We study quantum transport through two-terminal nanoscale devices in contact with two particle reservoirs at different temperatures and chemical potentials. We discuss the general expressions controlling the electric charge current, heat currents and the efficiency of energy transmutation in steady conditions in the linear regime.
With focus in the parameter domain where the electron system acts as a power-generator, we elaborate workable expressions for optimal efficiency and thermoelectric pameters of nanoscale devices. The general concepts are set at work in the paradigmatic cases of Lorentzian resonances and antiresonances, and the encompassing Fano transmission function: the treatments are fully analytic, in terms of the trigamma functions and Bernoulli numbers. From the general curves here reported describing transport through the above model transmission functions, useful guidelines for optimal efficiency and thermopower can be inferred for engineering nanoscale devices in energy regions where they show similar transmission functions.
We show that the thermoelectric properties of nanoscale junctions featuring states near the Fermi level strongly depend on the type of resonance generated by such states, which can be either Fano or Breit-Wigner-like. We give general expressions for the thermoelectric coefficients generated by the two types of resonances and calculate the thermoelectric properties of these systems, which encompass most nanoelectronics junctions. We include simulations of real junctions where metalloporphyrin molecules bridge gold electrodes and prove that for some metallic elements the thermoelectric propertie…
We present thermoelectric measurements of the heat dissipated due to ferromagnetic resonance of a Permalloy strip. A microwave magnetic field, produced by an on-chip coplanar strip waveguide, is used to drive the magnetization precession. The generated heat is detected via Seebeck measurements on a thermocouple connected to the ferromagnet. The observed resonance peak shape is in agreement with the Landau-Lifshitz-Gilbert equation and is compared with thermoelectric finite element modeling. Unlike other methods, this technique is not restricted to electrically conductive media and is therefore…
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…
We theoretically study how one can control and enhance nonlinear thermoelectricity by regulating quantum coherence in nanostructures such as a quantum dot system or a single-molecule junction. In nanostructures, the typical temperature scale is much smaller than the resonance width, which largely suppresses thermoelectric effects. Yet we demonstrate one can achieve a reasonably good thermoelectric performance by regulating quantum coherence. Engaging a quantum-dot interferometer (a quantum dot embedded in the ring geometry) as a heat engine, we explore the idea of thermoelectric enhancement in…
We analyze an electronic nanoscale thermal machine driven by time-dependent environment: besides bias and gate voltage variations, we consider also the less prevailing time modulation of the couplings between leads and dot. We provide energy and heat current expressions in such situations, as well as expressions for the power exchanged between the dot+leads system and its outside. Calculations are made in the Keldysh nonequilibrium Green's function framework. We apply these results to design a cyclic refrigerator, circumventing the ambiguity of defining energy flows between subsystems in the c…
Based on the Landauer-Büttiker theory, we explore the thermal regimes of two-terminal nanoscale systems with an energy-peaked transmission function. The device is in contact with two reservoirs held at different temperatures and chemical potentials. We identify the operation regions where the system acts as energy pump (thermal machine) or heat pump (refrigerator machine), or where it is working in dissipative modes. The corresponding thermoelectric parameters are obtained without numerical calculations. The recent literature, by focusing on systems with box-like or step-like shapes of the tra…
In this work, we aim to design a heterostructure based nanoscale thermoelectric generator that can maximize the waste-heat conversion efficiency at a given output power. The primary objective to be achieved for this is to realize a boxcar-shaped (bandpass) electronic transmission function (R. S. Whitney, Phys. Rev. Lett. 112, 130601 (2014)). In order to achieve that, we propose the use of an electronic analog of optical Fabry-Pérot cavity over a central resonant tunneling structure. We further explore the optimum design possibilities by varying the geometry of the cavity wall to ensure a nearl…
The addition of porosity to thermoelectric materials can significantly increase the figure of merit, ZT, by reducing the thermal conductivity. Unfortunately, porosity is also detrimental to the thermoelectric power factor in the numerator of the figure of merit ZT. In this manuscript we derive strategies to recoup electrical performance in nanoporous Si by fine tuning the carrier concentration and through judicious design of the pore size and shape so as to provide energy selective electron filtering. In this study, we considered phosphorus doped silicon containing discrete pores that are eith…
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 …
