We report first-principles calculations of local heating in nanoscale junctions formed by a single molecule and a gold point contact. Due to a larger heat dissipation, the single molecule heats up less than the gold point contact. We also find, at zero temperature, a threshold bias $V_{onset}$ of about 6 mV and 11 mV for the molecule and the point contact, respectively, is required to excite the smallest vibrational mode and generate heat. The latter estimate is in very good agreement with recent experimental results on the same system. At a given external bias $V$ below $V_{onset}$, heating becomes noticeable when the background temperature is on the order of $\sim e(V_{onset}-V)/k_{B}$. Above $V_{onset}$, local heating increases dramatically with increasing bias but is also considerably suppressed by thermal dissipation into the electrodes. The results provide a microscopic picture of current-induced heat generation in atomic-scale structures.
We present an overview of current-induced effects in nanoscale conductors with emphasis on their description at the atomic level. In particular, we discuss steady-state current fluctuations, current-induced forces, inelastic scattering and local heating. All of these properties are calculated in terms of single-particle wavefunctions computed using a scattering approach within the static density-functional theory of many-electron systems. Examples of current-induced effects in atomic and molecular wires will be given and comparison with experimental results will be provided when available.
I argue that the geometric phase, responsible for reversible pump currents in classical stochastic kinetics, can be observed experimentally with an electronic setup, similar to the ones reported recently in [Phys. Rev. Lett. 96,076605 (2006)] and [Nature Physics 3, 243 - 247 (2007)].
We present a formalism to calculate finite-frequency current correlations in interacting nanoscale conductors. We work within the n-resolved density matrix approach and obtain a multi-time cumulant generating function that provides the fluctuation statistics, solely from the spectral decomposition of the Liouvillian. We apply the method to the frequency-dependent third cumulant of the current through a single resonant level and through a double quantum dot. Our results, which show that deviations from Poissonian behaviour strongly depend on frequency, demonstrate the importance of finite-frequ…
The electron current density in nanoscale junctions is typically several orders of magnitude larger than the corresponding one in bulk electrodes. Consequently, the electron-electron scattering rate increases substantially in the junction. This leads to local electron heating of the underlying Fermi sea in analogy to the local ionic heating that is due to the increased electron-phonon scattering rates. We predict the bias dependence of local electron heating in quasi-ballistic nanoscale conductors, its effect on ionic heating, and discuss possible experimental tests of our results.
Theoretical description of the field emission of electrons from nanoscale objects weakly coupled to the cathode is presented. It is shown that the field- emission current increases in a step-like fashion due to single-electron charging which leads to abrupt changes of the effective electric field responsible for the field emission. A detailed consideration of the current-voltage characteristics is carried out for a nanocluster modelled by a metallic spherical particle in the close vicinity of the cathode and for a cylindrical silicon nanowire grown on the cathode surface.
