arXiv subjects

Tchavdar N. Todorov

Publications and source records attributed to Tchavdar N. Todorov.

At least 19 recordsLinked to original sources

arXiv2025

Viscous AC current-driven nanomotors

The recent discovery that electrons in nano-scale conductors can act like a highly viscous liquid has triggered a surge of research activities investigating consequences of this surprising fact. Here we demonstrate that the electronic viscosity has an enormous influence on the operation of a prototypical AC-current-driven nano-motor. The design of this prototype consists of a diatomic molecule immersed in an otherwise homogeneous electron liquid which carries an AC current. The motion of the diatomic is determined by a subtle balance between the current-induced forces and electronic friction. By ab-initio time-dependent density-functional simulations we demonstrate that the diatomic performs a continuous rotation provided the amplitude and frequency of the imposed AC current lie within certain islands of stability. Outside these islands the nuclear motion is either chaotic or comes to a stand-still. The proposed design of the nano-motor is the conceptually simplest realization of the idea of an molecular waterwheel sandwiched between conducting leads

cond-mat.mes-hall↗

arXiv2024

Viscous current-induced forces

We study the motion (translational, vibrational, and rotational) of a diatomic impurity immersed in an electron liquid and exposed to electronic current. An approach based on the linear response time-dependent density functional theory combined with the Ehrenfest dynamics leads to a system of linear algebraic equations, which account for the competing and counteracting effects of the current-induced force (electron wind) and the electronic friction. These forces, by means of the dynamic exchange-correlation kernel $f_{xc}({\bf r},{\bf r}',ω)$, include the electronic viscosity contribution. Starting from the ground state at the equilibrium inter-nuclear distance and applying a current pulse, we observe three phases of the motion: (I) acceleration due to the prevalence of the current-induced force, (II) stabilization upon balancing of the two forces, and (III) deceleration due to the friction after the end of the pulse. The viscous contribution to the force largely increases the acceleration (deceleration) at the first (third) phase of the process. For the aluminium HEG electron density, we find this correction to amount to up to 70% of the total electron wind and friction effects.

cond-mat.mtrl-sci↗

arXiv2020

Thermal conductivity of porous polycrystalline PbTe

PbTe is a leading thermoelectric material at intermediate temperatures, largely thanks to its low lattice thermal conductivity. However, its efficiency is too low to compete with other forms of power generation. This efficiency can be effectively enhanced by designing nanostructures capable of scattering phonons over a wide range of length scales to reduce the lattice thermal conductivity. The presence of grain boundaries can reduce the thermal conductivity to $\sim 0.5$ Wm$^{-1}$K$^{-1}$ for small vacancy concentrations and grain sizes. However, grains anneal at finite temperature, and equilibrium and metastable grain size distributions determine the extent of the reduction in thermal conductivity. In the present work, we propose a phase-field model informed by molecular dynamics simulations to study the annealing process in PbTe and how it is affected by the presence of grain boundaries and voids. We find that the thermal conductivity of PbTe is reduced by up to 35\% in the porous material at low temperatures. We observe that a phase transition at a finite density of voids governs the kinetics of impeding grain growth by Zener pinning.

cond-mat.mes-hall↗

arXiv2020

Towards temperature-induced topological phase transition in SnTe: A first principles study

The temperature renormalization of the bulk band structure of a topological crystalline insulator, SnTe, is calculated using first principles methods. We explicitly include the effect of thermal-expansion-induced modification of electronic states and their band inversion on electron-phonon interaction. We show that the direct gap decreases with temperature, as both thermal expansion and electron-phonon interaction drive SnTe towards the phase transition to a topologically trivial phase as temperature increases. The band gap renormalization due to electron-phonon interaction exhibits a non-linear dependence on temperature as the material approaches the phase transition, while the lifetimes of the conduction band states near the band edge show a non-monotonic behavior with temperature. These effects should have important implications on bulk electronic and thermoelectric transport in SnTe and other topological insulators.

cond-mat.mtrl-sci↗

arXiv2019

Driven Liouville-von Neumann Equation for Quantum Transport and Multiple-Probe Green's Functions

The so called Driven Liouville-von Neumann equation is a dynamical formulation to simulate a voltage bias across a molecular system and to model a time-dependent current in a grand-canonical framework. This approach introduces a damping term in the equation of motion that drives the charge to a reference, out of equilibrium density. Originally proposed by Horsfield and co-workers, further work on this scheme has led to different coexisting versions of this equation. On the other hand, the multiple-probe scheme devised by Todorov and collaborators, known as the hairy-probes method, is a formal treatment based on Green's functions that allows to fix the electrochemical potentials in two regions of an open quantum system. In this article, the equations of motion of the hairy probes formalism are rewritten to show that, under certain conditions, they can assume the same algebraic structure as the Driven Liouville-von Neumann equation in the form proposed by Morzan et al. [J. Chem. Phys. 2017, 146, 044110]. In this way, a new formal ground is provided for the latter, identifying the origin of every term. The performance of the different methods are explored using tight-binding time-dependent simulations in three trial structures, designated as ballistic, disordered, and resonant models. In the context of first-principles Hamiltonians the Driven Liouville-von Neumann approach is of special interest, because it does not require the calculation of Green's functions. Hence, the effects of replacing the reference density based on the Green's function by one obtained from an applied field are investigated, to gain a deeper understanding of the limitations and the range of applicability of the Driven Liouville-von Neumann equation.

