We derive rigorous quantum mechanical bounds for the heat current through a nanojunction connecting two thermal baths at different temperatures. Based on exact sum rules, these bounds compliment the well-known quantum of thermal conductance $κ_Q \equiv πk^2_B T/6\hbar$, which provides a bound for low-temperature heat transport in all systems, but is saturated only for noninteracting transport. In contrast, our bounds are saturated at high temperatures---but still in the quantum regime---, even when interactions are very strong. We evaluate these bounds for harmonic and strongly anharmonic junction models and compare with numerical approaches.
We investigate charge transport in pentacene-graphene nanojunctions employing density functional theory (DFT) electronic structure calculations and the Landauer transport formalism. The results show that the unique electronic properties of graphene strongly influence the transport in the nanojunctions. In particular, edge states in graphene electrodes with zigzag termination result in additional transport channels close to the Fermi energy which deeply affects the conductance at small bias voltages. Investigating different linker groups as well as chemical substitution, we demonstrate how the …
We present a simple model of electrical transport through a metal-molecule-metal nanojunction that includes charging effects as well as aspects of the electronic structure of the molecule. The interplay of a large charging energy and an asymmetry of the metal-molecule coupling can lead to various effects in non-linear electrical transport. In particular, strong negative differential conductance is observed under certain conditions.
We study the tunneling transport through a nanojunction in the far-from-equilibrium regime at relatively low temperatures. We show that the current-voltage characteristics is significantly modified as compared to the usual quasi-equilibrium result by lifting the suppression due to the Coulomb blockade. These effects are important in realistic nanojunctions. We study the high-impedance case in detail to explain the underlying physics and construct a more realistic theoretical model for the case of a metallic junction taking into account dynamic Coulomb interaction. This dynamic screening furthe…
Thermal transport through nanosystems is central to numerous processes in chemistry, material sciences, electrical and mechanical engineering, with classical molecular dynamics as the key simulation tool. Here we focus on thermal junctions with a molecule bridging two solids that are maintained at different temperatures. The classical steady state heat current in this system can be simulated in different ways, either at the interfaces with the solids, which are represented by thermostats, or between atoms within the conducting molecule. We show that while the latter, intramolecular definition …
An analog of the Meir-Wingreen formula for the steady-state heat current through a model molecular junction is derived. The expression relates the heat current to correlation functions that involve operators only acting on the degrees of freedom of the molecular junction. As a result, the macroscopic heat reservoirs are not treated explicitly. This allows one to exploit methods based on a reduced description of the dynamics of a relatively small part of the overall system to evaluate the heat current through a molecular junction. The derived expression is applied to calculate the steady-state …
Progress of experimental techniques at nanoscale in the last decade made optical measurements in current-carrying nanojunctions a reality thus indicating emergence of a new field of research coined as optoelectronics. Optical spectroscopy of open nonequilibrium systems is a natural meeting point for (at least) two research areas: nonlinear optical spectroscopy and quantum transport, each with its own theoretical toolbox. We review recent progress in the field comparing theoretical treatments of optical response in nanojunctions as is accepted in nonlinear spectroscopy and quantum transport com…
We show that a current-carrying coherent electron conductor can be treated as effective bosonic energy reservoir involving different types of electron-hole pair excitation. For weak electron-boson coupling, hybrid energy transport between nonequilibrium electrons and bosons can be described by a Landauer-like formula. This allows for unified account of a variety of heat transport problems in hybrid electron-boson systems. As applications, we study the non-reciprocal heat transport between electrons and bosons, thermoelectric current from a cold-spot and electronic cooling of the bosons. Our un…
As a fundamental requisite for thermotronics, controlling heat flow has been a longstanding quest in solid state physics. Recently, there has been a lot of interest in nanoscale hybrid systems as possible candidates for thermal devices. In this context, we study the heat current in the simplest hybrid device of a two level system weakly coupled to two heat baths. We use the reduced density matrix approach together with a simple Born-Markov approximation to calculate the heat current in the steady state. We consider different kinds of reservoirs and show that the nature of the reservoir plays a…
We theoretically investigate heat transport in hybrid normal metal-superconductor (NS) nanojunctions focusing on the effect of thermal rectification. We show that the heat diode effect in the junction strongly depends on the transmissivity and the nature of the NS contact. Thermal rectification efficiency can reach up to 123% for a fully-transmissive ballistic junction and up to 84% in diffusive NS contacts. Both values exceed the rectification efficiency of a NIS tunnel junction (I stands for an insulator) by a factor close to 5 and 3, respectively. Furthermore, we show that for NS point-cont…