Accelerated Discovery of Topological Conductors for Nanoscale Interconnects
NORDITA, KTH Royal Institute of Technology and Stockholm University（北欧理论粒子物理研究所，皇家理工学院和斯德哥尔摩大学）；University of Connecticut（康涅狄格大学）；Northwestern University（西北大学）；IBM Thomas J. Watson Research Center（IBM托马斯·J·沃森研究中心）；National Yang Ming Chiao Tung University（国立阳明交通大学）；Academia Sinica（中央研究院）
The description of electron-electron interactions in transport problems is both analytically and numerically difficult. Here we show that a much simpler description of electron transport in the presence of interactions can be achieved in nanoscale systems. In particular, we show that the electron flow in nanoscale conductors can be described by Navier-Stokes type of equations with an effective electron viscosity, i.e., on a par with the dynamics of a viscous and compressible classical fluid. By using this hydrodynamic approach we derive the conditions for the transition from laminar to turbule…
We describe a field-theoretic approach to calculate quantum shot noise in nanoscale conductors from first principles. Our starting point is the second-quantization field operator to calculate shot noise in terms of single quasi-particle wavefunctions obtained self-consistently within density functional theory. The approach is valid in both linear and nonlinear response and is particularly suitable in studying shot noise in atomic-scale conductors. As an example we study shot noise in Si atomic wires between metal electrodes. We find that shot noise is strongly nonlinear as a function of bias a…
The theory for current fluctuations in ac-driven transport through nanoscale systems is put forward. By use of a generalized, non-Hermitian Floquet theory we derive novel explicit expressions for the time-averaged current and the zero-frequency component of the power spectrum of current fluctuations. A distinct suppression of both the zero-frequency noise and the dc-current occurs for suitably tailored ac-fields. The relative level of transport noise, being characterized by a Fano factor, can selectively be manipulated by ac-sources; in particular, it exhibits both characteristic maxima and mi…
In this work, we study thermal conductivity (k) of BC5, an ultra-hard diamondlike semiconductor material, using first-principles computations and analyze the effect of both isotopic disorder as well as length scale dependence. k of isotopically pure BC5 is computed to be 169 Wm- 1K-1 (along a-axis) at 300K; this high k is found to be due to the high frequencies and phonon group velocities of both acoustic and optical phonons owing to the light atomic mass of Carbon (C) and Boron (B) atoms and strong C-C and B-C bonds. We also observe a dominance of optical phonons (~ 54%) over acoustic phonons…
We derive within a time-dependent scattering formalism expressions for both the current through ac-driven nanoscale conductors and its fluctuations. The results for the time-dependent current, its time average, and, above all, the driven shot noise properties assume an explicit and serviceable form by relating the propagator to a non-Hermitian Floquet theory. The driven noise cannot be expressed in terms of transmission probabilities. The results are valid for a driving of arbitrary strength and frequency. The connection with commonly known approximation schemes such as the Tien-Gordon approac…
We show, using a tight-binding model and time-dependent density-functional theory, that a quasi-steady state current can be established dynamically in a finite nanoscale junction without any inelastic effects. This is simply due to the geometrical constriction experienced by the electron wavepackets as they propagate through the junction. We also show that in this closed non-equilibrium system two local electron occupation functions can be defined on each side of the nanojunction which approach Fermi distributions with increasing number of atoms in the electrodes. The resultant conductance and…
We analyze the short-time behavior of the heat and charge currents through nanoscale conductors exposed to a temperature gradient. To this end, we employ Luttinger's thermomechanical potential to simulate a sudden change of temperature at one end of the conductor. We find that the direction of the charge current through an impurity is initially opposite to the direction of the charge current in the steady-state limit. Furthermore, we investigate the transient propagation of energy and particle density driven by a temperature variation through a conducting nanowire. Interestingly, we find that …
Recent experimental progress in coupling nanoscale conductors to superconducting microwave cavities has opened up for transport investigations of the deep quantum limit of light-matter interactions, with tunneling electrons strongly coupled to individual cavity photons. We have investigated theoretically the most basic cavity-conductor system with strong, single photon induced non-local transport effects; two spatially separated double quantum dots (DQD:s) resonantly coupled to the fundamental cavity mode. The system, described by a generalized Tavis-Cummings model, is investigated within a qu…
