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DFT approaches to transport calculations in magnetic single-molecule devices

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Abstract

Electron transport properties of single-molecule devices based on the [Fe(tzpy)2(NCS)2] complex placed between two gold electrodes have been explored using three different atomistic DFT methods. This kind of single-molecule devices is quite appealing because they can present magnetoresistance effects at room temperature. The three employed computational approaches are: (i) self-consistent non-equilibrium Green functions (NEGF) with periodic models that can be described as the most accurate between the state-of-art methods, and two non-self-consistent NEGF approaches using either periodic or non-periodic description of the electrodes (ii and iii). The analysis of the transmission spectra obtained with the three methods indicates that they provide similar qualitative results. To obtain a reasonable agreement with the experimental data, it is mandatory to employ density functionals beyond the commonly employed GGA (i.e., hybrid functionals) or to include on-site corrections for the Coulomb repulsion (GGA+U method).

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Acknowledgments

The research reported here was supported by the Spanish Ministerio de Economía y Competitividad (Grant CTQ2015-64579-C3-1-P, MINECO/FEDER, UE). E.R. thanks Generalitat de Catalunya for an ICREA Academia award. A.M.-R. acknowledges the University of Barcelona for a collaboration grant. D.A. thanks CONICYT + PAI “Concurso nacional de apoyo al retorno de investigadores/as desde el extranjero, convocatoria 2014 82140014” for financial support. E.R. thankfully acknowledges the computer resources in the Barcelona Supercomputer Center, technical expertise and assistance provided by the Red Española de Supercomputación. D.A. thanks the program Powered@NLHPC: This research was partially supported by the supercomputing infrastructure of the NLHPC (ECM-02).

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Authors and Affiliations

  1. Departament de Química Inorgànica i Orgànica and Institut de Química Teòrica i Computacional, Universitat de Barcelona, Diagonal 645, 08028, Barcelona, Spain

    Alejandro Martín-Rodríguez & Eliseo Ruiz

  2. Departamento de Química de los Materiales, Facultad de Química y Biología, Universidad de Santiago de Chile (USACH), Casilla 40, Correo 33, Santiago, Chile

    Daniel Aravena

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  1. Alejandro Martín-Rodríguez
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  2. Daniel Aravena
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Correspondence to Eliseo Ruiz.

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Published as part of the special collection of articles “Festschrift in honour of A. Vela”.

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Martín-Rodríguez, A., Aravena, D. & Ruiz, E. DFT approaches to transport calculations in magnetic single-molecule devices. Theor Chem Acc 135, 192 (2016). https://doi.org/10.1007/s00214-016-1941-6

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