Many phenomena in condensed matter are thought to result from competition between different ordered phases. Palladium is a paramagnetic metal close to both ferromagnetism and superconductivity, and is therefore a potentially interesting material to consider. Nanoscale structuring of matter can modify relevant physical energy scales leading to effects such as locally modified magnetic interactions. We present transport measurements in electromigrated palladium break junction devices showing the emergence at low temperatures of anomalous sharp features in the differential conductance. These feat…
(Dated: July 17, 2017) We calculate the electric charge current flowing through a vibrating molecular nanojunction, which is driven by an ac voltage, in its regime of nonlinear oscillations. Without loss of generality, we model the junction by a vibrating molecule which is doubly clamped to two metallic leads which are biased by time-periodic ac voltages. Dressed-electron tunneling between the leads and the molecule drives the mechanical degree of freedom out of equilibrium. In the deep quantum regime, where only a few vibrational quanta are excited, the formation of coherent vibrational reson…
Coherent electronic transport through a molecular device is studied using non-equilibrium Green's function (NEGF) formalism. Such device is made of a carbon nanowire which is connected to ferromagnetic electrodes. The molecule itself is described with the help of Hubbard model (Coulomb interactions are treated by means of the Hartree-Fock approximation), while the coupling to the electrodes is modeled through the use of a broad-band theory. It was shown that magnetoresistance varies periodically with increasing the length of atomic wire (in the linear response regime) and oscillates with incre…
Using non-equilibrium Green's functions, we derive a formula for the electron current through a lead-molecule-lead nanojunction where the interactions are not restricted to the central region, but are spread throughout the system, including the leads and the lead-molecule interfaces. The current expression consists of two sets of terms. The first set corresponds to a generalised Meir and Wingreen expression where the leads' self-energies are renormalised by the interactions crossing at the molecule-lead contacts. The second set corresponds to inelastic scattering events in the leads arising fr…
We report a theoretical study suggesting a novel type of electronic switching effect, driven by the geometrical reconstruction of nanoscale graphene-based junctions. We considered junction struc- tures which have alternative metastable configurations transformed by rotations of local carbon dimers. The use of external mechanical strain allows a control of the energy barrier heights of the potential profiles and also changes the reaction character from endothermic to exothermic or vice-versa. The reshaping of the atomic details of the junction encode binary electronic ON or OFF states, with ON/…
We overview nonequilibrium Green function combined with density functional theory (NEGF-DFT) modeling of independent electron and phonon transport in nanojunctions with applications focused on a new class of thermoelectric devices where a single molecule is attached to two metallic zigzag graphene nanoribbons (ZGNRs) via highly transparent contacts. Such contacts make possible injection of evanescent wavefunctions from ZGNRs, so that their overlap within the molecular region generates a peak in the electronic transmission. Additionally, the spatial symmetry properties of the transverse propaga…
We investigate a novel way to manipulate the spin polarized transmission in a two terminal zigzag graphene nanoribbon in presence of Rashba spin-orbit (SO) interaction with circular shaped cavity engraved into it. A usual technique to control the spin polarized transport behaviour of a nanoribbon can be achieved by tuning the strength of the SO coupling, while we show that an efficient engineering of the spin polarized transport properties can also be done via cavities of different radii engraved in the nanoribbon. Simplicity of the technique in creating such cavities in the experiments render…
Understanding the process of electron tunneling in chirality-induced single-molecule junctions is imperative for the development of nanoscale switching and artificial nanomotors. Based on the combined non-equilibrium Green functions formalism and the ground-state density functional theory, we present here the charge transport behavior of chiral gold (7,3) nanowires (NWs) in comparison with various other chiral and achiral 1D gold nanostructures as the principal leads to form stable single-molecule junctions. For sigma-saturated alkane chains, we find that the contact potential barriers vary wi…
We study spin-dependent electronic transport across ferromagnet/superconductor ballistic junctions modeled using tight-binding Hamiltonians with s, p and d orbitals and material-specific parameters. We show that by accurately modeling the band structure of the bulk materials, one can reproduce the measured differential conductance of Cu/Pb nanocontacts. In contrast the differential conductance of Co/Pb contacts can only be reproduced if an enhanced magnetic moment is present at the interface.