We consider the Johnson noise of a two-dimensional, two-terminal electrical conductor for which the electron system obeys the Wiedemann-Franz law. We derive two simple and generic relations between the Johnson Noise temperature and the heat flux into the electron system. First, we consider the case where the electron system is heated by Joule heating from a DC current, and we show that there is a universal proportionality coefficient between the Joule power and the increase in Johnson noise temperature. Second, we consider the case where heat flows into the sample from an external source, and …
We investigate the noise properties of pump currents through molecular wires and coupled quantum dots. As a model we employ a two level system that is connected to electron reservoirs and is non-adiabatically driven. Concerning the electron-electron interaction, we focus on two limits: non-interacting electrons and strong Coulomb repulsion. While the former case is treated within a Floquet scattering formalism, we derive for the latter case a master equation formalism for the computation of the current and the zero-frequency noise. For a pump operated close to internal resonances, the differen…
Thermoelectric transport in nanoscale conductors is analyzed in terms of the response of the system to a thermo-mechanical field, first introduced by Luttinger, which couples to the electronic energy density. While in this approach the temperature remains spatially uniform, we show that a spatially varying thermo-mechanical field effectively simulates a temperature gradient across the system and allows us to calculate the electric and thermal currents that flow due to the thermo-mechanical field. In particular, we show that, in the long-time limit, the currents thus calculated reduce to those …
Thermoelectric effects allow the generation of electrical power from waste heat and the electrical control of cooling and heating. Remarkably, these effects are also highly sensitive to the asymmetry in the density of states around the Fermi energy and can therefore be exploited as probes of distortions in the electronic structure at the nanoscale. Here we consider two-dimensional graphene as an excellent nanoscale carbon material for exploring the interaction between electronic and thermal transport phenomena, by presenting a direct and quantitative measurement of the Peltier component to ele…
Solid state ionic conductors are good candidates for the next generation of nonvolatile computer memory elements. Such devices have to show reproducible resistance switching at reasonable voltage and current values even if scaled down to the nanometer sizes. Here we study the switching characteristics of nanoscale junctions created between a tungsten tip and a silver film covered by a thin ionic conductor layer. Atomic-sized junctions show spectacular current induced switching characteristics, but both the magnitude of the switching voltage and the direction of the switching vary randomly for …
We investigate the heat flow between different terminals in an interacting coherent conductor when inelastic scattering is present. We illustrate our theory with a two-terminal quantum dot setup. Two types of heat asymmetries are investigated: electric asymmetry $Δ_E$, which describes deviations of the heat current in a given contact when voltages are exchanged, and contact asymmetry $Δ_C$, which quantifies the difference between the power measured in two distinct electrodes. In the linear regime, both asymmetries agree and are proportional to the Seebeck coefficient, the latter following at l…
Interactions between nanoscale semiconductor structures form the basis for charge detectors in the solid state. Recent experimental advances have demonstrated the on-chip detection of single electron transport through a quantum dot (QD). The discreteness of charge in units of e leads to intrinsic fluctuations in the electrical current, known as shot noise. To measure these single-electron fluctuations a nearby coherent conductor, called a quantum point contact (QPC), interacts with the QD and acts as a detector. An important property of the QPC charge detector is noninvasiveness: the system ph…
We report first-principles calculations of inelastic Seebeck coefficients in an aluminum monatomic junction. We compare the elastic and inelastic Seebeck coefficients with and without local heating. In the low temperature regime, the signature of normal modes in the profiles of the inelastic Seebeck effects is salient. The inelastic Seebeck effects are enhanced by the normal modes, and further magnified by local heating. In the high temperature regime, the inelastic Seebeck effects are weakly suppressed due to the quasi-ballistic transport.
We perform classical non-equilibrium molecular dynamics simulations to calculate heat flow through a microscopic junction connecting two larger reservoirs. In contrast to earlier works, we also include the reservoirs in the simulated region to study the effect of the bulk-nanostructure interfaces and the bulk conductance. The scalar Fermi--Pasta--Ulam (FPU) model is used to describe the effects of anharmonic interactions in a simple manner. The temperature profile close to the junction in the low temperature limit is shown to exhibit strong directional features that fade out when temperature i…
