Nonequilibrium photo dynamics of low-dimensional strongly correlated electron systems

One of the outstanding contemporary challenges in condensed matter physics is to understand the dynamics of interacting quantum systems exposed to an external perturbation. We theoretically examine nonequilibrium photo dynamics and its interplay of charge, spin, and lattice degrees of freedom on a Hubbard-Holstein chain in one dimension and a t-J-Holstein square lattice in two dimensions. In the chain, performing dynamical density-matrix renormalization group calculations, we find that many phonons generated dynamically after photo irradiation in Mott insulators cause initial relaxation process. On the other hand, in the square lattice with model parameters as relevant for cuprates, a Lanczos-type exact diagonalization calculation shows that the majority of absorbed energy flows into spin subsystem rather than phonon subsystem.     

Features of electron transfer along heterogeneous atomic chains

The problem of electron transfer along a linear chain of atoms is discussed. The process under study occurs after the electron has transited from a hydrogen ion to an atomic chain. The wave packet propagation method not involving the perturbation theory was used for the calculations. Conclusions on the electron transfer behavior and necessary conditions are drawn. The approach can be applied to real physical systems where electron transition from a charged particle takes place.     

Nonequilibrium thermofield dynamics

The dissipative effects in nonequilibrium thermodfield dynamics are the gauge fields of theSU(1, 1) symmetry of the free bosonic thermal theory [SU(2) for the fermionic one]. In two dimensions some nonequilibrium systems are equivalent to equilibrium systems. An interesting relation exists between the equivalence principle of general relativity and the assumption, in statistical mechanics, of the existence of local subsystems in equilibrium.     

Nonequilibrium molecular dynamics simulation of coupling between nanoparticles and base-fluid in a nanofluid

The intent of this study is to examine nonequilibrium heat transfer in a copper-argon nanofluid by molecular dynamics simulation. Two different methods, the physical definition method and the curve fitting method, are introduced to calculate the coupling factor between nanoparticles and base fluid. The results show that the coupling factors obtained by these two methods are consistent. The coupling factor is proportional to the volume fraction of the nanoparticle and inversely proportional to nanoparticle diameter. In the temperature range of 90-200 K, the coupling factor is not affected by temperature. The nanoparticle aggregation results in a decrease of the coupling factor.     

Single molecule electron transfer dynamics in complex environments

We propose a new theoretical approach to study the kinetics of the electron transfer (ET) under the dynamical influence of the complex environments with the first passage times (FPT) of the reaction events. By measuring the mean and high order moments of FPT and their ratios, the full kinetics of ET, especially the dynamical transitions across different temperature zones, is revealed. The potential applications of the current results to single molecule electron transfer are discussed.     

Realistic quantitative descriptions of electron transfer reactions: diabatic free-energy surfaces from first-principles molecular dynamics

A general approach to calculate the diabatic surfaces for electron-transfer reactions is presented, based on first-principles molecular dynamics of the active centers and their surrounding medium. The excitation energy corresponding to the transfer of an electron at any given ionic configuration (the Marcus energy gap) is accurately assessed within ground-state density-functional theory via a novel penalty functional for oxidation-reduction reactions that appropriately acts on the electronic degrees of freedom alone. The self-interaction error intrinsic to common exchange-correlation functionals is also corrected by the same penalty functional. The diabatic free-energy surfaces are then constructed from umbrella sampling on large ensembles of configurations. As a paradigmatic case study, the self-exchange reaction between ferrous and ferric ions in water is studied in detail.     

Vibrational control of molecular electron transfer reactions

ABSTRACT

Vibrational motions promote molecular electron transfer (ET) reactions by bringing electron donor and electron acceptor electronic states to fleeting resonance, and by modulating the donor-to-acceptor electronic coupling. The main experimental signature of molecular motion effects on the ET rate is the temperature dependence of the rate, which gives information about the overall free energy activation barrier for the ET reaction. Another approach to probing the vibrational control of ET reactions is to excite specific electron-transfer-active vibrational motions by external infrared (IR) fields. This type of experimental probe is potentially more specific than thermal excitation and recent experiments have shown that molecular ET rates can be perturbed by mode-specific IR driving. We review the theory and experiments of vibrational control of ET rates, and discuss future challenges that need to be tackled in order to achieve the mode-specific tuning of rates.     

New insights into electron spin dynamics in the presence of correlated noise

The changes in the spin depolarization length in zinc-blende semiconductors when an external component of correlated noise is added to a static driving electric field are analyzed for different values of field strength, noise amplitude and correlation time. Electron dynamics is simulated by a Monte Carlo procedure which takes into account all the possible scattering phenomena of the hot electrons in the medium and includes the evolution of spin polarization. Spin depolarization is studied by examining the decay of the initial spin polarization of the conduction electrons through the D'yakonov-Perel process, the only relevant relaxation mechanism in III-V crystals. Our results show that, for electric field amplitudes lower than the Gunn field, the dephasing length shortens with increasing noise intensity. Moreover, a nonmonotonic behavior of spin depolarization length with the noise correlation time is found, characterized by a maximum variation for values of noise correlation time comparable with the dephasing time. Instead, in high field conditions, we find that, critically depending on the noise correlation time, external fluctuations can positively affect the relaxation length. The influence of the inclusion of the electron-electron scattering mechanism is also shown and discussed.     