The correlation between transport properties across sub-nanometric metallic gaps and the optical response of the system is a complex effect which is determined by the fine atomic-scale details of the junction structure. As experimental advances are progressively accessing transport and optical characterization of smaller nanojunctions, a clear connection between the structural, electronic and optical properties in these nanocavities is needed. Using ab initio calculations, we present here a study of the simultaneous evolution of the structure and the optical response of a plasmonic junction as…
We present a nonperturbative and formally exact approach for the charge transport in interacting nanojunctions based on a real time path integral formulation of the reduced system dynamics. An expansion of the influence functional in terms of the number of tunneling transitions, and integration of the Grassmann variables between the tunneling times, allows us to obtain a still exact generalized master equation (GME) for the populations of the reduced density matrix (RDM) in the occupation number representation, as well as a formally exact expression for the current. By borrowing the nomenclatu…
The operation of many classical and quantum systems in nonequilibrium steady state is constrained by cost-precision (dissipation-fluctuation) tradeoff relations, delineated by the thermodynamic uncertainty relation (TUR). However, coherent quantum electronic nanojunctions can escape such a constraint, showing finite charge current and nonzero entropic cost with vanishing current fluctuations. Here, we analyze the absence, and restoration, of cost-precision tradeoff relations in fermionic nanojunctions under different affinities: voltage and temperature biases. With analytic work and simulation…
We report here the charge transport behavior in graphene nanojunctions in which graphene nanodots, with relatively long relaxation time, are interfaced with ferromagnetic electrodes. Subsequently we explore the effect of substitutional doping of transition metal atoms in zigzag graphene nanodots (z-GNDs) on the charge transport under non-collinear magnetization. Only substitutional doping of transition metal atoms in z-GNDs at certain sites demonstrates the spin filtering effect with a large tunnelling magnetoresistance as high as 700%, making it actually suitable for spintronic applications. …
We consider the electron transport properties through fully interacting nanoscale junctions beyond the linear-response regime. We calculate the current flowing through an interacting region connected to two interacting leads, with interaction crossing at the left and right contacts, by using a non-equilibrium Green's functions (NEGF) technique. The total current at one interface (the left one for example) is made of several terms which can be regrouped into two sets. The first set corresponds to a very generalised Landauer-like current formula with physical quantities defined only in the inter…
We study the effect of system reservoir coupling on currents flowing through quantum junctions. We consider two simple double-quantum dot configurations coupled to two external fermionic reservoirs and study the net current flowing between the two reservoirs. The net current is partitioned into currents carried by the eigenstates of the system and by the coherences between the eigenstates induced due to coupling with the reservoirs. We find that current carried by populations is always positive whereas current carried by coherences are negative for large couplings. This results in a non-monoto…
Rectification of heat transfer in nanodevices can be realized by combining the system inherent anharmonicity with structural asymmetry. we analyze this phenomenon within the simplest anharmonic system -a spin-boson nanojunction model. We consider two variants of the model that yield, for the first time, analytical solutions: a linear separable model in which the heat reservoirs contribute additively, and a non-separable model suitable for a stronger system-bath interaction. Both models show asymmetric (rectifying) heat conduction when the couplings to the heat reservoirs are different.