In nanoscale junctions the interaction between charge carriers and the local vibrations results in renormalization, damping and heating of the vibrational modes. We here formulate a nonequilibrium Green's functions based theory to describe such effects. Studying a generic junction model with an off-resonant electronic level, we find a strong bias dependence of the frequency renormalization and vibrational damping accompanied by pronounced nonlinear vibrational heating in junctions with intermediate values of the coupling to the leads. Combining our theory with ab-initio calculations we further…
We analyze the benefits and shortcomings of a thermal control in nanoscale electronic conductors by means of the contact heating scheme. Ideally, this straightforward approach allows one to apply a known thermal bias across nanostructures directly through metallic leads, avoiding conventional substrate intermediation. We show, by using the average noise thermometry and local noise sensing technique in InAs nanowire based devices, that a nanoscale metallic constriction on a SiO2 substrate acts like a diffusive conductor with negligible electron-phonon relaxation and non-ideal leads. The non-uni…
Understanding and controlling the flow of heat is a major challenge in nanoelectronics. When a junction is driven out of equilibrium by light or the flow of electric charge, the vibrational and electronic degrees of freedom are, in general, no longer described by a single temperature[1-6]. Moreover, characterizing the steady-state vibrational and electronic distributions {\it in situ} is extremely challenging. Here we show that surface-enhanced Raman emission may be used to determine the effective temperatures for both the vibrational modes and the flowing electrons in a biased metallic nanosc…
We investigate the different boiling régimes around a single continuously laser-heated 80 nm gold nanoparticle and draw parallels to the classical picture of boiling. Initially, nanoscale boiling takes the form of transient, inertia-driven, unsustainable boiling events characteristic of a nanoscale boiling crisis. At higher heating power, nanoscale boiling is continuous, with a vapor film being sustained during heating for at least up to 20 $μ$s. Only at high heating powers does a substantial stable vapour nanobubble form. At intermediate heating powers, unstable boiling sometimes takes the fo…
We study a three-terminal setup consisting of a single-level quantum dot capacitively coupled to a quantum point contact. The point contact connects to a source and drain reservoirs while the quantum dot is coupled to a single base reservoir. This setup has been used to implement a noninvasive, nanoscale thermometer for the bath reservoir by detecting the current in the quantum point contact. Here, we demonstrate that the device can also be operated as a thermal transistor where the average (charge and heat) current through the quantum point contact is controlled via the temperature of the bas…
Manipulating materials at the nanometer scale is challenging, particularly if alignment with nanoscale electrodes is desired. Here we describe a lithography-free, self-aligned nanotrench ablation (SANTA) technique to create nanoscale trenches in a polymer like poly(methyl) methacrylate (PMMA). The nanotrenches are self-aligned with carbon nanotube (CNT) and graphene ribbon electrodes through a simple Joule heating process. Using simulations and experiments we investigate how the Joule power, ambient temperature, PMMA thickness, and substrate properties can improve the spatial resolution of thi…
We investigate theoretically the interplay of current-induced forces (CIF), Joule heating, and heat transport inside a current-carrying nano-conductor. We find that the CIF, due to the electron-phonon coherence, can control the spatial heat dissipation in the conductor. This yields a significant asymmetric concentration of excess heating (hot-spot) even for a symmetric conductor. When coupled to the electrode phonons, CIF drive different phonon heat flux into the two electrodes. First-principles calculations on realistic biased nano-junctions illustrate the importance of the effect.
We propose a thermoelectric cooling device based on an atomic-sized junction. Using first-principles approaches, we investigate the working conditions and the coefficient of performance (COP) of an atomic-scale electronic refrigerator where the effects of phonon's thermal current and local heating are included. It is observed that the functioning of the thermoelectric nano-refrigerator is restricted to a narrow range of driving voltages. Compared with the bulk thermoelectric system with the overwhelmingly irreversible Joule heating, the 4-Al atomic refrigerator has a higher efficiency than a b…
Heating in nanoscale systems driven out of equilibrium is of fundamental importance, has ramifications for technological applications, and is a challenge to characterize experimentally. Prior experiments using nanoscale junctions have largely focused on heating of ionic degrees of freedom, while heating of the electrons has been mostly neglected. We report measurements in atomic-scale Au break junctions, in which the bias-driven component of the current noise is used as a probe of the electronic distribution. At low biases ($<$ 150~mV) the noise is consistent with expectations of shot noise at…