Focus of the chapter is on the theoretical approaches aimed to analyze thermoelectric properties at the nanoscale. We discuss several relevant theoretical approaches for different set-ups of nano-devices providing estimations of the thermoelectric parameters in the linear and non-linear regime, in particular the thermoelectric figure of merit and the power-efficiency trade-off. Moreover, we analyze the role of not only electronic, but also of vibrational degrees of freedom. First, nanoscale thermoelectric phenomena are considered in the quantum coherent regime using the Landauer-Büttiker metho…
Despite its intrinsic non-equilibrium origin, thermoelectricity in nanoscale systems is usually described within a static scattering approach which disregards the dynamical interaction with the thermal baths that maintain energy flow. Using the theory of open quantum systems we show instead that unexpected properties, such as a resonant structure and large sign sensitivity, emerge if the non-equilibrium nature of this problem is considered. Our approach also allows us to define and study a local temperature, which shows hot spots and oscillations along the system according to the coupling of t…
We propose here a feasible and effective design of new thermoelectric systems based on physical gaps in nanoscale junctions. We show that, depending on the type of features, i.e. the character of surface/edge states, on both sides of the gap, it is possible to achieve rather high figures of merit. In particular, we show that for configurations that have localized states at the surfaces/edges, which translate into sharp resonances in the transmission, it is possible to achieve large Seebeck coefficients and figures of merit by carefully tuning their energy and their coupling to other states. We…
This mini-review is intended as a short introduction to electron flow in nanostructures. Its aim is to provide a brief overview of this topic for people who are interested in the thermodynamics of quantum systems but know little about nanostructures. We particularly emphasize devices that work in the steady-state, such as simple thermoelectrics, but also mention cyclically driven heat engines. We do not aim to be either complete or rigorous, but use a few pages to outline some of the main ideas in the topic.
We propose a possible route to achieve high thermoelectric efficiency in molecular junctions by combining a local chemical tuning of the molecular electronic states with the use of semiconducting electrodes. The former allows to control the position of the HOMO transmission resonance with respect to the Fermi energy while the latter fulfills a twofold purpose: the suppression of electron-like contributions to the thermopower and the cut-off of the HOMO transmission tails into the semiconductor band gap. As a result a large thermopower can be obtained. Our results strongly suggest that large fi…
We have experimentally studied the role of thermoelectric effects in nanoscale nonlocal spin valve devices. A finite element thermoelectric model is developed to calculate the generated Seebeck voltages due to Peltier and Joule heating in the devices. By measuring the first, second and third harmonic voltage response non locally, the model is experimentally examined. The results indicate that the combination of Peltier and Seebeck effects contributes significantly to the nonlocal baseline resistance. Moreover, we found that the second and third harmonic response signals can be attributed to Jo…
The quest to identify the best heat engine has been at the center of science and technology. Thermoelectric nanoscale heat engines convert heat flows into useful work in the form of electrical power and promise the realization of on-chip power production. Considerable studies have so far revealed the potentials to yield an enhanced efficiency originating from quantum confinement effects and energy-dependent transport properties. However, the full benefit of many-body interactions in thermoelectric is yet to be investigated; identifying the optimal interaction is a hard problem due to combinato…
We investigate the transport through a nanoscale device consisting of a degenerate double-orbital Anderson dot coupled to two uncorrelated leads. We determine the thermoelectric transport properties close to the one-electron regime and compare them to a corresponding single-orbital dot. The linear and nonlinear regimes are addressed, the latter via a non-equilibrium generalization of the non-crossing approximation based on the Keldysh formalism. Power output and efficiency in the Kondo regime are shown to be strongly enhanced through the presence of a second orbital. We predict an experimental…
Research on thermoelectrical energy conversion, the reuse of waste heat produced by some mechanical or chemical processes to generate electricity, has recently gained some momentum. The calculation of the electronic parameters entering the figure of merit of this energy conversion, and therefore the discovery of efficient materials, is usually performed starting from the Landauer's approach to quantum transport coupled with the Onsager's linear response theory. As it is well known, that approach suffers of certain serious drawbacks. Here, we discuss alternative dynamical methods that can go be…
