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Register a new userMicroscopic theory and quantum simulation of atomic heat transport
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Quantum simulation methods based on density-functional theory are currently deemed unfit to cope with atomic heat transport within the Green-Kubo formalism, because quantum-mechanical energy densities and currents are inherently ill-defined at the atomic scale. We show that, while this difficulty would also affect classical simulations, thermal conductivity is indeed insensitive to such ill-definedness by virtue of a sort of gauge invariance resulting from energy extensivity and conservation. Based on these findings, we derive an expression for the adiabatic energy flux from density-functional theory, which allows heat transport to be simulated using ab-initio equilibrium molecular dynamics. Our methodology is demonstrated by comparing its predictions with those of classical equilibrium and ab-initio non-equilibrium (Muller-Plathe) simulations for a liquid-Argon model, and finally applied to heavy water at ambient conditions.
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Metallic atomic junctions pose the ultimate limit to the scaling of electrical contacts. They serve as model systems to probe electrical and thermal transport down to the atomic level as well as quantum effects occurring in one-dimensional systems. Charge transport in atomic junctions has been studied intensively in the last two decades. However, heat transport remains poorly characterized because of significant experimental challenges. Specifically the combination of high sensitivity to small heat fluxes and the formation of stable atomic contacts has been a major hurdle for the development of this field. Here we report on the realization of heat transfer measurements through atomic junctions and analyze the thermal conductance of single atomic gold contacts at room temperature. Simultaneous measurements of charge and heat transport reveal the proportionality of electrical and thermal conductance, quantized with the respective conductance quanta. This constitutes an atomic scale verification of the well-known Wiedemann-Franz law. We anticipate that our findings will be a major advance in enabling the investigation of heat transport properties in molecular junctions, with meaningful implications towards the manipulation of heat at the nanoscale
We present a quantum-kinetic scheme for the calculation of non-equilibrium transport properties in nanoscale systems. The approach is based on a Liouville-master equation for a reduced density operator and represents a generalization of the well-known Boltzmann kinetic equation. The system, subject to an external electromotive force, is described using periodic boundary conditions. We demonstrate the feasibility of the approach by applying it to a double-barrier resonant tunneling structure.
We have analyzed the atomic arrangements and quantum conductance of silver nanowires generated by mechanical elongation. The surface properties of Ag induce unexpected structural properties, as for example, predominance of high aspect ratio rod-like wires. The structural behavior was used to understand the Ag quantum conductance data and the proposed correlation was confirmed by means of theoretical calculations. These results emphasize that the conductance of metal point contacts is determined by the preferred atomic structures and, that atomistic descriptions are essential to interpret the quantum transport behavior of metal nanostructures.
We formulate a microscopic theory of the decay of a compound nucleus through fission which generalizes earlier microscopic approaches of fission dynamics performed in the framework of the adiabatic hypothesis. It is based on the constrained Hartree-Fock-Bogoliubov procedure and the Generator Coordinate Method, and requires an effective nucleon-nucleon interaction as the only input quantity. The basic assumption is that the slow evolution of the nuclear shape must be treated explicitely, whereas the rapidly time-dependent intrinsic excitations can be treated by statistical approximations. More precisely, we introduce a reference density which represents the slow evolution of the nuclear shape by a reduced density matrix and the state of intrinsic excitations by a canonical distribution at each given shape of the nucleus. The shape of the nuclear density distribution is described by parameters (generator coordinates), not by superabundant degrees of freedom introduced in addition to the complete set of nucleonic degrees of freedom. We first derive a rigorous equation of motion for the reference density and, subsequently, simplify this equation on the basis of the Markov approximation. The temperature which appears in the canonical distribution is determined by the requirement that, at each time t, the reference density should correctly reproduce the mean excitation energy at given values of the shape parameters. The resulting equation for the local temperature must be solved together with the equations of motion obtained for the reduced density matrix.
With the advent of atomic-resolution transmission electron microscopy (AR-TEM) achieving sub-{AA}ngstrom image resolution and submillisecond time resolution, an era of visual molecular science where chemists can visually study the time evolution of molecular motions and reactions at atomistic precision has arrived. However, the appearance of experimental TEM images often differs greatly from that of conventional molecular models, and the images are difficult to decipher unless we know in advance the structure of the specimen molecules. The difference arises from the fundamental design of the molecular models that represent atomic connectivity and/or the electronic properties of molecules rather than the nuclear charge of atoms and electrostatic potentials that are felt by the e-beam in TEM imaging. We found a good correlation between the atomic number (Z) and the atomic size seen in TEM images when we consider shot noise in digital images. We propose here Z-correlated (ZC) atomic radii for modeling AR-TEM images of single molecules and ultrathin crystals, with which we can develop a good estimate of the molecular structure from the TEM image much more easily than with conventional molecular models. Two parameter sets were developed for TEM images recorded under high-noise (ZCHN) and low-noise (ZCLN) conditions. The new molecular models will stimulate the imaginations of chemists planning to use AR-TEM for their research.
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