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Abstract:

We present a transition path sampling study of the dynamics of isomerization between the S4 and the D2d cubic structures of the water octamer. The reaction mechanism involves a transition state characterized by a distorted face exhibiting a diagonal hydrogen bond. Analysis of an ensemble of trajectories shows that the isomerization requires concerted flips of double proton donor molecules and the interchange between dangling and bonding hydrogens in single proton donor molecules. At a total energy E = -60.5 kcal/mol, we calculated that the characteristic time for the interconversion is of the order of milliseconds. We have also investigated pathways for the melting transition at temperatures T ≈ 200 K. We find that the barrier for solid-liquid interconversions never exceeds 2kBT measured from the liquid side. Such transitions between liquid and solid do not involve the passage over an energetic barrier; instead, the stabilization of the liquid phase is the result of a cancellation between energetic and entropic contributions. © 2001 American Chemical Society.

Registro:

Documento: Artículo
Título:Dynamical aspects of isomerization and melting transitions in [H2O]8
Autor:Laria, D.; Rodriguez, J.; Dellago, C.; Chandler, D.
Filiación:Unidad Actividad Química, Comisión Nacional de Energia Atómica, Avenida Libertador 8250, 1429 Capital Federal, Argentina
Departamento de Química Inorgánica, Analítica y Química-Física e INQUIMAE, Pabellón II, 1428, Capital Federal, Argentina
Department of Chemistry, University of Rochester, Rochester, NY 14627, United States
Department of Chemistry, Kenneth S. Pitzer Center for Theoretical Chemistry, University of California, Berkeley, CA 94720, United States
Palabras clave:Melting transitions; Entropy; Hydrogen bonds; Melting; Molecules; Protons; Reaction kinetics; Thermal effects; Water; Isomerization
Año:2001
Volumen:105
Número:12
Página de inicio:2646
Página de fin:2651
Título revista:Journal of Physical Chemistry A
Título revista abreviado:J. Phys. Chem. A
ISSN:10895639
Registro:https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_10895639_v105_n12_p2646_Laria

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Citas:

---------- APA ----------
Laria, D., Rodriguez, J., Dellago, C. & Chandler, D. (2001) . Dynamical aspects of isomerization and melting transitions in [H2O]8. Journal of Physical Chemistry A, 105(12), 2646-2651.
Recuperado de https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_10895639_v105_n12_p2646_Laria [ ]
---------- CHICAGO ----------
Laria, D., Rodriguez, J., Dellago, C., Chandler, D. "Dynamical aspects of isomerization and melting transitions in [H2O]8" . Journal of Physical Chemistry A 105, no. 12 (2001) : 2646-2651.
Recuperado de https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_10895639_v105_n12_p2646_Laria [ ]
---------- MLA ----------
Laria, D., Rodriguez, J., Dellago, C., Chandler, D. "Dynamical aspects of isomerization and melting transitions in [H2O]8" . Journal of Physical Chemistry A, vol. 105, no. 12, 2001, pp. 2646-2651.
Recuperado de https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_10895639_v105_n12_p2646_Laria [ ]
---------- VANCOUVER ----------
Laria, D., Rodriguez, J., Dellago, C., Chandler, D. Dynamical aspects of isomerization and melting transitions in [H2O]8. J. Phys. Chem. A. 2001;105(12):2646-2651.
Available from: https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_10895639_v105_n12_p2646_Laria [ ]