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Abstract:

Molecular dynamics experiments have been performed to study equilibrium aspects of the solvation of Coumarin-151 in polar nanoclusters containing Ns = 5, 10, and 50 water and methanol molecules. In small aggregates, both solvents show preferential solvation of the amino group of the solute. Whereas in aqueous aggregates the dye molecule shows a propensity to reside on the cluster surface for all sizes investigated, the 50 methanol cluster exhibits clear signs of more uniform, bulklike solvation. Using nonequilibrium simulations, we also studied the solvation dynamics upon an electronic excitation of the probe. At temperatures close to T = 200 K, small clusters exhibit two well differentiated equilibrium solvation structures for the excited states of the solute. Interconversions between these structures take place in a time scale much longer than the one characterizing the solvation relaxation. In Ns = 5 clusters, the nonequilibrium responses are exclusively dominated by a fast inertial relaxation lasting less that 0.1 ps; for Ns = 50, the relaxations exhibit a slow diffusional regime that dominates the long time behavior as well. The overall response of the largest clusters is also analyzed in terms of linear response theories.

Registro:

Documento: Artículo
Título:Equilibrium and dynamical aspects of solvation of Coumarin-151 in polar nanoclusters
Autor:Tamashiro, A.; Rodriguez, J.; Laria, D.
Filiación:Unidad Actividad Química, Comisión Nacional de Energía Atómica, Avenida Libertador 8250, 1429 Buenos Aires, Argentina
Departamento de Química Inorgánica, Analítica y Química-Física e INQUIMAE, Facultad de Ciencias Exactas y Naturales, Universidad de Buenos Aires, Pabellón II, Ciudad Universitaria, 1428 Buenos Aires, Argentina
Palabras clave:Polar nanoclusters; Agglomeration; Computer simulation; Diffusion; Dyes; Methanol; Molecular dynamics; Nanostructured materials; Organic solvents; Relaxation processes; Surface chemistry; Aromatic compounds
Año:2002
Volumen:106
Número:2
Página de inicio:215
Página de fin:221
DOI: http://dx.doi.org/10.1021/jp012626x
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_n2_p215_Tamashiro

Referencias:

