Time-resolved molecular dynamics of single and double hydrogen migration in ethanol
Abstract
Being the lightest, most mobile atom that exists, hydrogen plays an important role in the chemistry of hydrocarbons, proteins and peptides and most biomolecules. Hydrogen can undergo transfer, exchange and migration processes, having considerable impact on the chemical behavior of these molecules. Although much has been learned about reaction dynamics involving one hydrogen atom, less is known about those processes where two or more hydrogen atoms participate. Here we show that single and double hydrogen migrations occurring in ethanol cations and dications take place within a few hundred fs to ps, using a 3D imaging and laser pump-probe technique. For double hydrogen migration, the hydrogens are not correlated, with the second hydrogen migration promoting the breakup of the C–O bond. The probability of double hydrogen migration is quite significant, suggesting that double hydrogen migration plays a more important role than generally assumed. The conclusions are supported by state-of-the-art molecular dynamics calculations.
- Authors:
-
- Univ. of Connecticut, Storrs, CT (United States)
- Universidad Autónoma de Madrid (Spain)
- SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Universidad Autónoma de Madrid (Spain); Instituto Madrileño de Estudios Avanzados en Nanociencia (IMDEA-Nano), Madrid (Spain); Donostia International Physics Center (DIPC), Donostia-San Sebastián (Spain)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1546973
- Grant/Contract Number:
- AC02-76SF00515
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 08 HYDROGEN
Citation Formats
Kling, Nora G., Díaz-Tendero, S., Obaid, R., Disla, M. R., Xiong, H., Sundberg, M., Khosravi, S. D., Davino, M., Drach, P., Carroll, A. M., Osipov, T., Martín, F., and Berrah, N. Time-resolved molecular dynamics of single and double hydrogen migration in ethanol. United States: N. p., 2019.
Web. doi:10.1038/s41467-019-10571-9.
Kling, Nora G., Díaz-Tendero, S., Obaid, R., Disla, M. R., Xiong, H., Sundberg, M., Khosravi, S. D., Davino, M., Drach, P., Carroll, A. M., Osipov, T., Martín, F., & Berrah, N. Time-resolved molecular dynamics of single and double hydrogen migration in ethanol. United States. https://doi.org/10.1038/s41467-019-10571-9
Kling, Nora G., Díaz-Tendero, S., Obaid, R., Disla, M. R., Xiong, H., Sundberg, M., Khosravi, S. D., Davino, M., Drach, P., Carroll, A. M., Osipov, T., Martín, F., and Berrah, N. Thu .
"Time-resolved molecular dynamics of single and double hydrogen migration in ethanol". United States. https://doi.org/10.1038/s41467-019-10571-9. https://www.osti.gov/servlets/purl/1546973.
@article{osti_1546973,
title = {Time-resolved molecular dynamics of single and double hydrogen migration in ethanol},
author = {Kling, Nora G. and Díaz-Tendero, S. and Obaid, R. and Disla, M. R. and Xiong, H. and Sundberg, M. and Khosravi, S. D. and Davino, M. and Drach, P. and Carroll, A. M. and Osipov, T. and Martín, F. and Berrah, N.},
abstractNote = {Being the lightest, most mobile atom that exists, hydrogen plays an important role in the chemistry of hydrocarbons, proteins and peptides and most biomolecules. Hydrogen can undergo transfer, exchange and migration processes, having considerable impact on the chemical behavior of these molecules. Although much has been learned about reaction dynamics involving one hydrogen atom, less is known about those processes where two or more hydrogen atoms participate. Here we show that single and double hydrogen migrations occurring in ethanol cations and dications take place within a few hundred fs to ps, using a 3D imaging and laser pump-probe technique. For double hydrogen migration, the hydrogens are not correlated, with the second hydrogen migration promoting the breakup of the C–O bond. The probability of double hydrogen migration is quite significant, suggesting that double hydrogen migration plays a more important role than generally assumed. The conclusions are supported by state-of-the-art molecular dynamics calculations.},
doi = {10.1038/s41467-019-10571-9},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {2019},
month = {6}
}
Web of Science
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