Navegar

Colección

Datos Estadísticas

Artículo

Estamos trabajando para conseguir la versión final de este artículo
Consulte el artículo en la página del editor
Consulte la política de Acceso Abierto del editor

Abstract:

We present results of ring polymer molecular dynamics simulations that shed light on the effects of nuclear quantum fluctuations on tunneling motions in cyclic [H2O]3 and [D2O]3, at the representative temperature of T = 75 K. In particular, we focus attention on free energies associated with two key isomerization processes: The first one corresponds to flipping transitions of dangling OH bonds, between up and down positions with respect to the O-O-O plane of the cluster; the second involves the interchange between connecting and dangling hydrogen bond character of the H-atoms in a tagged water molecule. Zero point energy and tunneling effects lead to sensible reductions of the free energy barriers. Due to the lighter nature of the H nuclei, these modifications are more marked in [H2O]3 than in [D2O]3. Estimates of the characteristic time scales describing the flipping transitions are consistent with those predicted based on standard transition-state-approximation arguments. © 2016 AIP Publishing LLC.

Registro:

Documento: Artículo
Título:Communication: Isotopic effects on tunneling motions in the water trimer
Autor:Videla, P.E.; Rossky, P.J.; Laria, D.
Filiación:Departamento de Quimica Inorganica Analitica y Quimica-Fisica e INQUIMAe, Facultad de Ciencias Exactas y Naturales, Universidad de Buenos Aires, Ciudad Universitaria, Pabellón II, Buenos Aires, 1428, Argentina
Department of Chemistry, Rice University, Houston, TX 77251-1892, United States
Departamento de Física de la Materia Condensada, Comisión Nacional de Energía Atómica, Avenida Libertador 8250, Buenos Aires, 1429, Argentina
Palabras clave:Dangling bonds; Free energy; Hydrogen bonds; Molecules; Quantum electronics; Characteristic time; Isotopic effects; Molecular dynamics simulations; Quantum fluctuation; Transition state approximations; Tunneling effects; Tunneling motion; Zero-point energies; Molecular dynamics
Año:2016
Volumen:144
Número:6
DOI: http://dx.doi.org/10.1063/1.4941701
Título revista:Journal of Chemical Physics
Título revista abreviado:J Chem Phys
ISSN:00219606
CODEN:JCPSA
Registro:https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_00219606_v144_n6_p_Videla

Referencias:

