We study atoms trapped with a harmonic confinement in an optical lattice characterized by a flat band and Dirac cones. We show that such an optical lattice can be constructed which can be accurately described with the tight binding or Hubbard models. In the case of fermions the release of the harmonic confinement removes fast atoms occupying the Dirac cones while those occupying the flat band remain immobile. Using exact diagonalization and dynamics we demonstrate that a similar strong occupation of the flat band does not happen in bosonic case and furthermore that the mean field model is not capable for describing the dynamics of the boson cloud.

Electrocatalytic denitrification is a promising technology for the removal of NO x species in groundwater.However, a lack of understanding of the molecular pathways that control the overpotential and product distribution have limited the development of practical electrocatalysts, and additional atomic-level insights are needed to advance this field. Adsorbed NO has been identified as a key intermediate in the NO x electroreduction network, and the elementary steps by which it decomposes to NH 4 + , N 2 , NH 2 OH, or N 2 O remain a subject of debate. Herein, we report a combined Density Functional Theory (DFT) and kinetic Monte Carlo (kMC) study of this reaction on Pt(100), a catalytic surface that is known to be active for the activation of strong covalent bonds, in acidic electrolytes. This approach describes the effects of coverage-dependent adsorbate-adsorbate interactions, water-mediated protonation kinetics and thermodynamics, and transient potential sweeps, on reaction rates and selectivities. The results predict NO stripping curves in excellent agreement with experiments while, at the same time, providing a mechanistic interpretation of observed current peaks. Further, production of NH 4 + products is traced to the rapid kinetics of N-O bond breaking in reactive intermediates, while rapid hydrogenation of surface N* species prevent competing pathways from forming either N 2 or N 2 O. The combined DFT-kMC methodology thus provides a unique tool to describe the mechanism and energetics of platinum-catalyzed electroreduction in the nitrogen cycle, and this approach should also find application to related electrocatalytic processes that are of technological and environmental interest.

The difference between boson and fermion dynamics in quasi-one-dimensional lattices is studied by calculating the persistent current in small quantum rings and by exact simulations of the timeevolution of the many-particle state in two cases: Expansion of a localized cloud, and collisions in a Newtons cradle. We consider three different lattices which in the tight binding model exhibit flat bands. The physical realization is considered to be an optical lattice with bosonic or fermionic atoms. The atoms are assumed to interact with a repulsive short range interaction. The different statistics of bosons and fermions lead to different dynamics. Spinless fermions are easily trapped in the flat-band states due to the Pauli exclusion principle, which prevents them from interacting, while bosons are able to push each other out from the flat-band states.

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We study the pair correlations and excitations of a dipolar Bose gas layer. The anisotropy of the dipole-dipole interaction allows us to tune the strength of pair correlations from strong to weak perpendicular and weak to strong parallel to the layer by increasing the perpendicular trap frequency. This change is accompanied by a roton-roton crossover in the spectrum of collective excitations, from a roton caused by the head-to-tail attraction of dipoles to a roton caused by the side-by-side repulsion, while there is no roton excitation for intermediate trap frequencies. We discuss the nature of these two kinds of rotons and the relation to instabilities of dipolar Bose gases. In both regimes of trap frequencies where rotons occur, we observe strong damping of collective excitations by decay into two rotons.

We have investigated the one-dimensional spin-1 boson Hubbard model with antiferromagnetic interactions using quantum Monte Carlo methods. We obtain the shapes of the two lowest Mott lobes and show that the ground state within the lowest Mott lobe is dimerized. The results presented here are relevant for optically trapped antiferromagnetic spin-1 bosons. An experimental signature of the dimerized ground state is modulated Bragg peaks in the noise distribution of the atomic cloud obtained after switching off the trap. These Bragg peaks are located at wave vectors corresponding to half-integer multiples of the reciprocal wave vector of the optical lattice.

We design models for helium in matrices like aerogel, Vycor or Geltech from a manifestly microscopic point of view. For that purpose, we calculate the dynamic structure function of 4He on Si substrates and between two Si walls as a function of energy, momentum transfer, and the scattering angle. The angle--averaged results are in good agreement with the neutron scattering data; the remaining differences can be attributed to the simplified model used here for the complex pore structure of the materials. A focus of the present work is the detailed identification of coexisting layer modes and bulk--like excitations, and, in the case of thick films, ripplon excitations. Involving essentially two--dimensional motion of atoms, the layer modes are sensitive to the scattering angle.Comment: Phys. Rev. B (2003, in press

Density functional theory-based molecular dynamics (DFT-MD) has been widely used for studying the chemistry of heterogeneous interfacial systems under operational conditions. We report frequently overlooked errors in thermostated or constant-temperature DFT-MD simulations applied to study (electro)catalytic chemistry. Our results demonstrate that commonly used thermostats such as Nosé–Hoover, Berendsen, and simple velocity-rescaling methods fail to provide a reliable temperature description for systems considered. Instead, nonconstant temperatures and large temperature gradients within the different parts of the system are observed. The errors are not a “feature” of any particular code but are present in several ab initio molecular dynamics implementations. This uneven temperature distribution, due to inadequate thermostatting, is well-known in the classical MD community, where it is ascribed to the failure in kinetic energy equipartition among different degrees of freedom in heterogeneous systems ( J. Comput. Chem. et al 1998 726 740 ) and termed the flying ice cube effect. We provide tantamount evidence that interfacial systems are susceptible to substantial flying ice cube effects and demonstrate that the traditional Nosé–Hoover and Berendsen thermostats should be applied with care when simulating, for example, catalytic properties or structures of solvated interfaces and supported clusters. We conclude that the flying ice cube effect in these systems can be conveniently avoided using Langevin dynamics.