Electronic transport in molecular junctions: The generalized Kadanoff-Baym ansatz with initial contact and correlations

: Tuovinen Riku, van Leeuwen Robert, Perfetto Enrico, Stefanucci Gianluca

Publisher: AMER INST PHYSICS

: 2021

: Journal of Chemical Physics

: JOURNAL OF CHEMICAL PHYSICS

: J CHEM PHYS

: ARTN 094104

: 154

: 9

: 12

: 0021-9606

: 1089-7690

DOI: https://doi.org/10.1063/5.0040685

: https://helda.helsinki.fi/bitstream/handle/10138/328669/JCP20_AR_04994.pdf?sequence=1

The generalized Kadanoff-Baym ansatz (GKBA) offers a computationally inexpensive approach to simulate out-of-equilibrium quantum systems within the framework of nonequilibrium Green's functions. For finite systems, the limitation of neglecting initial correlations in the conventional GKBA approach has recently been overcome [Karlsson et al., Phys. Rev. B 98, 115148 (2018)]. However, in the context of quantum transport, the contacted nature of the initial state, i.e., a junction connected to bulk leads, requires a further extension of the GKBA approach. In this work, we lay down a GKBA scheme that includes initial correlations in a partition-free setting. In practice, this means that the equilibration of the initially correlated and contacted molecular junction can be separated from the real-time evolution. The information about the contacted initial state is included in the out-of-equilibrium calculation via explicit evaluation of the memory integral for the embedding self-energy, which can be performed without affecting the computational scaling with the simulation time and system size. We demonstrate the developed method in carbon-based molecular junctions, where we study the role of electron correlations in transient current signatures.