  • Keutsch, F.N., Cruzan, J.D., Saykally, R.J., (2003) Chem. Rev., 103, p. 2533
  • Luzar, A., Chandler, D., (1996) Phys. Rev. Lett., 76, p. 928
  • Pugliano, N., Saykally, R.J., (1992) Science, 257, p. 1937
  • Schutz, M., Burgi, T., Leutwyler, S., Burgi, H.B., (1993) J. Chem. Phys., 99, p. 5228
  • Wales, D.J., (1993) J. Am. Chem. Soc., 115, p. 11180
  • Wales, D.J., (1993) J. Am. Chem. Soc., 115, p. 11191
  • Liu, K., (1994) J. Am. Chem. Soc., 116, p. 3507
  • Suzuki, S., Blake, G.A., (1994) Chem. Phys. Lett., 229, p. 499
  • Liu, K., (1994) Faraday Discuss., 97, p. 35
  • Van Duijneveldt-Van De Rijdt, J.G.C.M., Van Duijneveldt, F.B., (1995) Chem. Phys. Lett., 237, p. 560
  • Burgi, T., Graf, S., Leutwyler, S., Klopper, W., (1995) J. Chem. Phys., 103, p. 1077
  • Gregory, J.K., Clary, D.C., (1995) J. Chem. Phys., 102, p. 7817
  • Liu, K., Brown, M.G., Viant, M.R., Cruzan, J.D., Saykally, R., (1996) Mol. Phys., 89, p. 1373
  • Van Der Avoird, A., Olthof, E.H.T., Wormer, P.E.S., (1996) J. Chem. Phys., 105, p. 8034
  • Walsh, T.R., Wales, D.J., (1996) J. Chem. Soc., Faraday Trans., 92, p. 2505
  • Viant, M.R., (1997) J. Phys. Chem. A, 101, p. 9032
  • Brown, M.G., (1999) J. Chem. Phys., 111, p. 7789
  • Sabo, D., Bacic, Z., Graf, S., Leutwyler, S., (1999) J. Chem. Phys., 111, p. 10727
  • Keutsch, F.N., Karyakin, E.N., Saykally, R.J., Van Der Avoird, A., (2001) J. Chem. Phys., 114, p. 3988
  • Keutsch, F.N., Fellers, R.S., Viant, M.R., Saykally, R.J., (2001) J. Chem. Phys., 114, p. 4005
  • Keutsch, F.N., (2001) J. Chem. Phys., 114, p. 3994
  • Taketsugu, T., Wales, D.J., (2002) Mol. Phys., 100, p. 2793
  • Mandziuk, M., (2004) J. Phys. Chem. A, 108, p. 121
  • Shalashilin, D.V., Child, M.S., Clary, D.C., (2004) J. Chem. Phys., 120, p. 5608
  • Anderson, J.A., Crager, K., Fedoroff, L., Tschumper, G.S., (2004) J. Chem. Phys., 121, p. 11023
  • Takahashi, M., Watanabe, Y., Taketsugu, T., Wales, D.J., (2005) J. Chem. Phys., 123
  • Han, J.-X., (2006) Chem. Phys. Lett., 423, p. 344
  • Czak, G., Kaledin, A.L., Bowman, J.M., (2010) Chem. Phys. Lett., 500, p. 217
  • Richardson, J.O., Althorpe, S.C., Wales, D.J., (2011) J. Chem. Phys., 135
  • Ch'Ng, L.C., Samanta, A.K., Wang, Y., Bowman, J.M., Reisler, H., (2013) J. Phys. Chem. A, 117, p. 7207
  • Craig, I.R., Manolopoulos, D.E., (2004) J. Chem. Phys., 121, p. 3368
  • Habershon, S., Manolopoulos, D.E., Markland, T.E., Miller, T.F., III, (2013) Annu. Rev. Phys. Chem., 64, p. 387
  • Chandler, D., Wolynes, P., (1981) J. Chem. Phys., 74, p. 4078
  • Tuckerman, M.E., Berne, B.J., Martyna, G.J., Klein, M.L., (1993) J. Chem. Phys., 99, p. 2796
  • Babin, V., Leforestier, C., Paesani, F., (2013) J. Chem. Theory Comput., 9, p. 5395
  • Babin, V., Medders, G.R., Paesani, F., (2014) J. Chem. Theory Comput., 10, p. 1599
  • Babin, V., Medders, G.R., Paesani, F., (2014) J. Chem. Theory Comput., 10, p. 2906
  • http://dx.doi.org/10.1063/1.4941701, See supplementary material at E-JCPSA6-144-031607 for additional technical details and a brief discussion about the reliability of the dynamical predictions of the RPMD method; Wang, Y., Shepler, B., Braams, B.J., Bowman, J.M., (2009) J. Chem. Phys., 131, p. 54511
  • Feynman, R.P., (1972) Statistical Mechanics, , Addison-Wesley, Reading, MA
  • Lobaugh, J., Voth, G.A., (1992) Chem. Phys. Lett., 198, p. 311
  • Lobaugh, J., Voth, G.A., (1994) J. Chem. Phys., 100, p. 3039
  • Nichols, A.L., Chandler, D., Singh, Y., Richardson, D.M., (1984) J. Chem. Phys., 81, p. 5109
  • Videla, P.E., Rossky, P.J., Laria, D., (2013) J. Chem. Phys., 139
  • Markland, T.E., Berne, B.J., (2012) Proc. Natl. Acad. Sci. U. S. A., 109, p. 7988
  • Liu, J., (2013) J. Phys. Chem. C, 117, p. 2944
  • Videla, P.E., Rossky, P.J., Laria, D., (2014) J. Phys. Chem. Lett., 4, p. 2375
  • Frenkel, D., Smit, B., (2001) Understanding Molecular Simulation: From Algorithms to Applications, , (Academic Press), Cha 7
  • Craig, I.R., Manolopoulos, D.E., (2005) J. Chem. Phys., 122
  • Craig, I.R., Manolopoulos, D.E., (2005) J. Chem. Phys., 123
  • Luzar, A., (2000) J. Chem. Phys., 113, p. 10663

Citas:

---------- APA ----------
Videla, P.E., Rossky, P.J. & Laria, D. (2016) . Communication: Isotopic effects on tunneling motions in the water trimer. Journal of Chemical Physics, 144(6).
http://dx.doi.org/10.1063/1.4941701
---------- CHICAGO ----------
Videla, P.E., Rossky, P.J., Laria, D. "Communication: Isotopic effects on tunneling motions in the water trimer" . Journal of Chemical Physics 144, no. 6 (2016).
http://dx.doi.org/10.1063/1.4941701
---------- MLA ----------
Videla, P.E., Rossky, P.J., Laria, D. "Communication: Isotopic effects on tunneling motions in the water trimer" . Journal of Chemical Physics, vol. 144, no. 6, 2016.
http://dx.doi.org/10.1063/1.4941701
---------- VANCOUVER ----------
Videla, P.E., Rossky, P.J., Laria, D. Communication: Isotopic effects on tunneling motions in the water trimer. J Chem Phys. 2016;144(6).
http://dx.doi.org/10.1063/1.4941701