Title
Origin of abnormally sharp features in collision-induced spectra of cryosolutions Origin of abnormally sharp features in collision-induced spectra of cryosolutions
Author
Faculty/Department
Faculty of Sciences. Chemistry
Publication type
article
Publication
New York, N.Y. ,
Subject
Physics
Chemistry
Source (journal)
The journal of chemical physics. - New York, N.Y.
Volume/pages
143(2015) :4 , 10 p.
ISSN
0021-9606
0021-9606
Article Reference
044508
Carrier
E-only publicatie
Target language
English (eng)
Full text (Publishers DOI)
Affiliation
University of Antwerp
Abstract
A weak, paradoxically narrow resonance feature (shortly, the r-line) near the O-2 fundamental frequency in the collision-induced absorption spectrum of oxygen dissolved in liquid argon and liquid nitrogen (T = 89 K) is resolved for the first time. An accurate band shape fitting routine to separate the r-line from the by-far more intense diffuse background and to study its behavior versus the oxygen mole fraction x which ranged from 0.03 up to 0.23 has been elaborated. At small x (less than or similar to 0.07), the r-line intensitywas found to scale as x(2) leaving no doubt that it is due to the solute-solute (O-2-O-2) interactions. In line with our results on the pH(2)-LNe cryosystem [Herrebout, Phys. Rev. Lett. 101, 093001 (2008)], the Lorentzian r-line shape and its extraordinary sharpness (half width at half height approximate to 1 cm(-1)) are indicative of the motional narrowing of the relative solute-solute translational spectrum. As x is further raised, ternary solute-solute interactions impede the r-line growth in the O-2-LAr spectrum because of the cancellation effect [J. Van Kranendonk, Physica 23, 825 (1957)]. Theoretical arguments are given that multiple interactions between the solutes should finally destroy the solute-solute induced r-line when the mixed solution approaches the limit of the pure liquid (x = 1). Interestingly, the nonbinary effects are too weak to appreciably affect the quadratic r-line scaling in the O-2-LN2 cryosystem which persists up to x = 0.23. It is emphasized that studies of the resonant features in the collision-induced spectra of binary cryosolutions open up unique opportunities to spectroscopically trace the microscopic-scale diffusion. (C) 2015 AIP Publishing LLC.
E-info
http://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000358929100052&DestLinkType=RelatedRecords&DestApp=ALL_WOS&UsrCustomerID=ef845e08c439e550330acc77c7d2d848
http://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000358929100052&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=ef845e08c439e550330acc77c7d2d848
Full text (open access)
https://repository.uantwerpen.be/docman/irua/35f021/aa42b370.pdf
Handle