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Abstract:

We have carried out path integral-molecular dynamics simulations to describe microscopic details of excess electrons in supercritical water over a wide range of solvent densities, ρw, along the T = 645 K isotherm. The well-tested simple-point charge model for water was used. The transition from localized to quasifree states described in terms of the electron spatial extent is observed in the vicinity of ρw = 0.15 g cm-3. For smaller densities, the electron undergoes quantum tunneling through nearest neighboring water molecules. The groundstate absorption spectrum exhibits significant red shifts in the absorption maxima with decreasing density, showing reasonable agreement with recent pulse radiolysis measurements.

Registro:

Documento: Artículo
Título:Path integral-molecular dynamics study of electronic states in supercritical water
Autor:Laria, D.; Skaf, M.S.
Filiación:Unidad Actividad Química, Comision Nacional de Energia Atomica, Avenida Libertador 8250, 1429 Buenos Aires, Argentina
Departamento de QIAQFI, Ciudad Universitaria, Universidad de Buenos Aires, Pabellón II, 1428 Buenos Aires, Argentina
Instituto de Química, Universidade Estadual de Campinas, Cx. P. 6154, Campinas, SP 13083-970, Brazil
Palabras clave:Density of liquids; Electronic structure; Ground state; Molecules; Radiolysis; Solvents; Supercritical fluids; Water; Supercritical water; Molecular dynamics
Año:2002
Volumen:106
Número:35
Página de inicio:8066
Página de fin:8069
DOI: http://dx.doi.org/10.1021/jp021278b
Título revista:Journal of Physical Chemistry A
Título revista abreviado:J Phys Chem A
ISSN:10895639
CODEN:JPCAF
Registro:https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_10895639_v106_n35_p8066_Laria

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Citas:

---------- APA ----------
Laria, D. & Skaf, M.S. (2002) . Path integral-molecular dynamics study of electronic states in supercritical water. Journal of Physical Chemistry A, 106(35), 8066-8069.
http://dx.doi.org/10.1021/jp021278b
---------- CHICAGO ----------
Laria, D., Skaf, M.S. "Path integral-molecular dynamics study of electronic states in supercritical water" . Journal of Physical Chemistry A 106, no. 35 (2002) : 8066-8069.
http://dx.doi.org/10.1021/jp021278b
---------- MLA ----------
Laria, D., Skaf, M.S. "Path integral-molecular dynamics study of electronic states in supercritical water" . Journal of Physical Chemistry A, vol. 106, no. 35, 2002, pp. 8066-8069.
http://dx.doi.org/10.1021/jp021278b
---------- VANCOUVER ----------
Laria, D., Skaf, M.S. Path integral-molecular dynamics study of electronic states in supercritical water. J Phys Chem A. 2002;106(35):8066-8069.
http://dx.doi.org/10.1021/jp021278b