Van der Waals Density Functional for General Geometries

A scheme within density functional theory is proposed that provides a practical way to generalize to unrestricted geometries the method applied with some success to layered geometries [H. Rydberg, et al., Phys. Rev. Lett. 91, 126402 (2003)]. It includes van der Waals forces in a seamless fashion. By expansion to second order in a carefully chosen quantity contained in the long range part of the correlation functional, the nonlocal correlations are expressed in terms of a density-density interaction formula. It contains a relatively simple parametrized kernel, with parameters determined by the local density and its gradient. The proposed functional is applied to rare gas and benzene dimers, where it is shown to give a realistic description.Comment: 4 pages, 4 figure

van der Waals interaction of parallel polymers and nanotubes

We study the mutual interactions of simple, parallel polymers and nanotubes, and develop a scheme to include the van der Waals interactions in the framework of density functional theory (DFT) for these molecules at intermediate to long-range separations. We primarily focus on the polymers polyethylene, isotactic polypropylene, and isotactic polyvinylchloride, but our approach applies more generally to all simple polymers and nanotubes. From first-principle DFT calculations we extract the electron density of the polymers and their static electric response. We derive explicit expressions for the van der Waals interaction energy under simple symmetry assumptions.Comment: 8 pages, 2 figures (2 eps figure files

Binding Energies in Benzene Dimers: Nonlocal Density Functional Calculations

The interaction energy and minimum energy structure for different geometries of the benzene dimer has been calculated using the recently developed nonlocal correlation energy functional for calculating dispersion interactions. The comparison of this straightforward and relatively quick density functional based method with recent calculations can elucidate how the former, quicker method might be exploited in larger more complicated biological, organic, aromatic, and even infinite systems such as molecules physisorbed on surfaces, and van der Waals crystals.Comment: 17 pages, 6 figure

First-principles approach to rotational-vibrational frequencies and infrared intensity for H2_2 adsorbed in nanoporous materials

The absorption sites and the low-lying rotational and vibrational (RV) energy states for H$_2$ adsorbed within a metal-organic framework are calculated via van der Waals density functional theory. The induced dipole due to bond stretching is found to be accurately given by a first-principles driven approximation using maximally-localized-Wannier-function analysis. The strengths and positions of lines in the complex spectra of RV transitions are in reasonable agreement with experiment, and in particular explain the experimentally mysteriously missing primary line for para hydrogen

Spin dynamics from Majorana fermions

Using the Majorana fermion representation of spin-1/2 local moments, we show how it is possible to directly read off the dynamic spin correlation and susceptibility from the one-particle propagator of the Majorana fermion. We illustrate our method by applying it to the spin dynamics of a non-equilibrium quantum dot, computing the voltage-dependent spin relaxation rate and showing that, at weak coupling, the fluctuation-dissipation relation for the spin of a quantum dot is voltage-dependent. We confirm the voltage-dependent Curie susceptibility recently found by Parcollet and Hooley [Phys. Rev. B {\bf 66}, 085315 (2002)].Comment: Small modifications added to figure and tex

Parasitic pumping currents in an interacting quantum dot

We analyze the charge and spin pumping in an interacting dot within the almost adiabatic limit. By using a non-equilibrium Green's function technique within the time-dependent slave boson approximation, we analyze the pumped current in terms of the dynamical constraints in the infinite-U regime. The results show the presence of parasitic pumping currents due to the additional phases of the constraints. The behavior of the pumped current through the quantum dot is illustrated in the spin-insensitive and in the spin-sensitive case relevant for spintronics applications

Evaluation of New Density Functional with Account of van der Waals Forces by Use of Experimental H2 Physisorption Data on Cu(111)

Detailed experimental data for physisorption potential-energy curves of H2 on low-indexed faces of Cu challenge theory. Recently, density-functional theory has been developed to also account for nonlocal correlation effects, including van der Waals forces. We show that one functional, denoted vdW-DF2, gives a potential-energy curve promisingly close to the experiment-derived physisorptionenergy curve. The comparison also gives indications for further improvements of the functionals

Adiabatic pumping through a quantum dot in the Kondo regime: Exact results at the Toulouse limit

Transport properties of ultrasmall quantum dots with a single unpaired electron are commonly modeled by the nonequilibrium Kondo model, describing the exchange interaction of a spin-1/2 local moment with two leads of noninteracting electrons. Remarkably, the model possesses an exact solution when tuned to a special manifold in its parameter space known as the Toulouse limit. We use the Toulouse limit to exactly calculate the adiabatically pumped spin current in the Kondo regime. In the absence of both potential scattering and a voltage bias, the instantaneous charge current is strictly zero for a generic Kondo model. However, a nonzero spin current can be pumped through the system in the presence of a finite magnetic field, provided the spin couples asymmetrically to the two leads. Tunneling through a Kondo impurity thus offers a natural mechanism for generating a pure spin current. We show, in particular, that one can devise pumping cycles along which the average spin pumped per cycle is closely equal to $\hbar$. By analogy with Brouwer's formula for noninteracting systems with two driven parameters, the pumped spin current is expressed as a geometrical property of a scattering matrix. However, the relevant %Alex: I replaced topological with geometrical in the sentence above scattering matrix that enters the formulation pertains to the Majorana fermions that appear at the Toulouse limit rather than the physical electrons that carry the current. These results are obtained by combining the nonequilibrium Keldysh Green function technique with a systematic gradient expansion, explicitly exposing the small parameter controlling the adiabatic limit.Comment: 14 pages, 3 figures, revised versio