Artículo

Morzan, U.N.; Ramírez, F.F.; González Lebrero, M.C.; Scherlis, D.A."Electron transport in real time from first-principles" (2017) Journal of Chemical Physics. 146(4)
Estamos trabajando para incorporar este artículo al repositorio
Consulte el artículo en la página del editor
Consulte la política de Acceso Abierto del editor

Abstract:

While the vast majority of calculations reported on molecular conductance have been based on the static non-equilibrium Green’s function formalism combined with density functional theory (DFT), in recent years a few time-dependent approaches to transport have started to emerge. Among these, the driven Liouville-von Neumann equation [C. G. Sánchez et al., J. Chem. Phys. 124, 214708 (2006)] is a simple and appealing route relying on a tunable rate parameter, which has been explored in the context of semi-empirical methods. In the present study, we adapt this formulation to a density functional theory framework and analyze its performance. In particular, it is implemented in an efficient all-electron DFT code with Gaussian basis functions, suitable for quantum-dynamics simulations of large molecular systems. At variance with the case of the tight-binding calculations reported in the literature, we find that now the initial perturbation to drive the system out of equilibrium plays a fundamental role in the stability of the electron dynamics. The equation of motion used in previous tight-binding implementations with massive electrodes has to be modified to produce a stable and unidirectional current during time propagation in time-dependent DFT simulations using much smaller leads. Moreover, we propose a procedure to get rid of the dependence of the current-voltage curves on the rate parameter. This method is employed to obtain the current-voltage characteristic of saturated and unsaturated hydrocarbons of different lengths, with very promising prospects. © 2017 Author(s).

Registro:

Documento: Artículo
Título:Electron transport in real time from first-principles
Autor:Morzan, U.N.; Ramírez, F.F.; González Lebrero, M.C.; Scherlis, D.A.
Filiación:Departamento de Química Inorgánica, Analítica y Química Física/INQUIMAE, Facultad de Ciencias Exactas y Naturales, Universidad de Buenos Aires, Ciudad Universitaria, Pab. II, Buenos Aires, C1428EHA, Argentina
Palabras clave:Bins; Calculations; Current voltage characteristics; Dynamics; Electron transport properties; Equations of motion; Quantum theory; Current voltage curve; Gaussian basis functions; Initial perturbation; Molecular conductance; Quantum dynamics simulation; Semi-empirical methods; Tight-binding calculations; Unsaturated hydrocarbons; Density functional theory
Año:2017
Volumen:146
Número:4
DOI: http://dx.doi.org/10.1063/1.4974095
Handle:http://hdl.handle.net/20.500.12110/paper_00219606_v146_n4_p_Morzan
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_v146_n4_p_Morzan

Referencias:

