Large-amplitude transfer motion of hydrated excess protons mapped by ultrafast 2D IR spectroscopy
Solvation and transport of excess protons in aqueous systems play a fundamental role in acid-base chemistry and biochemical processes. We mapped ultrafast proton excursions along the proton transfer coordinate by means of two-dimensional infrared spectroscopy, both in bulk water and in a Zundel cati...
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| Veröffentlicht in: | Science (American Association for the Advancement of Science) 2017-08, Vol.357 (6350), p.491-495 |
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| creator | Dahms, Fabian Fingerhut, Benjamin P. Nibbering, Erik T. J. Pines, Ehud Elsaesser, Thomas |
| description | Solvation and transport of excess protons in aqueous systems play a fundamental role in acid-base chemistry and biochemical processes. We mapped ultrafast proton excursions along the proton transfer coordinate by means of two-dimensional infrared spectroscopy, both in bulk water and in a Zundel cation (H₅O₂)⁺ motif selectively prepared in acetonitrile. Electric fields from the environment and stochastic hydrogen bond motions induce fluctuations of the proton double-minimum potential. Within the lifetime of a particular hydration geometry, the proton explores a multitude of positions on a sub-100-femtosecond time scale. The proton transfer vibration is strongly damped by its 20- to 40-femtosecond population decay. Our results suggest a central role of Zundel-like geometries in aqueous proton solvation and transport. |
| doi_str_mv | 10.1126/science.aan5144 |
| format | Article |
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J. ; Pines, Ehud ; Elsaesser, Thomas</creator><creatorcontrib>Dahms, Fabian ; Fingerhut, Benjamin P. ; Nibbering, Erik T. J. ; Pines, Ehud ; Elsaesser, Thomas</creatorcontrib><description>Solvation and transport of excess protons in aqueous systems play a fundamental role in acid-base chemistry and biochemical processes. We mapped ultrafast proton excursions along the proton transfer coordinate by means of two-dimensional infrared spectroscopy, both in bulk water and in a Zundel cation (H₅O₂)⁺ motif selectively prepared in acetonitrile. Electric fields from the environment and stochastic hydrogen bond motions induce fluctuations of the proton double-minimum potential. Within the lifetime of a particular hydration geometry, the proton explores a multitude of positions on a sub-100-femtosecond time scale. The proton transfer vibration is strongly damped by its 20- to 40-femtosecond population decay. Our results suggest a central role of Zundel-like geometries in aqueous proton solvation and transport.</description><identifier>ISSN: 0036-8075</identifier><identifier>EISSN: 1095-9203</identifier><identifier>DOI: 10.1126/science.aan5144</identifier><identifier>PMID: 28705988</identifier><language>eng</language><publisher>United States: American Association for the Advancement of Science</publisher><subject>Acetonitrile ; Acids ; Chemical bonds ; Homing ; Hydrogen bonding ; Hydrogen bonds ; Infrared spectroscopy ; Literary Devices ; Organic Chemistry ; Persistence ; Protons ; Solvation ; Spectroscopy ; Stochasticity ; Time ; Transport ; Vibration ; Water ; Water chemistry</subject><ispartof>Science (American Association for the Advancement of Science), 2017-08, Vol.357 (6350), p.491-495</ispartof><rights>Copyright © 2017 by the American Association for the Advancement of Science</rights><rights>Copyright © 2017 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. 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| subjects | Acetonitrile Acids Chemical bonds Homing Hydrogen bonding Hydrogen bonds Infrared spectroscopy Literary Devices Organic Chemistry Persistence Protons Solvation Spectroscopy Stochasticity Time Transport Vibration Water Water chemistry |
| title | Large-amplitude transfer motion of hydrated excess protons mapped by ultrafast 2D IR spectroscopy |
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