{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2025,10,14]],"date-time":"2025-10-14T01:11:06Z","timestamp":1760404266066,"version":"3.41.2"},"reference-count":64,"publisher":"AIP Publishing","issue":"7","content-domain":{"domain":["pubs.aip.org"],"crossmark-restriction":true},"short-container-title":[],"published-print":{"date-parts":[[2005,8,15]]},"abstract":"<jats:p>Far-infrared (FIR) and mid-infrared (MIR) profiles of D2O infinitely dilute in supercritical CO2 have been studied using molecular-dynamics simulations. For this purpose, we have proposed an intermolecular potential model taking implicitly into account electron donor-acceptor (EDA) interactions between water and CO2 evaluated from ab initio calculations of the intermolecular potential-energy surface (IPS). Interaction-induced dipole mechanisms have been also taken into account in addition to the water permanent dipole to evaluate the simulated FIR profiles of water and CO2 polarizable molecules. They were found to play a minor role in the genesis of the FIR profiles of water\/CO2 under supercritical conditions. The analysis of the reorientational dynamics of D2O shows that the rotational dynamics of water is weakly anisotropic due to the EDA interactions which affect more specifically the reorientational motions of the C2 symmetry axis of solute. These results have been used to assess the contribution of the vibrational relaxation in the experimental mid-infrared profiles associated with the \u03bd1 symmetric and \u03bd3 antisymmetric stretching and \u03bd2 bending modes of D2O. It was found that the rotational dynamics mainly contribute to the broadening of the infrared (IR) profiles. Nevertheless, the vibrational processes play a role in the frequency shifts of the band centers and the relative intensity enhancements of the \u03bd1 and \u03bd3 modes of D2O. In particular, the EDA interactions between water and CO2 lead to the appearance of a well-defined IR band of the \u03bd1 mode of D2O. Finally, a comparison with another model taking only into account dipole-quadrupole electrostatic interactions between water and CO2 molecules clearly reveals that EDA interactions have to be considered to reproduce both MIR and FIR measurements. From this point of view CO2 can be classified on a hydrophilic solvent scale based upon the solubility criterion as an intermediate solvent between \u201cinert\u201d xenon and carbon tetrachloride.<\/jats:p>","DOI":"10.1063\/1.1953561","type":"journal-article","created":{"date-parts":[[2005,8,19]],"date-time":"2005-08-19T22:00:46Z","timestamp":1124488846000},"update-policy":"https:\/\/doi.org\/10.1063\/aip-crossmark-policy-page","source":"Crossref","is-referenced-by-count":20,"title":["Infrared and molecular-dynamics studies of the rotational dynamics of water highly diluted in supercritical CO2"],"prefix":"10.1063","volume":"123","author":[{"given":"Y.","family":"Danten","sequence":"first","affiliation":[{"name":"Universit\u00e9 Bordeaux I Laboratoire de Physico-Chimie Mol\u00e9culaire, Unite Mixte de Recherche (UMR) Centre National de la Recherche (CNRS) 5803, , 351 Cours de la Lib\u00e9ration, 33405 Talence, France"}]},{"given":"T.","family":"Tassaing","sequence":"additional","affiliation":[{"name":"Universit\u00e9 Bordeaux I Laboratoire de Physico-Chimie Mol\u00e9culaire, Unite Mixte de Recherche (UMR) Centre National de la Recherche (CNRS) 5803, , 351 Cours de la Lib\u00e9ration, 33405 Talence, France"}]},{"given":"M.","family":"Besnard","sequence":"additional","affiliation":[{"name":"Universit\u00e9 Bordeaux I Laboratoire de Physico-Chimie Mol\u00e9culaire, Unite Mixte de Recherche (UMR) Centre National de la Recherche (CNRS) 5803, , 351 Cours de la Lib\u00e9ration, 33405 Talence, France"}]}],"member":"317","published-online":{"date-parts":[[2005,8,23]]},"reference":[{"key":"2023080123081865000_c1","doi-asserted-by":"publisher","first-page":"3777","DOI":"10.1021\/ja00350a004","volume":"105","year":"1983","journal-title":"J. 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