DOI: 10.1126/science.1106525. Electron Spectroscopy of Aqueous Solution Interfaces Reveals Surface Enhancement of Halides

Electron Spectroscopy of Aqueous Solution Interfaces Reveals Surface Enhancement of Halides

10.1126/science.1106525

Crossref journal-article

American Association for the Advancement of Science (AAAS)

Science (221)

Abstract

It has been suggested that enhanced anion concentrations at the liquid/vapor interface of airborne saline droplets are important to aerosol reactions in the atmosphere. We report ionic concentrations in the surface of such solutions. Using x-ray photoelectron spectroscopy operating at near ambient pressure, we have measured the composition of the liquid/vapor interface for deliquesced samples of potassium bromide and potassium iodide. In both cases, the surface composition of the saturated solution is enhanced in the halide anion compared with the bulk of the solution. The enhancement of anion concentration is more dramatic for the larger, more polarizable iodide anion. By varying photoelectron kinetic energies, we have obtained depth profiles of the liquid/vapor interface. Our results are in good qualitative agreement with classical molecular dynamics simulations. Quantitative comparison between the experiments and the simulations indicates that the experimental results exhibit more interface enhancement than predicted theoretically.

Bibliography

Ghosal, S., Hemminger, J. C., Bluhm, H., Mun, B. S., Hebenstreit, E. L. D., Ketteler, G., Ogletree, D. F., Requejo, F. G., & Salmeron, M. (2005). Electron Spectroscopy of Aqueous Solution Interfaces Reveals Surface Enhancement of Halides. Science, 307(5709), 563â566.

Authors 9

Sutapa Ghosal (first)
John C. Hemminger (additional)
Hendrik Bluhm (additional)
Bongjin Simon Mun (additional)
Eleonore L. D. Hebenstreit (additional)
Guido Ketteler (additional)
D. Frank Ogletree (additional)
Felix G. Requejo (additional)
Miquel Salmeron (additional)

