We have developed an efficient simulation tool GOLLUM for the computation of electrical, spin and thermal transport characteristics of complex nanostructures. The new multi-scale, multi-terminal tool addresses a number of new challenges and functiona
lities that have emerged in nanoscale-scale transport over the past few years. To illustrate the flexibility and functionality of GOLLUM, we present a range of demonstrator calculations encompassing charge, spin and thermal transport, corrections to density functional theory such as LDA+U and spectral adjustments, transport in the presence of non-collinear magnetism, the quantum-Hall effect, Kondo and Coulomb blockade effects, finite-voltage transport, multi-terminal transport, quantum pumps, superconducting nanostructures, environmental effects and pulling curves and conductance histograms for mechanically-controlled-break-junction experiments.
We present a general analytical formula and an ab initio study of quantum interference in multi-branch molecules. Ab initio calculations are used to investigate quantum interference in a benzene-1,2-dithiolate (BDT) molecule sandwiched between gold e
lectrodes and through oligoynes of various lengths. We show that when a point charge is located in the plane of a BDT molecule and its position varied, the electrical conductance exhibits a clear interference effect, whereas when the charge approaches a BDT molecule along a line normal to the plane of the molecule and passing through the centre of the phenyl ring, interference effects are negligible. In the case of olygoynes, quantum interference leads to the appearance of a critical energy $E_c$, at which the electron transmission coefficient $T(E)$ of chains with even or odd numbers of atoms is independent of length. To illustrate the underlying physics, we derive a general analytical formula for electron transport through multi-branch structures and demonstrate the versatility of the formula by comparing it with the above ab-initio simulations. We also employ the analytical formula to investigate the current inside the molecule and demonstrate that large counter currents can occur within a ring-like molecule such as BDT, when the point charge is located in the plane of the molecule. The formula can be used to describe quantum interference and Fano resonances in structures with branches containing arbitrary elastic scattering regions connected to nodal sites.
We present a study of the thermopower $S$ and the dimensionless figure of merit $ZT$ in molecules sandwiched between gold electrodes. We show that for molecules with side groups, the shape of the transmission coefficient can be dramatically modified
by Fano resonances near the Fermi energy, which can be tuned to produce huge increases in $S$ and $ZT$. This shows that molecules exhibiting Fano resonances have a high efficiency of thermoelectric cooling which is not present for conventional un-gated molecules with only delocalized states along their backbone.