A model is presented for the quantum transport of electrons, across finite atomic wire nanojunctions between electric leads, at zero bias limit. In order to derive the appropriate transmission and reflection spectra, familiar in the Landauer-Büttiker formalism, we develop the algebraic phase field matching theory (PFMT). In particular, we apply our model calculations to determine the electronic conductance for freely suspended monatomic linear sodium wires (MLNaW) between leads of the same element, and for the diatomic copper-cobalt wires (DLCuCoW) between copper leads on a Cu(111) substrate. …
We present a formulation of a nonequilibrium Green's function method for thermal current in nanojunction atomic systems with nonlinear interactions. This first-principle approach is applied to the calculation of the thermal conductance in carbon nanotube junctions. It is shown that nonlinearity already becomes important at low temperatures. Nonlinear interactions greatly suppress phonon transmission at room temperature. The peak of thermal conductance is found to be around 400K, in good agreement with experiments. High-order phonon scattering processes are important for diffusive heat transpor…
We present a hierarchical quantum master equation (HQME) approach, which allows the numerically exact evaluation of higher-order current cumulants in the framework of full counting statistics for nonequilibrium charge transport in nanosystems. The novel methodology is exemplarily applied to a model of vibrationally coupled electron transport in a molecular nanojunction. We investigate the influence of cotunneling on avalanche-like transport, in particular in the nonresonant transport regime, where we find that inelastic cotunneling acts as trigger process for resonant avalanches. In this regim…
We investigate the quantum heat exchange between a nanojunction and a many-body or electromagnetic environment far from equilibrium. It is shown that the two-temperature energy emission-absorption mechanism gives rise to a giant heat flow between the junction and the environment. We obtain analytical results for the heat flow in an idealized high impedance environment and perform numerical calculations for the general case of interacting electrons and discuss the giant freezing and heating effects in the junction under typical experimental conditions.
Optical techniques have been employed to coherently control the quantum transport through nanojunctions. Conventional works on optical control of quantum transport usually applied a tailored electrical pulses to perform specific tasks. In this work, an opposite way is employed and a time-dependent driving field is searched to force the system behave in desired pattern. In order to achieve the goal, an optimal control theory for time-dependent quantum transport is developed. The theory provides a theoretical tool for the design of driving field to control the transient current through a nano ju…
Here we present a theoretical analysis of the effect of inelastic electron scattering on spin-dependent transport characteristics (conductance, current-voltage dependence, magnetoresistance, shot noise spectrum, Fano factor) for magnetic nanojunction. Such device is composed of molecular quantum dot (with discrete energy levels)connected to ferromagnetic electrodes (treated within the wide-band approximation), where molecular vibrations are modeled as dispersionless phonons. Non-perturbative computational scheme, used in this work, is based on the Green's function theory within the framework o…
In this paper, we present a Hamiltonian and thermodynamic theory of heat transport on various levels of description. Transport of heat is formulated within kinetic theory of polarized phonons, kinetic theory of unpolarized phonons, hydrodynamics of polarized phonons, and hydrodynamics of unpolarized phonons. These various levels of description are linked by Poisson reductions, where no linearizations are made. Consequently, we obtain a new phonon hydrodynamics that contains convective terms dependent on vorticity of the heat flux, which are missing in the standard theories of phonon hydrodynam…
There has been much interest in semiconductor superlattices because of showing very low thermal conductivities. This makes them especially suitable for applications in a variety of devices for thermoelectric generation of energy, heat control at the nanometric length scale, etc. Recent experiments have confirmed that the effective thermal conductivity of superlattices at room temperature have a minimum for very short periods (in the order of nanometers) as some kinetic calculations had anticipated previously. This work will show advances on a thermodynamic theory of heat transport in nanometri…
We introduce a new thermal transport phenomenon, a unidirectional selection-rule blockade, and show how it produces unprecedented rectification of bosonic heat flow through molecular or mesoscopic quantum systems. Rectification arises from the quantization of energy levels of the conduction element and selection rules of reservoir coupling operators. The simplest system exhibiting the selection-rule blockade is an appropriately coupled three-level system, providing a candidate for a high-performance heat diode. We present an analytical treatment of the transport problem and discuss how the phe…
