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  Experimentally probing the libration of interfacial water: the rotational potential of water is stiffer at the air/water interface than in bulk liquid

Tong, Y., Kampfrath, T., & Campen, R. K. (2016). Experimentally probing the libration of interfacial water: the rotational potential of water is stiffer at the air/water interface than in bulk liquid. Physical Chemistry Chemical Physics, 18(27), 18424-18430. doi:10.1039/C6CP01004K.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-002A-FB14-B Version Permalink: http://hdl.handle.net/11858/00-001M-0000-002D-D430-4
Genre: Journal Article

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2016
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 Creators:
Tong, Yujin1, Author              
Kampfrath, Tobias1, Author              
Campen, R. Kramer1, Author              
Affiliations:
1Physical Chemistry, Fritz Haber Institute, Max Planck Society, ou_634546              

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 Abstract: Most properties of liquid water are determined by its hydrogen-bond network. Because forming an aqueous interface requires termination of this network, one might expect the molecular level properties of interfacial water to markedly differ from water in bulk. Intriguingly, much prior experimental and theoretical work has found that, from the perspective of their time-averaged structure and picosecond structural dynamics, hydrogen-bonded OH groups at an air/water interface behave the same as hydrogen-bonded OH groups in bulk liquid water. Here we report the first experimental observation of interfacial water’s libration (i.e. frustrated rotation). We find this mode has a frequency of 834 cm-1, ≈ 165 cm-1 higher than in bulk liquid water at the same temperature and similar to bulk ice. Because libration frequency is proportional to the stiffness of water's rotational potential, this increase suggests that one effect of terminating bulk water's hydrogen bonding network at the air/water interface is retarding rotation of water around intact hydrogen bonds. Because in bulk liquid water the libration plays a key role in stabilizing reaction intermediates and dissipating excess vibrational energy, the ability to probe this mode in interfacial water opens new perspectives on the kinetics of heterogeneous reactions at aqueous interfaces.

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Language(s): eng - English
 Dates: 2016-02-142016-06-142016-06-152016-07-21
 Publication Status: Published in print
 Pages: 7
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1039/C6CP01004K
 Degree: -

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Title: Physical Chemistry Chemical Physics
  Abbreviation : Phys. Chem. Chem. Phys.
Source Genre: Journal
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Publ. Info: Cambridge, England : Royal Society of Chemistry
Pages: 7 Volume / Issue: 18 (27) Sequence Number: - Start / End Page: 18424 - 18430 Identifier: ISSN: 1463-9076
CoNE: /journals/resource/954925272413_1