Exploring electron transport in carbon wire systems using a wave function-based multiconfigurational non-equilibrium Green's function approach

Abstract

One-dimensional carbon wire materials are an interesting class of materials which have potentially useful applications in sub-nanoscale junction technology due to their unique quantum transport properties. In this work, we apply a non-equilibrium Green's function approach based on multiconfiguration pair-density functional theory (NEGF-MCPDFT). NEGF-MCPDFT is a wave-function-based non-periodic framework to study electron transport in systems exhibiting strong correlation. The advantage of this approach is multiconfigurational wave functions are used which offer enhanced abilities to describe strong electron correlation beyond single-determinant approaches. MC-PDFT necessitates the use of an active space, and a key step in such calculations is the determination of which orbitals to include. In application of this theory to carbon wire junctions of various lengths, we find that NEGF-MCPDFT is capable of reproducing trends from recent experimental results, and we use our findings to further the development of best practices in active space design for transport calculations of this type.