Calculation of energy level alignment and interface electronic structure in molecular junctions beyond DFT

0560555 - FZÚ 2023 RIV US eng J - Journal Article
Montes Muñoz, Enrique - Vázquez, Héctor
Calculation of energy level alignment and interface electronic structure in molecular junctions beyond DFT.
Journal of Physical Chemistry C. Roč. 125, č. 46 (2021), s. 25825-25831. ISSN 1932-7447. E-ISSN 1932-7455
R&D Projects: GA MŠMT EF18_070/0010126; GA ČR GA19-23702S
Research Infrastructure: e-INFRA CZ - 90140
Institutional support: RVO:68378271
Keywords : DFT * circuits * charge-transport * metallic electrodes
OECD category: Condensed matter physics (including formerly solid state physics, supercond.)
Impact factor: 4.177, year: 2021
Method of publishing: Limited access
https://doi.org/10.1021/acs.jpcc.1c07407

In atomistic simulations of molecular junctions, it is important to develop methods beyond density-functional theory (DFT) to describe the interface electronic structure and alignment of frontier molecular orbitals accurately. Here we describe a first-principles approach for molecular junctions that extends the DFT+Σ method, an approximate scheme based on self-energy corrections. The DFT+Σtot method presented here acts on junction states and introduces corrections to DFT-based molecular frontier orbitals not only on the molecular subspace but on the whole junction Hamiltonian. These self-energy corrections are scaled according to the molecular character of each junction wave function, a character which is given by projection coefficients between molecular orbitals and junction states. We illustrate this formalism in three paradigmatic weakly interacting single molecule junctions.
Permanent Link: https://hdl.handle.net/11104/0333418