{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2025,7,30]],"date-time":"2025-07-30T11:20:56Z","timestamp":1753874456947,"version":"3.41.2"},"reference-count":33,"publisher":"AIP Publishing","issue":"14","funder":[{"DOI":"10.13039\/100000001","name":"National Science Foundation","doi-asserted-by":"publisher","award":["CHE-1665271","CHE 2053117","PHY 1734006"],"award-info":[{"award-number":["CHE-1665271","CHE 2053117","PHY 1734006"]}],"id":[{"id":"10.13039\/100000001","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/100000181","name":"Air Force Office of Scientific Research","doi-asserted-by":"publisher","award":["FA9550-15-1-0090"],"award-info":[{"award-number":["FA9550-15-1-0090"]}],"id":[{"id":"10.13039\/100000181","id-type":"DOI","asserted-by":"publisher"}]}],"content-domain":{"domain":["pubs.aip.org"],"crossmark-restriction":true},"short-container-title":[],"published-print":{"date-parts":[[2023,4,14]]},"abstract":"<jats:p>First measurements of internal quantum-state distributions for nitric oxide (NO) evaporating from liquid benzyl alcohol are presented over a broad range of temperatures, performed by liquid-microjet techniques in an essentially collision-free regime, with rotational\/spin\u2013orbit populations in the 2\u03a01\/2,3\/2 manifolds measured by laser-induced fluorescence. The observed rotational distributions exhibit highly linear (i.e., thermal) Boltzmann plots but notably reflect rotational temperatures (Trot) as much as 30\u00a0K lower than the liquid temperature (Tjet). A comparable lack of equilibrium behavior is also noted in the electronic degrees of freedom but with populations corresponding to spin\u2013orbit temperatures (TSO) consistently higher than Trot by \u223c15\u00a0K. These results unambiguously demonstrate evaporation into a non-equilibrium distribution, which, by detailed-balance considerations, predict quantum-state-dependent sticking coefficients for incident collisions of NO at the gas\u2013liquid interface. Comparison and parallels with previous experimental studies of NO thermal desorption and molecular-beam scattering in other systems are discussed, which suggests the emergence of a self-consistent picture for the non-equilibrium dynamics.<\/jats:p>","DOI":"10.1063\/5.0143254","type":"journal-article","created":{"date-parts":[[2023,4,11]],"date-time":"2023-04-11T10:56:18Z","timestamp":1681210578000},"update-policy":"https:\/\/doi.org\/10.1063\/aip-crossmark-policy-page","source":"Crossref","is-referenced-by-count":1,"title":["Non-equilibrium dynamics at the gas\u2013liquid interface: State-resolved studies of NO evaporation from a benzyl alcohol liquid microjet"],"prefix":"10.1063","volume":"158","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-7269-6436","authenticated-orcid":false,"given":"Mikhail","family":"Ryazanov","sequence":"first","affiliation":[{"name":"JILA, National Institute of Standards and Technology and University of Colorado 1 , Boulder, Colorado 80309, USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5365-1120","authenticated-orcid":false,"given":"David J.","family":"Nesbitt","sequence":"additional","affiliation":[{"name":"JILA, National Institute of Standards and Technology and University of Colorado 1 , Boulder, Colorado 80309, USA"},{"name":"Department of Physics, University of Colorado 2 , Boulder, Colorado 80309, USA"},{"name":"Department of Chemistry, University of Colorado 3 , Boulder, Colorado 80309, USA"}],"role":[{"role":"author","vocabulary":"crossref"}]}],"member":"317","published-online":{"date-parts":[[2023,4,11]]},"reference":[{"volume-title":"Statistical Thermodynamics","year":"2000","key":"2024041100012568100_c1"},{"volume-title":"Molecular Reaction Dynamics and Chemical Reactivity","year":"1987","key":"2024041100012568100_c2"},{"key":"2024041100012568100_c3","doi-asserted-by":"publisher","first-page":"667","DOI":"10.1016\/0039-6028(94)90688-2","article-title":"The dynamics of adsorption and desorption","volume":"299\u2013300","year":"1994","journal-title":"Surf. 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