  • Nitzan, A., Ratner, M.A., (2003) Science, 300, p. 1384
  • Di Ventra, M., Pantelides, S.T., Lang, N.D., (2000) Phys. Rev. Lett., 84, p. 979
  • Lambert, C.J., (2015) Chem. Soc. Rev., 44, p. 875
  • Khoo, K.H., Chen, Y., Li, S., Quek, S.Y., (2015) Phys. Chem. Chem. Phys., 17, p. 77
  • Datta, S., (1995) Electronic Transport in Mesoscopic Systems, , University Press: Cambridge, United Kingdom
  • Yam, C., Zheng, X., Chen, G., Wang, Y., Frauenheim, T., Niehaus, T.A., (2011) Phys. Rev. B, 83, p. 245448
  • Brandbyge, M., Mozos, J.-L., Ordejón, P., Taylor, J., Stokbro, K., (2002) Phys. Rev. B, 65, p. 165401
  • Joachim, C., Ratner, M.A., (2005) Proc. Natl. Acad. Sci. U. S. A., 102, p. 8801
  • Solomon, G.C., Andrews, D.Q., Duyne, R.P.V., Ratner, M.A., (2008) J. Am. Chem. Soc., 130, p. 7788
  • Stefanucci, G., Almbladh, C.-O., (2004) Europhys. Lett., 67, p. 14
  • Stefanucci, G., Almbladh, C.-O., (2004) Phys. Rev. B, 69, p. 195318
  • Zheng, X., Wang, F., Yam, C.Y., Mo, Y., Chen, G., (2007) Phys. Rev. B, 75, p. 195127
  • Kurth, S., Stefanucci, G., Almbladh, C.-O., Rubio, A., Gross, E.K.U., (2005) Phys. Rev. B, 72, p. 035308
  • Gebauer, R., Piccinin, S., Car, R., (2005) ChemPhysChem, 6, p. 1727
  • Burke, K., Car, R., Gebauer, R., (2005) Phys. Rev. Lett., 94, p. 146803
  • Ventra, M.D., Todorov, T.N., (2004) J. Phys.: Condens. Matter, 16, p. 8025
  • Cheng, C.-L., Evans, J.S., Van Voorhis, T., (2006) Phys. Rev. B, 74, p. 155112
  • Sánchez, C.G., Stamenova, M., Sanvito, S., Bowler, D.R., Horsfield, A.P., Todorov, T.N., (2006) J. Chem. Phys., 124, p. 214708
  • Subotnik, J.E., Hansen, T., Ratner, M.A., Nitzan, A., (2009) J. Chem. Phys., 130, p. 144105
  • Zelovich, T., Kronik, L., Hod, O., (2014) J. Chem. Theory Comput., 10, p. 2927
  • Zelovich, T., Kronik, L., Hod, O., (2016) J. Phys. Chem. C, 120, p. 15052
  • Morzan, U.N., Ramírez, F.F., Oviedo, M.B., Sánchez, C.G., Scherlis, D.A., Gonzalez Lebrero, M.C., (2014) J. Chem. Phys., 140, p. 164105
  • Nitsche, M.A., Ferreria, M., Mocskos, E.E., Gonzalez-Lebrero, M.C., (2014) J. Chem. Theory Comput., 10, p. 959
  • Chen, L., Hansen, T., Franco, I., (2014) J. Phys. Chem. C, 118, p. 20009
  • Hod, O., Rodrguez-Rosario, C.A., Zelovich, T., Frauenheim, T., (2016) J. Phys. Chem. A, 120, p. 3278
  • Zelovich, T., Kronik, L., Hod, O., (2015) J. Chem. Theory Comput., 11, p. 4861
  • Evans, J.S., Voorhis, T.V., (2009) Nano Lett., 9, p. 2671
  • Landauer, R., (1989) J. Phys.: Condens. Matter, 1, p. 8099
  • Liu, H., Wang, N., Zhao, J., Guo, Y., Yin, X., Boey, F.Y.C., Zhang, H., (2008) ChemPhysChem, 9, p. 1416
  • Yao, J., Li, Y., Zou, Z., Wang, H., Shen, Y., (2012) Superlattices Microstruct., 51, p. 396

Citas:

---------- APA ----------
Morzan, U.N., Ramírez, F.F., González Lebrero, M.C. & Scherlis, D.A. (2017) . Electron transport in real time from first-principles. Journal of Chemical Physics, 146(4).
http://dx.doi.org/10.1063/1.4974095
---------- CHICAGO ----------
Morzan, U.N., Ramírez, F.F., González Lebrero, M.C., Scherlis, D.A. "Electron transport in real time from first-principles" . Journal of Chemical Physics 146, no. 4 (2017).
http://dx.doi.org/10.1063/1.4974095
---------- MLA ----------
Morzan, U.N., Ramírez, F.F., González Lebrero, M.C., Scherlis, D.A. "Electron transport in real time from first-principles" . Journal of Chemical Physics, vol. 146, no. 4, 2017.
http://dx.doi.org/10.1063/1.4974095
---------- VANCOUVER ----------
Morzan, U.N., Ramírez, F.F., González Lebrero, M.C., Scherlis, D.A. Electron transport in real time from first-principles. J Chem Phys. 2017;146(4).
http://dx.doi.org/10.1063/1.4974095