerization in model base pairs
Douhal, A., Kim, S. K., & Zewail, A. H. (1995) · Nature · doi:10.1038/378260a0 · Cited by 492
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Recent Advances and Perspectives on Nonadiabatic Mixed Quantum–Classical Dynamics
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Hsieh, C.-C., Jiang, C.-M., & Chou, P.-T. (2010) · Accounts of Chemical Research · doi:10.1021/ar1000499 · Cited by 383
Brovarets, O. O., & Hovorun, D. M. (2014) · Journal of Biomolecular Structure and Dynamics · doi:10.1080/07391102.2012.755795 · Cited by 148
Sauri, V., Gobbo, J. P., Serrano-Pérez, J. J., Lundberg, M., Coto, P. B., Serrano-Andrés, L., Borin, A. C., Lindh, R., Merchán, M., & Roca-Sanjuán, D. (2013) · Journal of Chemical Theory and Computation · doi:10.1021/ct3006166 · Cited by 56
Metadata
- Authors
- Kwon, O.-H., & Zewail, A. H.
- Venue
- Proceedings of the National Academy of Sciences
- Published
- 2007-05-22
- Volume
- 104
- Issue
- 21
- Pages
- 8703-8708
- ISSN
- 0027-8424 (ISSN-L)
- 1091-6490
- OpenAlex
- W2074319606
- Cited by
- 174
- References
- 1
- FWCI
- 10.18
- Type
- journal article
- Language
- en
- Open access
- bronze
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- Kwon, O.-H., & Zewail, A. H. (2007). Double proton transfer dynamics of model DNA base pairs in the condensed phase. Proceedings of the National Academy of Sciences. https://doi.org/10.1073/pnas.0702944104
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