We determine the temperature profile in magnetic nanocontacts submitted to the very large current densities that are commonly used for spin-torque oscillator behavior. Experimentally, the quadratic current-induced increase of the resistance through Joule heating is independent of the applied temperature from 6 K to 300 K. The modeling of the experimental rate of the current-induced nucleation of a vortex under the nanocontact, assuming a thermally-activated process, is consistent with a local temperature increase between 150 K and 220 K. Simulations of heat generation and diffusion for the act…
We investigate the effect of electron-phonon inelastic scattering on shot noise in nanoscale junctions in the regime of quasi-ballistic transport. We predict that when the local temperature of the junction is larger than its lowest vibrational mode energy $eV_c$, the inelastic contribution to shot noise (conductance) increases (decreases) with bias as $V$ ($\sqrt{V}$). The corresponding Fano factor thus increases as $\sqrt{V}$. We also show that the inelastic contribution to the Fano factor saturates with increasing thermal current exchanged between the junction and the bulk electrodes to a va…
The Thomson effect induces heat release or absorption under the simultaneous application of a charge current and a temperature gradient to conductors. Here, we theoretically investigate the temperature profile due to the Thomson-effect-induced heat release/absorption in junctionless single conductors which can be a simple temperature modulator. We also perform analysis of the temperature profile for realistic conductors. As a result, we find that, for a conductor with a large Thomson coefficient, the temperature derivative of the Seebeck coefficient, the Thomson-effect-induced heat absorption …
Nanoscale mapping of internal magnetization dynamics reveals how disorder shapes heat generation in magnetic particle hyperthermia
University of Luxembourg（卢森堡大学）；Ghent University（根特大学）；Instituto de Ciencia de Materiales de Madrid (ICMM-CSIC)（马德里材料科学研究所）；Physikalisch-Technische Bundesanstalt（德国联邦物理技术研究院）
We study the effect of localized Joule heating on the mechanical properties of doubly clamped nanowires under tensile stress. Local heating results in systematic variation of the resonant frequency; these frequency changes result from thermal stresses that depend on temperature dependent thermal conductivity and expansion coefficient. The change in sign of the linear expansion coefficient of InAs is reflected in the resonant response of the system near a bath temperature of 20 K. Using finite element simulations to model the experimentally observed frequency shifts, we show that the thermal co…
The rate at which excited charge carriers relax to their equilibrium state affects many aspects of the performance of nanoscale devices, including switching speed, carrier mobility and luminescent efficiency. Better understanding of the processes that govern carrier relaxation therefore has important technological implications. A significant increase in carrier-carrier interactions caused by strong spatial confinement of electronic excitations in semiconductor nanostructures leads to a considerable enhancement of Auger effects, which can further result in unusual, Auger-process-controlled reco…
Temperature imaging of nanoscale systems is a fundamental problem which has myriad potential technological applications. For example, nanoscopic cold spots can be used for spot cooling electronic components while hot spots could be used for precise activation of chemical or biological reactions. More fundamentally, imaging the temperature fields in quantum coherent conductors can provide a wealth of information on heat flow and dissipation at the smallest scales. However, despite significant technological advances, the spatial resolution of temperature imaging remains in the few nanometers ran…
Rectification of thermal fluctuations in mesoscopic conductors is the key idea of today's attempts to build nanoscale thermoelectric energy harvesters in order to convert heat into a useful electric power. So far, most concepts make use of the Seebeck effect in a two-terminal geometry where heat and charge are both carried by the same particles. Here, we experimentally demonstrate the working principle of a new kind of energy harvester, proposed recently using two capacitively coupled quantum dots. We show that due to its novel three-terminal design which spatially separates the heat reservoir…
Controlling the temperature in architectures involving nanoparticles and substrates is a key issue for applications involving micro and nanoscale heat transfer. We study the thermal behavior of a single nanoparticle interacting with a flat substrate under external monochromatic illumination, and with thermal radiation as the unique heat loss channel. We develop a model to compute the temperature of the nanoparticle, based on an effective dipole-polarizability approach. Using numerical simulations, we thoroughly investigate the impacts of various parameters affecting the nanoparticle temperatur…