We show that in mesoscopic four-terminal thermoelectric devices with two electrodes (the source and the drain) and two heat baths, inelastic scattering processes can lead to unconventional thermoelectric transport. The source (or the drain) can be cooled by passing a thermal current between the two heat baths, with no net heat exchange between the heat baths and the electrodes. This effect, termed as cooling by heat current, is a mesoscopic heat drag effect. In addition, there is a transverse thermoelectric effect where electrical current and power can be generated by a transverse temperature …
We study the statistics of thermal energy transfer in the nonequilibrium (two-bath) spin-boson model. This quantum many-body impurity system serves as a canonical model for quantum energy transport. Our method makes use of the Majorana fermion representation for the spin operators, in combination with the Keldysh nonequilibrium Green's function approach. We derive an analytical expression for the cumulant generating function of the model in the steady state limit, and show that it satisfies the Gallavotti-Cohen fluctuation symmetry. We obtain analytical expressions for the heat current and its…
We study classical heat conduction in a dissipative open system composed of interacting oscillators. By exactly solving a twisted Fokker-Planck equation which describes the full counting statistics of heat flux flowing through the system, we identify the geometric-phase-like effect and examine its impact on the classical heat transport. Particularly, we find that the nonlinear interaction as well as the closely related temperature-dependence of system-parameters are crucial in manifesting the geometric-phase contribution of heat flux. Finally, we propose an electronic experiment based on RC ci…
In this colloquia review we discuss methods for thermal transport calculations for nanojunctions connected to two semi-infinite leads served as heat-baths. Our emphases are on fundamental quantum theory and atomistic models. We begin with an introduction of the Landauer formula for ballistic thermal transport and give its derivation from scattering wave point of view. Several methods (scattering boundary condition, mode-matching, Piccard and Caroli formulas) of calculating the phonon transmission coefficients are given. The nonequilibrium Green's function (NEGF) method is reviewed and the Caro…
We study electron transport in nanojunctions in which an electron on a quantum dot or a molecule is interacting with an N-state local impurity, a harmonic ("Holstein") mode, or a two-state system ("spin"). These two models, the Anderson-Holstein model and the spin-fermion model, can be conveniently transformed by a shift transformation into a form suitable for a perturbative expansion in the tunneling matrix element. We explore the current-voltage characteristics of the two models in the limit of high temperature and weak electron-metal coupling using a kinetic rate equation formalism, conside…
Molecular dynamics simulations and nonequilibrium importance sampling are used to study the heat transport of low dimensional carbon lattices. For both carbon nanotubes and graphene sheets heat transport is found to be anomalous, violating Fourier's law of conduction with a system size dependent thermal conductivity and concomitant nonlinear temperature profiles. For carbon nanotubes, the thermal conductivity is found to increase as the square root of the length of the nanotube, while for graphene sheets the thermal conductivity is found to increase as the logarithm of the length of the sheet.…
Developing simplified, but accurate, theoretical approaches to treat heat transport on all length and time scales is needed to further enable scientific insight and technology innovation. Using a simplified form of the Boltzmann transport equation (BTE), originally developed for electron transport, we demonstrate how ballistic phonon effects and finite-velocity propagation are easily and naturally captured. We show how this approach compares well to the phonon BTE, and readily handles a full phonon dispersion and energy-dependent mean-free-path. This study of transient heat transport shows i) …
Heat transport in the quantum Hall regime is investigated using micron-scale heaters and thermometers positioned along the edge of a millimeter-scale two dimensional electron system (2DES). The heaters rely on localized current injection into the 2DES, while the thermometers are based on the thermoelectric effect. In the $ν= 1$ integer quantized Hall state, a thermoelectric signal appears at an edge thermometer only when it is "downstream," in the sense of electronic edge transport, from the heater. When the distance between the heater and the thermometer is increased, the thermoelectric signa…