  • Castleman, A.W., Keese, R.G., (1986) Chem. Rev., 86, p. 589
  • Castleman, A.W., Keese, R.G., (1986) Annu. Rev. Phys. Chem., 37, p. 525
  • Castleman, A.W., Keese, R.G., (1988) Science, 241, p. 36
  • Castleman, A.W., Wei, S., (1994) Annu. Rev. Phys. Chem., 45, p. 685
  • Jena, P., Khana, S.N., Rao, B.K., (1992) Physics and Chemistry of Finite Systems: From Clusters to Crystals, , Kluwer: Dordrech, The Netherlands
  • Andersen, H.H., (1997) Small Particles and Inorganic Clusters, , Springer-Verlag: Berlin, Germany
  • Jorgensen, W.L., Severance, D.L., (1993) J. Chem. Phys., 99, p. 4233
  • Dang, L.X., Smith, D.E., (1993) J. Chem. Phys., 99, p. 6950
  • Perera, L., Berkowitz, M.L., (1991) J. Chem. Phys., 95, p. 1954
  • Perera, L., Berkowitz, M.L., (1992) J. Chem. Phys., 96, p. 8288
  • Perera, L., Berkowitz, M.L., (1993) J. Chem. Phys., 99, p. 4236
  • Tobias, D.J., Jungwirth, P., Parrinello, M., (2001) J. Chem. Phys., 114, p. 7036
  • Pryor, B.A., Palmer, P.M., Andrews, P.M., Berger, M.B., Topp, M.R., (1998) J. Phys. Chem. A, 102, p. 3284
  • Palmer, P.M., Chen, Y., Topp, M.R., (2000) Chem. Phys. Lett., 318, p. 440
  • Palmer, P.M., Chen, Y., Topp, M.R., (2000) Chem. Phys. Lett., 321, p. 62
  • Michael, D., Benjamin, I., (2001) J. Chem. Phys., 114, p. 2817
  • Nandi, N., Bagchi, B., (1997) J. Phys. Chem. B, 101, p. 10954
  • Nandi, N., Bagchi, B., Pethig, R., (1992) Annu. Rev. Phys. Chem., 43, p. 177
  • Nandi, N., Bhattacharyya, K., Bagchi, B., (2000) Chem. Rev., 100, p. 2013
  • Bagchi, B., (1989) Annu. Rev. Phys. Chem., 40, p. 115
  • Bagchi, B., Chandra, A., (1991) Adv. Chem. Phys., 80, p. 1
  • Maroncelli, M., (1993) J. Mol. Liq., 57, p. 1
  • Maroncelli, M., Kumar, P.V., Papazyan, A., Homg, M.L., Rosenthal, S.J., Fleming, G.R., (1994) Ultrafast Reaction Dynamics and Solvent Effects, , Gandel, Y., Rossky, P.J., Eds.; American Institute of Physics: New York
  • Stratt, R.M., Maroncelli, M., (1996) J. Phys. Chem., 100, p. 12981
  • Fleming, G.R., (1986) Chemical Applications of Ultrafast Spectroscopy, , Oxford University Press: New York
  • Simon, J.D., (1988) Acc. Chem. Res., 21, p. 128
  • Landayi, B.M., (2000) Theoretical Methods in Condensed Phase Chemistry, , Schwartz, S.D., Ed.; Kluwer Academic Publishers: Dordrech, The Netherlands
  • Liotard, D.A., Healy, E.F., Ruiz, J.M., Dewar, M.J.S., (1989) QCPE Bull., 9, p. 123
  • AMPAC, version 2.1 Quantum Chemistry Program Exchange program, 506
  • McCarthy, P.K., Blanchard, G.J., (1993) J. Phys. Chem., 97, p. 12205
  • Rechthaler, K., Köhler, G., (1994) Chem. Phys., 189, p. 99
  • Kumar, P.V., Maroncelli, M., (1995) J. Chem. Phys., 103, p. 3038
  • Reynolds, L., Gardecki, J.A., Frankland, S.J.V., Horng, M.L., Maroncelli, M., (1996) J. Phys. Chem., 100, p. 10337
  • Berendsen, H.J.C., Postma, J.P.M., Von Gunsteren, W.F., Hermans, J., (1981) Intermolecular Forces, , Reidel: Dordrecht, The Netherlands
  • Jorgensen, W.L., (1986) J. Phys. Chem., 90, p. 1276
  • note; Allen, M.P., Tildesley, D.J., (1987) Computer Simulations of Liquids, , Clarendon Press: Oxford, U.K
  • Ryckaert, J.-P., Ciccotti, G., Berendsen, H.J.C., (1977) J. Comput. Phys., 23, p. 327
  • Chandler, D., (1987) An Introduction to Modern Statistical Mechanics, , Oxford University Press: New York, Chapter 8
  • Ladanyi, B., Stratt, R.M., (1995) J. Phys. Chem., 99, p. 2502
  • Fonseca, T., Ladanyi, B.M., (1991) J. Chem. Phys., 2116, p. 95
  • note

Citas:

---------- APA ----------
Tamashiro, A., Rodriguez, J. & Laria, D. (2002) . Equilibrium and dynamical aspects of solvation of Coumarin-151 in polar nanoclusters. Journal of Physical Chemistry A, 106(2), 215-221.
http://dx.doi.org/10.1021/jp012626x
---------- CHICAGO ----------
Tamashiro, A., Rodriguez, J., Laria, D. "Equilibrium and dynamical aspects of solvation of Coumarin-151 in polar nanoclusters" . Journal of Physical Chemistry A 106, no. 2 (2002) : 215-221.
http://dx.doi.org/10.1021/jp012626x
---------- MLA ----------
Tamashiro, A., Rodriguez, J., Laria, D. "Equilibrium and dynamical aspects of solvation of Coumarin-151 in polar nanoclusters" . Journal of Physical Chemistry A, vol. 106, no. 2, 2002, pp. 215-221.
http://dx.doi.org/10.1021/jp012626x
---------- VANCOUVER ----------
Tamashiro, A., Rodriguez, J., Laria, D. Equilibrium and dynamical aspects of solvation of Coumarin-151 in polar nanoclusters. J Phys Chem A. 2002;106(2):215-221.
http://dx.doi.org/10.1021/jp012626x