cond-mat.mes-hall↗

arXiv2017

Efficient electron open boundaries for simulating electrochemical cells

Non-equilibrium electrochemistry raises new challenges for atomistic simulation: we need to perform molecular dynamics for the nuclear degrees of freedom with an explicit description of the electrons, which in turn must be free to enter and leave the computational cell. Here we present a limiting form for electron open boundaries that applies when the magnitude of the electric current is determined by the drift and diffusion of ions in solution, and which is sufficiently computationally efficient to be used with molecular dynamics. We demonstrate its capabilities by way of tight binding simulations of a parallel plate capacitor with and without a dimer situated in the space between the plates.

cond-mat.mes-hall↗

arXiv2017

Inelastic electron injection in a water chain

Irradiation of biological matter triggers a cascade of secondary particles that interact with their surroundings, resulting in damage. Low-energy electrons are one of the main secondary species and electron-phonon interaction plays a fundamental role in their dynamics. We have developed a method to capture the electron-phonon inelastic energy exchange in real time and have used it to inject electrons into a simple system that models a biological environment, a water chain. We simulated both an incoming electron pulse and a steady stream of electrons and found that electrons with energies just outside bands of excited molecular states can enter the chain through phonon emission or absorption. Furthermore, this phonon-assisted dynamical behaviour shows great sensitivity to the vibrational temperature, highlighting a crucial controlling factor for the injection and propagation of electrons in water.

physics.chem-ph↗

arXiv2016

Efficient simulations with electronic open boundaries

We present a reformulation of the Hairy Probe method for introducing electronic open boundaries that is appropriate for steady state calculations involving non-orthogonal atomic basis sets. As a check on the correctness of the method we investigate a perfect atomic wire of Cu atoms, and a perfect non-orthogonal chain of H atoms. For both atom chains we find that the conductance has a value of exactly one quantum unit, and that this is rather insensitive to the strength of coupling of the probes to the system, provided values of the coupling are of the same order as the mean inter-level spacing of the system without probes. For the Cu atom chain we find in addition that away from the regions with probes attached, the potential in the wire is uniform, while within them it follows a predicted exponential variation with position. We then apply the method to an initial investigation of the suitability of graphene as a contact material for molecular electronics. We perform calculations on a carbon nanoribbon to determine the correct coupling strength of the probes to the graphene, and obtain a conductance of about two quantum units corresponding to two bands crossing the Fermi surface. We then compute the current through a benzene molecule attached to two graphene contacts and find only a very weak current because of the disruption of the $π$-conjugation by the covalent bond between the benzene and the graphene. In all cases we find that very strong or weak probe couplings suppress the current.

cond-mat.mes-hall↗

arXiv2016

Electron-phonon thermalization in a scalable method for real-time quantum dynamics

We present a quantum simulation method that follows the dynamics of out-of-equilibrium many-body systems of electrons and oscillators in real time. Its cost is linear in the number of oscillators and it can probe timescales from attoseconds to hundreds of picoseconds. Contrary to Ehrenfest dynamics, it can thermalize starting from a variety of initial conditions, including electronic population inversion. While an electronic temperature can be defined in terms of a non-equilibrium entropy, a Fermi-Dirac distribution in general emerges only after thermalization. The time evolution of the populations is rationalized in terms of a kinetic model.

cond-mat.mes-hall↗

arXiv2015

Non-conservative current-driven dynamics: beyond the nanoscale

Long metallic nanowires combine crucial factors for non-conservative current-driven atomic mo- tion. These systems have degenerate vibrational frequencies, clustered about a Kohn anomaly in the dispersion relation, that can couple under current to form non-equilibrium modes of motion growing exponentially in time. Such motion is made possible by non-conservative current-induced forces on atoms, and we refer to it generically as the waterwheel effect. Here the connection be- tween the waterwheel effect and the stimulated directional emission of phonons propagating along the electron flow is discussed in an intuitive manner. Non-adiabatic molecular dynamics show that waterwheel modes self-regulate by reducing the current and by populating modes nearby in fre- quency, leading to a dynamical steady state in which non-conservative forces are counter-balanced by the electronic friction. The waterwheel effect can be described by an appropriate effective non- equilibrium dynamical response matrix. We show that the current-induced parts of this matrix in metallic systems are long-ranged, especially at low bias. This non-locality is essential for the characterisation of non-conservative atomic dynamics under current beyond the nanoscale.