Nanoscale structuring holds promise to improve thermoelectric properties of materials for energy conversion and photodetection. We report a study of the spatial distribution of the photothermoelectric voltage in thin-film nanowire devices fabricated from single metal. A focused laser beam is used to locally heat the metal nanostructure via a combination of direct absorption and excitation of a plasmon resonance in Au devices. As seen previously, in nanowires shorter than the spot size of the laser, we observe a thermoelectric voltage distribution that is consistent with the local Seebeck coeff…
A nanostructured thermoelectric device is designed by connecting a double-barrier resonant tunneling heterostructure to two electron reservoirs. Based on Landauers equation and Fermi-Dirac statistics, the exact solution of the heat flow is calculated. The maximum power output and efficiency are calculated through the optimizations of several key parameters. The optimum characteristic curve of the performance is obtained. The reasonably working region of the device is determined, the selection criteria of main parameters are provided, and the optimum configuration of the device is drawn. Result…
Thermoelectric material provides a high hope for converting harmful and useless heat into useful energy, electricity. It can also be used as solid state Peltier coolers in integrated circuits, an outstanding challenge for electronic engineers. The desire for a high efficient thermoelectric material has never been so keen. Although many works have been done, we are still far from having a recipe for thermoelectric materials. Nano-structuring provides an effective way to increase figure of merit (ZT) by reducing the thermal conductivity without affecting electronic property.1 Here, we propose a …
Realistic thermoelectric modeling and simulation tools are needed to explain the experiments and for device design. In this paper, we present a simple computational technique to make use of rigorous band structure calculations in thermoelectric device design. Our, methodology, based on Landauer theory, provides a way to benchmark effective mass level models against rigorous band structures. It can also be used for determining the temperature-dependent Fermi-level from a given doping density and numerically generated density-of-states, which can then be used with the numerically generated distr…
Local variations in the Seebeck coefficient in low-dimensional materials-based nanostructures and devices play a major role in their thermoelectric performance. Unfortunately, currently most thermoelectric measurements probe the aggregate characteristics of the device as a whole, failing to observe the effects of the local variations and internal structure. Such variations can be caused by local defects, geometry, electrical contacts or interfaces and often substantially influence thermoelectric properties, most profoundly in two-dimensional (2D) materials. Here, we use Scanning Thermal Gate M…
The reduction of the thermal conductivity in nanostructures opens up the possibility of exploiting for thermoelectric purposes also materials such as silicon, which are cheap, available and sustainable but with a high thermal conductivity in their bulk form. The development of thermoelectric devices based on these innovative materials requires reliable techniques for the measurement of thermal conductivity on a nanometric scale. The approximations introduced by conventional techniques for thermal conductivity measurements can lead to unreliable results when applied to nanostructures, because h…
Using first-principles approaches, we have investigated the thermoelectric properties and the energy conversion efficiency of the paired metal-Br-Al junction. Owing to the narrow states in the vicinity of the chemical potential, the nanojunction has large Seebeck coefficients such that it can be considered an efficient thermoelectric power generator. We also consider the nanojunction in a three-terminal geometry, where the current, voltage, power, and efficiency can be efficiently modulated by the gate voltages. Such current-voltage characteristics could be useful in the design of nano-scale e…
The quest for good thermoelectric materials and/or high-efficiency thermoelectric devices is of primary importance from theoretical and practical points of view. Low-dimensional structures with quantum dots or molecules are promising candidates to achieve the goal. Interactions between electrons, far-from-equilibrium conditions and strongly non-linear transport are important factors affecting the usefulness of the devices. This paper analyses the thermoelectric power of a two-terminal quantum dot under large thermal $ΔT$ and voltage $V$ biases as well as the performance of the three-terminal s…
A three-terminal thermoelectric device based on a $p$-$i$-$n$ semiconductor junction is proposed, where the intrinsic region is mounted onto a, typically bosonic, thermal terminal. Remarkably, the figure of merit of the device is governed also by the energy distribution of the {\em bosons} participating in the transport processes, in addition to the electronic one. An enhanced figure of merit can be obtained when the relevant distribution is narrow and the electron-boson coupling is strong (such as for optical phonons). We study the conditions for which the figure of merit of the three-termina…
