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- W1599252336 abstract "The present work is concerned with the electronic structure ofliquid water and aqueous solutions as inferred from photoemission.Of central focus is a better understanding of the effect ofhydrogen bonding. A specially designed liquid microjet, providinga free liquid surface in vacuum, enables the detection ofphotoelectrons from highly volatile liquid surfaces. Incombination with high-intensity synchrotron light from anundulator (U125/1 at BESSY II) for photoexcitation, in the 30-140eV range, electron binding energies of the liquid constituents aredetermined. This includes energies of liquid water's valenceorbitals as well as of a number of solvated ions, particularlyalkali cations and halide anions. Liquid-specific energy losses ofphotoelectrons will be also addressed. Measured binding energiesfor liquid water, which are about 1.4 eV lower than in the gasphase, are discussed in terms of surface dipoles, polarizationscreening after photoionization, and hydrogen bonding. Therelative signal decrease of the H_2O 1b_2orbital results from a change of the respective anisotropyparameter β. Broadening of the 3a_1 orbitalfeature correlates with peak splitting. Both effects are due tohydrogen bonding. Hydrogen bonding also plays a central role inion solvation. Here, a number of salt solutions (XY for X = Li,Na, K, Cs, and Y = Cl, Br, I; CaI_2; MgCl_2;Na_2CO_3; Na_4[Fe(CN)_6];K_3[Fe(CN)_6]; But_4NI;Prop_4NI), are systematically investigated byphotoemission in order to address various aspects of ionicsolvation. One focus is on correlating measured electron bindingenergies, obtained for different counter ions and concentrations,with solvation shell structural details. Experimental bindingenergies, which are considerably different from gas-phase values,are discussed within a dielectric continuum model and also withrespect to comparative measurements performed for some gas-phasealkali halides. The other important topic, regarding photoemissionfrom aqueous salt solutions, was the structure of thesolution/vacuum interface. Two processes have been investigated,ion depletion near the solution surface for high-concentration NaIsolutions, and the surface segregation of hydrophobictetrabutylammoiumiodide, But_4NI (and also the smallerProp_4NI). The former aspect is related to the questionif for high NaI concentration surface ions are incompletelysolvated, with the possibility of anion surface excess. Solutionsof surface-active But_4N^+I^-provide the opportunity to investigate the formation of asegregation monolayer (electric double layer) at the liquidsurface. The resulting molecular surface dipoles correlate withspectral shifts of the photoemission features, due to workfunction changes of the solution as a function of the saltconcentration.%%%%In der vorliegenden Arbeit wird die elektronische Struktur vonflussigem Wasser sowie von wassrigen Salzlosungenmittels Photoemission untersucht, um insbesondere die Bedeutungder…" @default.
- W1599252336 created "2016-06-24" @default.
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- W1599252336 date "2003-01-01" @default.
- W1599252336 modified "2023-09-23" @default.
- W1599252336 title "Photoelectron Spectroscopy of Liquid Water and Aqueous Solutions in Free Microjets Using Synchrotron Radiation" @default.
- W1599252336 hasPublicationYear "2003" @default.
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