dc.creatorVidela, Pablo Ernesto
dc.creatorRossky, Peter J.
dc.creatorLaria, Daniel Hector
dc.date.accessioned2017-12-27T20:06:45Z
dc.date.accessioned2018-11-06T12:13:34Z
dc.date.available2017-12-27T20:06:45Z
dc.date.available2018-11-06T12:13:34Z
dc.date.created2017-12-27T20:06:45Z
dc.date.issued2014-06
dc.identifierVidela, Pablo Ernesto; Laria, Daniel Hector; Rossky, Peter J.; Surface Isotope Segregation as a Probe of Temperature in Water Nanoclusters; American Chemical Society; Journal of Physical Chemistry Letters; 5; 13; 6-2014; 2375-2379
dc.identifier1948-7185
dc.identifierhttp://hdl.handle.net/11336/31739
dc.identifierCONICET Digital
dc.identifierCONICET
dc.identifier.urihttp://repositorioslatinoamericanos.uchile.cl/handle/2250/1864520
dc.description.abstractUsing ring polymer molecular dynamics simulations, we examine equilibrium and dynamical characteristics of solid-like, aqueous clusters that combine isotopic mixtures of HDO dilute in H2O, at temperatures intermediate between 50 and 175 K. In particular, we focus attention on the relative thermodynamic stabilities of the two isotopes at dangling hydrogen bond sites. The water octamer is analyzed as a reference system. For this aggregate, decreasing temperature yields a gradual stabilization of the light isotope at dangling sites in molecules acting as single-donor-double-acceptors of hydrogen bonds. At T ∼ 50 K, the imbalance between the corresponding quantum kinetic energies leads to a free energy difference between dangling and hydrogen bonded sites of the order of ∼2kBT. Similar free energy differences were found at dangling sites in Nw = 50 water clusters. The extent of the H/D segregation can be adequately monitored by modifications in the peak intensity of the high frequency shoulder of the stretching band of the infrared spectrum. These signals, in turn, represent a potential experimental signature of the elusive temperature of clusters in molecular beams.
dc.languageeng
dc.publisherAmerican Chemical Society
dc.relationinfo:eu-repo/semantics/altIdentifier/doi/http://dx.doi.org/10.1021/jz501043k
dc.relationinfo:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/10.1021/jz501043k
dc.rightshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.rightsinfo:eu-repo/semantics/restrictedAccess
dc.subjectPATH INTEGRALS
dc.subjectISOTOPE EFFECTS
dc.subjectNUCLEAR QUANTUM FLUCTUATIONS
dc.subjectRING POLYMER MOLECULAR DYNAMICS
dc.titleSurface Isotope Segregation as a Probe of Temperature in Water Nanoclusters
dc.typeArtículos de revistas
dc.typeArtículos de revistas
dc.typeArtículos de revistas


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