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)
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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

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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