Funct. Mater. 2020; 27 (1): 147-158.
doi:https://doi.org/10.15407/fm27.01.147
Extended quasi-correlated orbitals with long-range effects: Application to organic single-molecule electronics
STC "Institute for Single Crystals", National Academy of Sciences of Ukraine, 60 Nauky Ave., 61001 Kharkiv, Ukraine
Abstract:
The previously given quasi-correlated tight-binding (QCTB) π-electron scheme is generalized in a very simple way. We now include long-range electronic effects while retaining, to a certain extent, a tight-binding (TB) basis of the theory. The thus extended quasi-correlated (EQC) method is applied, along with QCTB and usual TB schemes, to compute and analyze Green's functions (GF) and related quantities needed for molecular electronics theory. Several interpretative indexes are suggested (distance correlator, collectivity measure and others) for analyzing GF. This new scheme is used for describing π-electron conductance of large-scale graphene-type molecules. We show that lacking the long-range effects in TB leads to drastic consequences for electron transport (overestimation of conductance by orders of magnitude, nonphysical very large long-distance transmission etc.)
Keywords:
molecular electronics, transmission spectra, conjugated molecules, tight-binding models, electron correlation, long-range interactions.
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