DFT approaches to transport calculations in magnetic single-molecule devices

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 are 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 indicate 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) or to include on-site corrections for the Coulomb repulsion (GGA+U method).

Element-Selective Molecular Charge Transport Characteristics of Binuclear Copper(II)-Lanthanide(III) Complexes

“…The DFT-Hamiltonian and overlap matrices were mapped into a tight-binding scheme to compute the coherent transport properties. The EGF is the nonself-consistent method that presents a good compromise between accuracy and computational cost …”

“…The EGF is the nonself-consistent method that presents a good compromise between accuracy and computational cost. 60 ■ ASSOCIATED CONTENT * S Supporting Information…”

Single-Molecule Transport of Fullerene-Based Curcuminoids

“…41,42,43, This transport code allows calculations with more accurate hybrid functionals improving the orbital energies but using non-periodic models with a rather simpler wide-band limit approximation. 44 The fullerene-electrode contacts for the sliding process were optimized by using the tight-binding approach proposed by Grimme et al. 45 AUTHOR INFORMATION *Email: diana.dulic@gmail.com , h.s.j.vanderzant@tudelft.nl The Journal of Physical Chemistry…”

“…The transmission function was obtained in a postprocessing routine through the Artaios , program. Hamiltonian and overlap matrices needed for the calculation of the transmission function were obtained using ORCA 4.0.1 (B3LYP functional/def2-SVP basis set). − This transport code allows calculations with more accurate hybrid functionals improving the orbital energies but using nonperiodic models with a rather simpler wide-band limit approximation . The fullerene-electrode contacts for the sliding process were optimized by using the tight-binding approach proposed by Grimme et al…”

Polyoxoplatinates as covalently dynamic electron sponges and molecular electronics materials

“…† This level of analysis is quite common for electron transportation calculations along with different sets of molecular junction models. 79 The kinetic energy cut-off of 150 Ryd was set for the self-consistent calculations. The Brillouin zone of the two-probe system was sampled using a 3 × 3 × 100 Monkhorst–Pack grid.…”