Nonequilibrium molecular dynamics simulation of shear viscosity by a uniform momentum source-and-sink scheme

A uniform momentum source-and-sink scheme of nonequilibrium molecular dynamics (NEMD) is developed to calculate the shear viscosity of fluids in this paper. The uniform momentum source and sink are realized by momentum exchanges of individual atoms in the left and right half systems, like the reverse nonequilibrium molecular dynamics (RNEMD) method [20] [Müller-Plathe, Phys. Rev. E, 49 (359), 1999]. This method has all features of RNEMD. In addition, the present momentum swap strategy maximizes the perturbation relaxation and eliminates the boundary jumps, which often harm other NEMD methods greatly. With periodic boundary conditions quadratic velocity profiles can be constructed and from the mean velocities of the right and left half systems the shear viscosity can be easily extracted. The scheme is tested on Lennard-Jones fluids over a wide range of state points (temperature and density), momentum exchange intervals and system sizes. It is demonstrated that the present approach can give reliable results with fast convergence by properly selecting the simulation parameters, i.e. particle number and exchange interval.     

Semiclassical dynamics of electron transfer at metal surfaces

In this Letter, we demonstrate that nonadiabatic dynamics of molecular scattering from metal surfaces can be efficiently simulated by semiclassical Gaussian wave packet propagation on a local complex potential. The method relies on the wideband limit decoupling of the nuclear equations of motion on different electronic states. If the continuum diabatic potential surfaces are assumed to be parallel, the number of Gaussian wave packets spawned scales at most linearly with propagation time, allowing efficient propagation of nuclear dynamics.     

Soliton dynamics in chiral molecular chains with first- and third-neighbour interactions

We investigate the propagation and interaction of solitons associated with circularly polarized vibrations in gyrotropic media. The chirality of the structure yields different dispersion laws and hence different phase and group velocities for the left- and right-handed modes. The helical arrangement of the monomers is modelled through first- and third-neighbour interactions. The dynamics of the excitations is governed by a system of coupled discrete nonlinear Schr?dinger equations which is studied both analytically and numerically. Depending on the initial conditions and the interaction constants, different evolutionary patterns are obtained corresponding to unbound or bound one- and two-soliton solutions. The results can be applied to the process of energy transfer in helical polymers. Received 1st October 2001 / Received in final form 30 April 2002 Published online 2 October 2002 RID="a" ID="a"e-mail: krad@issp.bas.bg     

Nonequilibrium dynamics of ultracold Fermi superfluids

The aim of this mini review is to survey the literature on the study of nonequilibrium dynamics of Fermi superfluids in the BCS and BEC limits, both in the single channel and dual channel cases. The focus is on mean field approaches to the dynamics, with specific attention drawn to the dynamics of the Ginzburg-Landau order parameters of the Fermi and composite Bose fields, as well as on the microscopic dynamics of the quantum degrees of freedom. The two approaches are valid approximations in two different time scales of the ensuing dynamics. The system is presumed to evolve during and/or after a quantum quench in the parameter space. The quench can either be an impulse quench with virtually instantaneous variation, or a periodic variation between two values. The literature for the order parameter dynamics, described by the time-dependent Ginzburg-Landau equations, is reviewed, and the works of the author in this area highlighted. The mixed phase regime in the dual channel case is also considered, and the dual order parameter dynamics of Fermi-Bose mixtures reviewed. Finally, the nonequilibrium dynamics of the microscopic degrees of freedom for the superfluid is reviewed for the self-consistent and non self-consistent cases. The dynamics of the former can be described by the Bogoliubov de-Gennes equations with the equilibrium BCS gap equation continued in time and self -consistently coupled to the BdG dynamics. The latter is a reduced BCS problem and can be mapped onto the dynamics of Ising and Kitaev models. This article reviews the dynamics of both impulse quenches in the Feshbach detuning, as well as periodic quenches in the chemical potential, and highlights the author’s contributions in this area of research.     

Contaminants in suspended gold chains: an ab initio molecular dynamics study

Recently, we have proposed that the origin of anomalously long interatomic distances in suspended gold chains could be the result of carbon contamination during sample manipulation [Phys. Rev. Lett. 88, 076105 (2002)]]. More recently, however, other works have proposed that hydrogen instead of carbon should be the most probable contaminant. We report ab initio molecular dynamics results for different temperatures considering different possible contaminants. Our results show that at nonzero temperatures (more realistic to simulate the experimental conditions) hydrogen may be ruled out and carbon atoms remain the best candidate for contamination.     

Nonequilibrium dynamics in two-dimensional Ising spin glass

This paper investigates the nonequilibrium dynamics of two-dimensional Ising spin glass by dynamical Monte Carlo simulations. A new method is developed to quantitatively measure the age of domain growth. Using this method it investigates how temperature shift affects the effective age of domain growth. It finds that the T -shift dependence of the effective age follows the prediction of the droplet model quite well. It also investigates the overlap length between the spin glass states as well as the correlated flips of spins,which are not consistent with the theoretical predictions. The possible reasons are discussed.