We study nondiffusive thermal transport by phonons at small distances within the framework of the Boltzmann transport equation (BTE) and demonstrate that the transport is significantly affected by the distribution of phonons emitted by the source. We discuss analytical solutions of the steady-state BTE for a source with a sinusoidal spatial profile, as well as for a three- dimensional Gaussian hot spot, and provide numerical results for single crystal silicon at room temperature. If a micro/nanoscale heat source produces a thermal phonon distribution, it gets hotter than predicted by the heat …
Heat transport by acoustic phonons in 2D materials is fundamentally different from that in 3D crystals because the out-of-plane phonons propagate in a unique way that strongly depends on tension and bending rigidity. Since in-plane and out-of-plane phonon baths are decoupled, initial studies suggested they provide independent pathways for heat transport and storage in 2D materials. Here, we induce tension in freestanding graphene membranes by electrostatic force, and use optomechanical techniques to demonstrate that it can change the rate of heat transport by as much as 33%. Using a ballistic …
We demonstrate a direct approach to investigate heat transport in the fractional quantum Hall regime. At filling factor of 4/3, we inject power at quantum point contacts and detect the related heating from the activated current through a quantum dot. The experiment reveals a chargeless heat transport from a significant heating that occurs upstream of the power injection point, in the absence of a concomitant electrical current. By tuning in-situ the edge path, we show that the chargeless heat transport does not follow the reverse direction of the electrical current path along the edge. This un…
Unlike classical heat diffusion at the macroscale, nanoscale heat transport can occur without energy dissipation because phonons can travel in straight lines for hundreds of nanometres. Despite recent experimental evidence of such ballistic phonon transport, control over its directionality, and thus its practical use, remains a challenge, as the directions of individual phonons are chaotic. Here, we show a way to control the directionality of ballistic phonon transport using silicon thin-films with arrays of holes. First, we demonstrate the formation of directional heat fluxes in the passages …
We study heat transport in quantum spin systems analytically and numerically. First, we demonstrate that heat current through a two-level quantum spin system can be modulated from zero to a finite value by tuning a magnetic field. Second, we show that a spin system, consisting of two dissimilar parts - one is gapped and the other is gapless, exhibits current rectification and negative differential thermal resistance. Possible experimental realizations by using molecular junctions or magnetic materials are discussed.
We investigate nonlinear heat properties in mesoscopic conductors using a scattering theory of transport. Our approach is based on a leading-order expansion in both the electrical and thermal driving forces. Beyond linear response, the transport coefficients are functions of the nonequilibrium screening potential that builds up in the system due to interactions. Within a mean-field approximation, we self-consistently calculate the heat rectification properties of a quantum dot attached to two terminals. We discuss nonlinear contributions to the Peltier effect and find departures from the Wiede…
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 o…
We investigate heat transport through an assembly consisting of a two-level system coupled between two harmonic oscillators, which is described by the quantum Rabi model, as a prototype of nanoscale heat devices using controllable multi-level systems. Using the noninteracting-blip approximation (NIBA), we find that the linear thermal conductance shows a characteristic temperature dependence with a two-peak structure. We also show that heat transport is sensitive to model parameters for weak system-bath coupling and strong hybridization between the two-level system and the harmonic oscillators.…
We show that the local temperature dependence of thermalized electron and phonon populations along metallic carbon nanotubes is the main reason behind this non-linear transport characteristics in the high bias regime. Our model that considers optical and zone boundary phonon emission as well as absorption by charge carriers is based on the solution of the Boltzmann transport equation that assumes a local temperature along the nanotube, determined self-consistently with the heat transport equation. By using realistic transport parameters, our results not only reproduce experimental data for ele…
Nonlinear transport coefficients do not obey, in general, reciprocity relations. We here discuss the magnetic-field asymmetries that arise in thermoelectric and heat transport of mesoscopic systems. Based on a scattering theory of weakly nonlinear transport, we analyze the leading-order symmetry parameters in terms of the screening potential response to either voltage or temperature shifts. We apply our general results to a quantum Hall antidot system. Interestingly, we find that certain symmetry parameters show a dependence on the measurement configuration.