cond-mat.mes-hall↗

arXiv2015

Length matters: keeping atomic wires in check

Dynamical effects of non-conservative forces in long, defect free atomic wires are investigated. Current flow through these wires is simulated and we find that during the initial transient, the kinetic energies of the ions are contained in a small number of phonon modes, closely clustered in frequency. These phonon modes correspond to the waterwheel modes determined from preliminary static calculations. The static calculations allow one to predict the appearance of non-conservative effects in advance of the more expensive real-time simulations. The ion kinetic energy redistributes across the band as non-conservative forces reach a steady state with electronic frictional forces. The typical ion kinetic energy is found to decrease with system length, increase with atomic mass, and its dependence on bias, mass and length is supported with a pen and paper model. This paper highlights the importance of non-conservative forces in current carrying devices and provides criteria for the design of stable atomic wires.

cond-mat.mes-hall↗

arXiv2014

Nonconservative dynamics in long atomic wires

The effect of nonconservative current-induced forces on the ions in a defect-free metallic nanowire is investigated using both steady-state calculations and dynamical simulations. Non-conservative forces were found to have a major influence on the ion dynamics in these systems, but their role in increasing the kinetic energy of the ions decreases with increasing system length. The results illustrate the importance of nonconservative effects in short nanowires and the scaling of these effects with system size. The dependence on bias and ion mass can be understood with the help of a simple pen and paper model. This material highlights the benefit of simple preliminary steady-state calculations in anticipating aspects of brute-force dynamical simulations, and provides rule of thumb criteria for the design of stable quantum wires.

cond-mat.mes-hall↗

arXiv2014

Current-induced forces: a simple derivation

We revisit the problem of forces on atoms under current in nanoscale conductors. We derive and discuss the five principal kinds of force under steady-state conditions from a simple standpoint that - with the help of background literature - should be accessible to physics undergraduates. The discussion aims at combining methodology with an emphasis on the underlying physics through examples. We discuss and compare two forces present only under current - the non-conservative electron wind force and a Lorentz-like velocity-dependent force. It is shown that in metallic nanowires both display significant features at the wire surface, making it a candidate for the nucleation of current-driven structural transformations and failure. Finally we discuss the problem of force noise and the limitations of Ehrenfest dynamics.

cond-mat.mes-hall↗

arXiv2012

An ignition key for atomic-scale engines

A current-carrying resonant nanoscale device, simulated by non-adiabatic molecular dynamics, exhibits sharp activation of non-conservative current-induced forces with bias. The result, above the critical bias, is generalized rotational atomic motion with a large gain in kinetic energy. The activation exploits sharp features in the electronic structure, and constitutes, in effect, an ignition key for atomic-scale motors. A controlling factor for the effect is the non-equilibrium dynamical response matrix for small-amplitude atomic motion under current. This matrix can be found from the steady-state electronic structure by a simpler static calculation, providing a way to detect the likely appearance, or otherwise, of non-conservative dynamics, in advance of real-time modelling.

cond-mat.mes-hall↗

arXiv2012

Current-induced atomic dynamics, instabilities, and Raman signals: Quasi-classical Langevin equation approach

We derive and employ a semi-classical Langevin equation obtained from path-integrals to describe the ionic dynamics of a molecular junction in the presence of electrical current. The electronic environment serves as an effective non-equilibrium bath. The bath results in random forces describing Joule heating,current-induced forces including the non-conservative wind force,dissipative frictional forces, and an effective Lorentz-like force due to the Berry phase of the non-equilibrium electrons. Using a generic two-level molecular model, we highlight the importance of both current-induced forces and Joule heating for the stability of the system. We compare the impact of the different forces, and the wide-band approximation for the electronic structure on our result. We examine the current-induced instabilities (excitation of runaway "waterwheel" modes) and investigate the signature of these in the Raman signals.

cond-mat.mes-hall↗

arXiv2010

On the density-potential mapping in time-dependent density functional theory

The key questions of uniqueness and existence in time-dependent density functional theory are usually formulated only for potentials and densities that are analytic in time. Simple examples, standard in quantum mechanics, lead however to non-analyticities. We reformulate these questions in terms of a non-linear Schrödinger equation with a potential that depends non-locally on the wavefunction.

cond-mat.mtrl-sci↗

arXiv2008

Inelastic quantum transport: the self-consistent Born approximation and correlated electron-ion dynamics

A dynamical method for inelastic transport simulations in nanostructures is compared with a steady-state method based on non-equilibrium Green's functions. A simplified form of the dynamical method produces, in the steady state in the weak-coupling limit, effective self-energies analogous to those in the Born Approximation due to electron-phonon coupling. The two methods are then compared numerically on a resonant system consisting of a linear trimer weakly embedded between metal electrodes. This system exhibits enhanced heating at high biases and long phonon equilibration times. Despite the differences in their formulation, the static and dynamical methods capture local current-induced heating and inelastic corrections to the current with good agreement over a wide range of conditions, except in the limit of very high vibrational excitations, where differences begin to emerge.

cond-mat.mes-hall↗

arXiv2007

On the Newtonian origin of the spin motive force in ferromagnetic atomic wires

We demonstrate numerically the existence of a spin-motive force acting on spin-carriers when moving in a time and space dependent internal field. This is the case of electrons in a one-dimensional wires with a precessing domain wall. The effect can be explained solely by considering adiabatic dynamics and it is shown to exist for both classical and quantum systems.

cond-mat.mtrl-sci↗