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  Molecular Arrangement of a Mixture of Organosulfur Surfactants at the Aqueous Solution–Vapor Interface Studied by Photoelectron Intensity and Angular Distribution Measurements and Molecular Dynamics Simulations

Lewis, T. L., Winter, B., Thurmer, S., Seidel, R., Stephansen, A. B., Freites, J. A., et al. (2019). Molecular Arrangement of a Mixture of Organosulfur Surfactants at the Aqueous Solution–Vapor Interface Studied by Photoelectron Intensity and Angular Distribution Measurements and Molecular Dynamics Simulations. The Journal of Physical Chemistry C, 123(13), 8160-8170. doi:10.1021/acs.jpcc.8b08260.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0002-9C51-3 Version Permalink: http://hdl.handle.net/21.11116/0000-0003-684E-2
Genre: Journal Article

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 Creators:
Lewis, Tanza Lee1, Author
Winter, Bernd2, Author              
Thurmer, Stephan3, Author
Seidel, Robert4, Author
Stephansen, Anne B.2, Author              
Freites, J. Alfredo1, Author
Tobias, Douglas J.1, Author
Hemminger, John C.1, 2, Author
Affiliations:
1Department of Chemistry, University of California, Irvine, California 92697, USA, ou_persistent22              
2Molecular Physics, Fritz Haber Institute, Max Planck Society, ou_634545              
3Department of Chemistry, Graduate School of Science, Kyoto University, Kitashirakawa-Oiwakecho, Sakyo-Ku, Kyoto 606-8502, Japan , ou_persistent22              
4Division of Renewable Energy, Helmholtz-Zentrum Berlin, Albert-Einstein-Strasse 15, D-12489 Berlin, Germany, ou_persistent22              

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 Abstract: Photoelectron angular distributions (PADs) from aqueous solution surfaces reveal details on the spatial arrangement of solute molecules at the solution – gas-phase interface. This is demonstrated here for mixed equimolar aqueous solutions of dimethyl sulfoxide / dimethyl sulfone ((CH3)2SO) / (CH3)2S)O2, and dimethyl sulfoxide / dimethyl sulfite ((CH3)2SO / (CH3)2SO3), all molecules having a propensity to reside near the solution surface. Although the surface-active molecules coexist at the surface, (CH3)2SO2 yields a more intense sulfur 2p surface photoelectron signal than (CH3)2SO, and for (CH3)2SO3 the effect is even larger. To understand this behavior we have for one of the solutions mixtures, (CH3)2SO / (CH3)2SO2, performed PAD measurements. Surprisingly, both molecules exhibit almost identical PADs implying that the emitted photoelectrons have experienced similar (limited) amount of scattering interactions. Hence, the molecules reside at the same distance with respect to the solution – vacuum interface rather than (CH3)2SO2 being closer to the surface than (CH3)2SO, as one may have assumed based on the relative photoelectron signal intensities. Instead, the relative surface and bulk concentrations of the two compounds differ. We also report S 2p photoelectron spectra from single-component dimethyl sulfide, (CH3)2S, aqueous solutions measured at a single detection angle. The exceptionally large surface propensity of (CH3)2S is recognized by a narrow, gas-phase-like photoelectron spectrum revealing that (CH3)2S experiences very little hydration interactions. Experimentally observed trends in surface activity for the different molecules, which are complemented here by molecular dynamics simulations, agree with findings obtained with other surface sensitive techniques. New information on the surface structure of mixed solutions is uniquely obtained from the anisotropic angular distributions of the photoelectrons.

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Language(s): eng - English
 Dates: 2018-11-202018-08-042018-11-272019-04-04
 Publication Status: Published in print
 Pages: 11
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1021/acs.jpcc.8b08260
 Degree: -

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Title: The Journal of Physical Chemistry C
  Alternative Title : J. Phys. Chem. C
Source Genre: Journal
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Publ. Info: Washington, D.C. : American Chemical Society
Pages: - Volume / Issue: 123 (13) Sequence Number: - Start / End Page: 8160 - 8170 Identifier: n.a.: https://pure.mpg.de/cone/journals/resource/954926947766