References 25 Referenced 575

10.1126/science.288.5464.301
S. W. Hunt et al., J. Phys. Chem. A108, 11559 (2004). (10.1021/jp0467346) / J. Phys. Chem. A (2004)
10.1038/28584
R. Sander et al., Atmos. Chem. Phys.3, 1301 (2003). (10.5194/acp-3-1301-2003) / Atmos. Chem. Phys. (2003)
C. W. Spicer et al., Atmos. Environ.36, 2721 (2002). (10.1016/S1352-2310(02)00125-5) / Atmos. Environ. (2002)
S. Ghosal, A. Shbeeb, J. C. Hemminger, Geophys. Res. Lett.27, 1879 (2000). (10.1029/2000GL011381) / Geophys. Res. Lett. (2000)
10.1038/334138a0
L. A. Barrie, U. Platt, Tellus49B, 450 (1997). (10.3402/tellusb.v49i5.15984) / Tellus (1997)
J. H. Hu et al., J. Phys. Chem.99, 8768 (1995). (10.1021/j100021a050) / J. Phys. Chem. (1995)
P. Jungwirth, D. J. Tobias, J. Phys. Chem. B105, 10468 (2001). / J. Phys. Chem. B (2001)
10.1021/jp020242g
10.1126/science.1089801
D. Liu, G. Ma, L. M. Levering, H. C. Allen, J. Phys. Chem. B108, 2252 (2004). (10.1021/jp036169r) / J. Phys. Chem. B (2004)
E. A. Raymond, G. L. Richmond, J. Phys. Chem. B108, 5051 (2004). (10.1021/jp037725k) / J. Phys. Chem. B (2004)
P. B. Petersen et al., Chem. Phys. Lett.397, 46 (2004). (10.1016/j.cplett.2004.08.048) / Chem. Phys. Lett. (2004)
R. Weber et al., J. Phys. Chem. B108, 4729 (2004). (10.1021/jp030776x) / J. Phys. Chem. B (2004)
10.1063/1.1512336
The experiments were carried out at the Berkeley Advanced Light Source in beamlines 9.3.2 and 11.0.2. Salt crystals ∼2 mm thick and ∼5mm 2 were mounted on a cooled copper substrate. They were cleaved in situ or just before introduction into the vacuum system. Vapor from degassed Milli-Q water (Millipore Corporation Billerica MA) was introduced through a leak valve and monitored with a capacitance nanometer absolute pressure gauge.
J. J. Yeh, I. Lindau, At. Data Nuc. Data Tables32, 1 (1985). (10.1016/0092-640X(85)90016-6) / At. Data Nuc. Data Tables (1985)
W. F. Linke Solubilities Inorganic and Metal Organic Compounds: A Compilation of Solubility Data from the Periodical Literature (Van Nostrand Princeton NJ ed. 4 1958) vol. 2.
The probability that a photoelectron generated below the sample surface will contribute to the well-defined photoelectron peak for an element depends on the IMFP of the electron Γ(KE) which is a function of its kinetic energy. The photoelectron signal predicted from the classical MD simulations is then calculated with the convolution integral \batchmode \documentclass[fleqn 10pt legalpaper]{article} \usepackage{amssymb} \usepackage{amsfonts} \usepackage{amsmath} \pagestyle{empty} \begin{document} \(S={{\int}}e^{\frac{-z}{{\Gamma}(KE)}}{\bullet}D(z)dz\) \end{document} where z is the distance into the sample from the vapor/liquid interface and D ( z ) is the density of the particular element as a function of z from the simulation.
C. J. Powell A. Jablonski NIST Electron Inelastic-Mean-Free-Path Database Version 1.1 (National Institute of Standards and Technology Gaithersburg MD 2000).
M. Roeselová Department of Molecular Modeling Institute of Organic Chemistry and Biochemistry Academy of Sciences of the Czech Republic private communication.
L. X. Dang, T. M. Chang, J. Phys. Chem. B106, 235 (2002). (10.1021/jp011853w) / J. Phys. Chem. B (2002)
Supported by the Director Office of Science Office of Basic Energy Science U.S. Department of Energy under contract no. DE-AC03-76SD00098 and DE-AC03-76SF00098. J.C.H. and S.G. thank the NSF for support (grants 0080806 0209719 and 0431312). G.K. thanks the Alexander von Humboldt Foundation for support. F.G.R. thanks the Consejo Nacional de Investigaciones Científicas y Técnicas (Argentina). The authors thank D. Tobias and P. Jungwirth for providing the numerical data from their classical MD simulations of 1.2 M alkali-halide solutions which were used for comparison with the experiments. We thank M. Roeselová for discussion of the preliminary results of classical MD simulations of higher concentration KBr solutions at –10°C. S.G. and M.S. thank M. Luna for assistance in the initial phase of this project and J. Newberg for help procuring the single-crystal samples. S.G. also thanks H. Liu for experimental help in the initial phase of these experiments. E. Wong's help and expertise with the technical aspects of the experiments are greatly appreciated.

Dates

Type	When
Created	20 years, 7 months ago (Jan. 20, 2005, 4:11 p.m.)
Deposited	1 year, 7 months ago (Jan. 9, 2024, 9:26 p.m.)
Indexed	2 days, 2 hours ago (Aug. 29, 2025, 6:01 a.m.)
Issued	20 years, 7 months ago (Jan. 28, 2005)
Published	20 years, 7 months ago (Jan. 28, 2005)
Published Print	20 years, 7 months ago (Jan. 28, 2005)

Funders 0

None

BibTeX

@article{Ghosal_2005, title={Electron Spectroscopy of Aqueous Solution Interfaces Reveals Surface Enhancement of Halides}, volume={307}, ISSN={1095-9203}, url={http://dx.doi.org/10.1126/science.1106525}, DOI={10.1126/science.1106525}, number={5709}, journal={Science}, publisher={American Association for the Advancement of Science (AAAS)}, author={Ghosal, Sutapa and Hemminger, John C. and Bluhm, Hendrik and Mun, Bongjin Simon and Hebenstreit, Eleonore L. D. and Ketteler, Guido and Ogletree, D. Frank and Requejo, Felix G. and Salmeron, Miquel}, year={2005}, month=jan, pages={563–566} }

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