Time-dependent Kohn-Sham theory with memory

In time-dependent density-functional theory, exchange and correlation (xc) beyond the adiabatic local density approximation can be described in terms of viscoelastic stresses in the electron liquid. In the time domain, this leads to a velocity-dependent xc vector potential with a memory containing short- and long-range components. The resulting time-dependent Kohn-Sham formalism describes the dynamics of electronic systems including decoherence and relaxation. For the example of collective charge-density oscillations in a quantum well, we illustrate the xc memory effects, clarify the dissipation mechanism, and extract intersubband relaxation rates for weak and strong excitations.Comment: 4 pages, 4 figure

On the problem of mass-dependence of the two-point function of the real scalar free massive field on the light cone

We investigate the generally assumed inconsistency in light cone quantum field theory that the restriction of a massive, real, scalar, free field to the nullplane $\Sigma=\{x^0+x^3=0\}$ is independent of mass \cite{LKS}, but the restriction of the two-point function depends on it (see, e.g., \cite{NakYam77, Yam97}). We resolve this inconsistency by showing that the two-point function has no canonical restriction to $\Sigma$ in the sense of distribution theory. Only the so-called tame restriction of the two-point function exists which we have introduced in \cite{Ull04sub}. Furthermore, we show that this tame restriction is indeed independent of mass. Hence the inconsistency appears only by the erroneous assumption that the two-point function would have a (canonical) restriction to $\Sigma$.Comment: 10 pages, 2 figure

A minimal model for excitons within time-dependent density-functional theory

The accurate description of the optical spectra of insulators and semiconductors remains an important challenge for time-dependent density-functional theory (TDDFT). Evidence has been given in the literature that TDDFT can produce bound as well as continuum excitons for specific systems, but there are still many unresolved basic questions concerning the role of dynamical exchange and correlation (xc). In particular, the role of the long spatial range and the frequency dependence of the xc kernel $f_{\rm xc}$ for excitonic binding are still not very well explored. We present a minimal model for excitons in TDDFT, consisting of two bands from a one-dimensional Kronig-Penney model and simple approximate xc kernels, which allows us to address these questions in a transparent manner. Depending on the system, it is found that adiabatic xc kernels can produce a single bound exciton, and sometimes two bound excitons, where the long spatial range of $f_{\rm xc}$ is not a necessary condition. It is shown how the Wannier model, featuring an effective electron-hole interaction, emerges from TDDFT. The collective, many-body nature of excitons is explicitly demonstrated.Comment: 12 pages, 11 figure

Ultra-nonlocality in density functional theory for photo-emission spectroscopy

We derive an exact expression for the photo-current of photo-emission spectroscopy using time-dependent current density functional theory (TDCDFT). This expression is given as an integral over the Kohn-Sham spectral function renormalized by effective potentials that depend on the exchange-correlation kernel of current density functional theory. We analyze in detail the physical content of this expression by making a connection between the density-functional expression and the diagrammatic expansion of the photo-current within many-body perturbation theory. We further demonstrate that the density functional expression does not provide us with information on the kinetic energy distribution of the photo-electrons. Such information can, in principle, be obtained from TDCDFT by exactly modeling the experiment in which the photo-current is split into energy contributions by means of an external electromagnetic field outside the sample, as is done in standard detectors. We find, however, that this procedure produces very nonlocal correlations between the exchange-correlation fields in the sample and the detector.Comment: 11 pages, 11 figure

Singlet-triplet oscillations and far-infrared spectrum of four-minima quantum-dot molecule

We study ground states and far-infrared spectra (FIR) of two electrons in four-minima quantum-dot molecule in magnetic field by exact diagonalization. Ground states consist of altering singlet and triplet states, whose frequency, as a function of magnetic field, increases with increasing dot-dot separation. When the Zeeman energy is included, only the two first singlet states remain as ground states. In the FIR spectra, we observe discontinuities due to crossing ground states. Non-circular symmetry induces anticrossings, and also an additional mode above $\omega_+$ in the spin-triplet spectrum. In particular, we conclude that electron-electron interactions cause only minor changes to the FIR spectra and deviations from the Kohn modes result from the low-symmetry confinement potential.Comment: 4 pages, 3 figures, QD2004 conference paper, accepted in Physica

Time-resolved X-ray microscopy of nanoparticle aggregates under oscillatory shear

Of all current detection techniques with nanometer resolution, only X-ray microscopy allows imaging nanoparticles in suspension. Can it also be used to investigate structural dynamics? When studying response to mechanical stimuli, the challenge lies in applying them with precision comparable to spatial resolution. In the first shear experiments performed in an X-ray microscope, we accomplished this by inserting a piezo actuator driven shear cell into the focal plane of a scanning transmission X-ray microscope (STXM). Thus shear-induced reorganization of magnetite nanoparticle aggregates could be demonstrated in suspension. As X-ray microscopy proves suitable for studying structural change, new prospects open up in physics at small length scales.Comment: submitted to J. Synchrot. Radia

Redox regulation in disease and ageing

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A systematic benchmark of the ab initio Bethe-Salpeter equation approach for low-lying optical excitations of small organic molecules

The predictive power of the ab initio Bethe-Salpeter equation (BSE) approach, rigorously based on many-body Green's function theory but incorporating information from density functional theory, has already been demonstrated for the optical gaps and spectra of solid-state systems. Interest in photoactive hybrid organic/inorganic systems has recently increased, and so has the use of the BSE for computing neutral excitations of organic molecules. However, no systematic benchmarks of the BSE for neutral electronic excitations of organic molecules exist. Here, we study the performance of the BSE for the 28 small molecules in Thiel's widely-used time-dependent density functional theory benchmark set [M. Schreiber et al. J. Chem. Phys. 128, 134110 (2008)]. We observe that the BSE produces results that depend critically on the mean-field starting point employed in the perturbative approach. We find that this starting point dependence is mainly introduced through the quasiparticle energies obtained at the intermediate GW step, and that with a judicious choice of starting mean-field, singlet excitation energies obtained from BSE are in excellent quantitative agreement with higher-level wavefunction methods. The quality of the triplet excitations is slightly less satisfactory