We theoretically investigate the effect of inter-molecular Coulomb interactions on transport through molecular monolayers (or other devices based on a large number of nanoscale conductors connected in parallel). Due to the interactions, the current through different molecules become correlated, resulting in distinct features in the non-linear current-voltage characteristics, as we show by deriving and solving a type of modified master equation, suitable for describing transport through an infinite number of interacting conductors. Furthermore, if some of the molecules fail to bond to both elec…
We propose and analyze the use of hybrid microwave cavities as quantum heat engines. A possible realization consists of two macroscopically separated quantum dot conductors coupled capacitively to the fundamental mode of a microwave cavity. We demonstrate that an electrical current can be induced in one conductor through cavity-mediated processes by heating up the other conductor. The heat engine can reach Carnot efficiency with optimal conversion of heat to work. When the system delivers the maximum power, the efficiency can be a large fraction of the Carnot efficiency. The heat engine functi…
The phonon Boltzmann transport equation (BTE) has been widely utilized to study thermal transport in solids. While for a number of materials the exact solution to the BTE has been obtained for a uniform heat flow, problems arising in micro/nanoscale heat transport have been analyzed within the relaxation time approximation (RTA). Since the RTA breaks down at temperatures low compared to the Debye temperature, this approximation prevents the study of an important class of high Debye temperature materials such as diamond, graphite, graphene and some other 2D materials. We present a full scatteri…
Heat production and dissipation induced by current flow in nanostructures is of primary importance to understand the stability of these systems. These effects have contributions from both electron-phonon and electron-electron interactions. Here, we consider the effect of the local electron and ionic heating on the conductance of nanoscale systems. Specifically we show that the non-linear dependence of the conductance on the external bias may be used to infer information about the local heating of both electrons and ions. We compare our results with available experimental data on transport in $…
Heat management and refrigeration are key concepts for nanoscale devices operating at cryogenic temperatures. The design of an on-chip mesoscopic refrigerator that works thanks to the input heat is presented, thus realizing a solid state implementation of the concept of cooling by heating. The system consists of a circuit featuring a thermoelectric element based on a ferromagnetic insulator-superconductor tunnel junction (N-FI-S) and a series of two normal metal-superconductor tunnel junctions (SINIS). The N-FI-S element converts the incoming heat in a thermovoltage, which is applied to the SI…
Heat transport in nanoscale systems is both hard to measure microscopically, and hard to interpret. Ballistic and diffusive heat flow coexist, adding confusion. This paper looks at a very simple case: a nanoscale crystal repeated periodically. This is a popular model for simulation of bulk heat transport using classical molecular dynamics (MD), and is related to transient thermal grating experiments. Nanoscale effects are seen in perhaps their simplest form. The model is solved by an extension of standard quasiparticle gas theory of bulk solids. Both structure and heat flow are constrained by …
Quantum thermocouples: nonlocal conversion and control of heat in nanostructures
Universidad Autónoma de Madrid（马德里自治大学）；Condensed Matter Physics Center (IFIMAC), Universidad Autónoma de Madrid（马德里自治大学凝聚态物理中心 (IFIMAC)）；Instituto Nicolás Cabrera (INC), Universidad Autónoma de Madrid（马德里自治大学尼古拉斯·卡布雷拉研究所 (INC)）
The energetic properties of electron transport in mesoscopic and nanoscale conductors is of large current interest. Here we theoretically investigate the possibility of probing fluctuations of charge and heat currents as well as their mixed correlations via fluctuations of the temperature and electrochemical potential of a probe coupled to the conductor. Our particular interest is devoted to the charge and energy noise stemming from time-dependently driven nanoelectronic systems designed for the controlled emission of single electrons, even though our setup is appropriate for more general AC d…
In the effort to make 2D materials-based devices smaller, faster, and more efficient, it is important to control charge carrier at lengths approaching the nanometer scale. Traditional gating techniques based on capacitive coupling through a gate dielectric cannot generate strong and uniform electric fields at this scale due to divergence of the fields in dielectrics. This field divergence limits the gating strength, boundary sharpness, and pitch size of periodic structures, and restricts possible geometries of local gates (due to wire packaging), precluding certain device concepts, such as pla…
