Thermal conductance through molecular wires

We consider phononic heat transport through molecular chains connecting two thermal reservoirs. For relatively short molecules at normal temperatures heat conduction is dominated by the harmonic part of the molecular force-field. We develop a general theory for the heat conduction through harmonic chains in 3-dimensions. A Landauer-type expression for the heat conduction is obtained, in agreement with other recent studies. We use this formalism to study the heat conduction properties of alkanes. For relatively short (1-30 carbon atoms) chains the length and temperature dependence of the molecular heat conduction result from the balance of three factors: (i) The molecular frequency spectrum in relation to the frequency cutoff of the thermal reservoirs, (ii) the degree of localization of the molecular normal modes and (iii) the molecule-heat reservoirs coupling. The fact that molecular modes at different frequency regimes have different localization properties gives rise to intricate dependence of the heat conduction on molecular length at different temperatures. For example, the heat conduction increases with molecular length for short molecular chains at low temperatures. Similar considerations apply for isotopically substituted disordered chains. Finally, we compare the heat conduction obtained from this microscopic calculation to that estimated by considering the molecule as a cylinder characterized by a macroscopic heat conduction typical to organic solids. We find that this classical model overestimates the heat conduction of single alkane molecules by about an order of magnitude at room temperature. Implications of the present study to the problem of heating in electrically conducting molecular junctions are pointed out.Comment: 40 pages, 11 figures. J. Chem. Phys. Submitte

From a kinetic equation to a diffusion under an anomalous scaling

A linear Boltzmann equation is interpreted as the forward equation for the probability density of a Markov process (K(t), i(t), Y(t)), where (K(t), i(t)) is an autonomous reversible jump process, with waiting times between two jumps with finite expectation value but infinite variance, and Y(t) is an additive functional of K(t). We prove that under an anomalous rescaling Y converges in distribution to a two-dimensional Brownian motion. As a consequence, the appropriately rescaled solution of the Boltzmann equation converges to a diffusion equation

Transport in the XX chain at zero temperature: Emergence of flat magnetization profiles

We study the connection between magnetization transport and magnetization profiles in zero-temperature XX chains. The time evolution of the transverse magnetization, m(x,t), is calculated using an inhomogeneous initial state that is the ground state at fixed magnetization but with m reversed from -m_0 for x0. In the long-time limit, the magnetization evolves into a scaling form m(x,t)=P(x/t) and the profile develops a flat part (m=P=0) in the |x/t|1/2 while it expands with the maximum velocity, c_0=1, for m_0->0. The states emerging in the scaling limit are compared to those of a homogeneous system where the same magnetization current is driven by a bulk field, and we find that the expectation values of various quantities (energy, occupation number in the fermionic representation) agree in the two systems.Comment: RevTex, 8 pages, 3 ps figure

Existence of temperature on the nanoscale

We consider a regular chain of quantum particles with nearest neighbour interactions in a canonical state with temperature $T$. We analyse the conditions under which the state factors into a product of canonical density matrices with respect to groups of $n$ particles each and under which these groups have the same temperature $T$. In quantum mechanics the minimum group size $n_{min}$ depends on the temperature $T$, contrary to the classical case. We apply our analysis to a harmonic chain and find that $n_{min} = const.$ for temperatures above the Debye temperature and $n_{min} \propto T^{-3}$ below.Comment: Version that appeared in PR

Anomalous thermal conductivity and local temperature distribution on harmonic Fibonacci chains

The harmonic Fibonacci chain, which is one of a quasiperiodic chain constructed with a recursion relation, has a singular continuous frequency-spectrum and critical eigenstates. The validity of the Fourier law is examined for the harmonic Fibonacci chain with stochastic heat baths at both ends by investigating the system size N dependence of the heat current J and the local temperature distribution. It is shown that J asymptotically behaves as (ln N)^{-1} and the local temperature strongly oscillates along the chain. These results indicate that the Fourier law does not hold on the harmonic Fibonacci chain. Furthermore the local temperature exhibits two different distribution according to the generation of the Fibonacci chain, i.e., the local temperature distribution does not have a definite form in the thermodynamic limit. The relations between N-dependence of J and the frequency-spectrum, and between the local temperature and critical eigenstates are discussed.Comment: 10 pages, 4 figures, submitted to J. Phys.: Cond. Ma

Heat conduction in the diatomic Toda lattice revisited

The problem of the diverging thermal conductivity in one-dimensional (1-D) lattices is considered. By numerical simulations, it is confirmed that the thermal conductivity of the diatomic Toda lattice diverges, which is opposite to what one has believed before. Also the diverging exponent is found to be almost the same as the FPU chain. It is reconfirmed that the diverging thermal conductivity is universal in 1-D systems where the total momentum preserves.Comment: 3 pages, 3 figures. To appear in Phys. Rev.

Energy transport through rare collisions

We study a one-dimensional hamiltonian chain of masses perturbed by an energy conserving noise. The dynamics is such that, according to its hamiltonian part, particles move freely in cells and interact with their neighbors through collisions, made possible by a small overlap of size $\epsilon > 0$ between near cells. The noise only randomly flips the velocity of the particles. If $\epsilon \rightarrow 0$, and if time is rescaled by a factor $1/{\epsilon}$, we show that energy evolves autonomously according to a stochastic equation, which hydrodynamic limit is known in some cases. In particular, if only two different energies are present, the limiting process coincides with the simple symmetric exclusion process.Comment: 24 pages, 2 figure

Thermal conductivity of one-dimensional lattices with self-consistent heat baths: a heuristic derivation

We derive the thermal conductivities of one-dimensional harmonic and anharmonic lattices with self-consistent heat baths (BRV lattice) from the Single-Mode Relaxation Time (SMRT) approximation. For harmonic lattice, we obtain the same result as previous works. However, our approach is heuristic and reveals phonon picture explicitly within the heat transport process. The results for harmonic and anharmonic lattices are compared with numerical calculations from Green-Kubo formula. The consistency between derivation and simulation strongly supports that effective (renormalized) phonons are energy carriers in anharmonic lattices although there exist some other excitations such as solitons and breathers.Comment: 4 pages, 3 figures. accepted for publication in JPS

A Symmetry Property of Momentum Distribution Functions in the Nonequilibrium Steady State of Lattice Thermal Conduction

We study a symmetry property of momentum distribution functions in the steady state of heat conduction. When the equation of motion is symmetric under change of signs for all dynamical variables, the distribution function is also symmetric. This symmetry can be broken by introduction of an asymmetric term in the interaction potential or the on-site potential, or employing the thermal walls as heat reservoirs. We numerically find differences of behavior of the models with and without the on-site potential.Comment: 13 pages. submitted to JPS

Correlations and scaling in one-dimensional heat conduction

We examine numerically the full spatio-temporal correlation functions for all hydrodynamic quantities for the random collision model introduced recently. The autocorrelation function of the heat current, through the Kubo formula, gives a thermal conductivity exponent of 1/3 in agreement with the analytical prediction and previous numerical work. Remarkably, this result depends crucially on the choice of boundary conditions: for periodic boundary conditions (as opposed to open boundary conditions with heat baths) the exponent is approximately 1/2. This is expected to be a generic feature of systems with singular transport coefficients. All primitive hydrodynamic quantities scale with the dynamic critical exponent predicted analytically.Comment: 7 pages, 11 figure