The power factor of a thermoelectric device is a measure of the heat-to-energy conversion efficiency in nanoscopic devices. Yet, even as interest in low-dimensional thermoelectric materials has increased, experimental research on what influences the power factor in these systems is scarce. Here, we present a detailed thermoelectric study of graphene quantum dot devices. We show that spin-degeneracy of the quantum dot states has a significant impact on the zero-bias conductance of the device and leads to an increase of the power factor. Conversely, we demonstrate that non-ideal heat exchange wi…
The resonant tunneling model is the simplest model for describing electronic transport through nanoscale objects like individual molecules. A complete understanding includes not only charge transport but also thermal transport and their intricate interplay. Key linear response observables are the electrical conductance G and the Seebeck coefficient S. Here we present experiments on unspecified resonant tunnel junctions and molecular junctions that uncover correlations between $G$ and $S$, in particular rigid boundaries for $S(G)$. We find that these correlations can be consistently understood …
Miniaturization of electronic devices aims at manufacturing ever smaller products, from mesoscopic to nanoscopic sizes. This trend is challenging because the increased levels of dissipated power demands a better understanding of heat transport in small volumes. A significant amount of the consumed energy is transformed into heat and dissipated to the environment. Thermoelectric materials offer the possibility to harness dissipated energy and make devices less energy-demanding. Heat-to-electricity conversion requires materials with a strongly suppressed thermal conductivity but still high elect…
We study thermoelectric devices where a single 18-annulene molecule is connected to metallic zigzag graphene nanoribbons (ZGNR) via highly transparent contacts that allow for injection of evanescent wave functions from ZGNRs into the molecular ring. Their overlap generates a peak in the electronic transmission, while ZGNRs additionally suppress hole-like contributions to the thermopower. Thus optimized thermopower, together with suppression of phonon transport through ZGNR-molecule-ZGNR structure, yield the thermoelectric figure of merit ZT ~ 0.5 at room temperature and 0.5 < ZT < 2.5 below li…
Thermodynamic currents can fluctuate significantly at the nanoscale. But some currents fluctuate less than others. Hyperaccurate currents are those which fluctuate the least, in the sense that they maximize the signal-to-noise ratio (precision). In this letter we analytically determine the hyperaccurate current in the case of a quantum thermoelectric, modeled by the Landauer-Büttiker formalism.
Fast and controllable cooling at nanoscales requires a combination of highly efficient passive cooling and active cooling. While passive cooling in graphene-based devices is quite effective due to graphene's extraordinary heat-conduction, active cooling has not been considered feasible due to graphene's low thermoelectric power factor. Here we show that the thermoelectric performance of graphene can be significantly improved by using hBN substrates instead of SiO2. We find the room temperature efficiency of active cooling, as gauged by the power factor times temperature, reaches values as high…
We have studied thermoelectric effect of a Kane-Mele normal-insulator-superconductor (KMNIS) junction at ultra-low temperatures using a modified version of the well-known Blonder-Tinkham-Klapwijk (BTK) theory. Since both the (electronic) charge and thermal current due to the carriers are sensitive to the strengths of the spin-orbit coupling (SOC) present in the Kane-Mele model, a tunability of this junction device with regard to its thermoelectric properties can be experimentally achieved by certain techniques that are used to manipulate the values of the spin-orbit couplings. We have computed…
The performance of thermoelectric energy harvesters can be improved by nanostructures that exploit inelastic transport processes. One prototype is the three-terminal hopping thermoelectric device where electron hopping between quantum-dots are driven by hot phonons. Such three-terminal hopping thermoelectric devices have potential in achieving high efficiency or power via inelastic transport and without relying on heavy-elements or toxic compounds. We show in this work how output power of the device can be optimized via tuning the number and energy configuration of the quantum-dots embedded in…
We theoretically investigate the enhancement of thermoelectric cooling performance in thermoelectric devices made of materials with inhomogeneous thermal conductivity, beyond the usual practice of enhancing thermoelectric figure of merit ZT. The dissipation of Joule heat in such thermoelectric devices is asymmetric which can give rise to better thermoelectric cooling performance. Although the thermoelectric figure of merit and the coefficient-of-performance are only slightly enhanced, both the maximum cooling power and the maximum cooling temperature difference can be enhanced significantly. T…
We calculate the electronic and thermal transport properties of devices based on finite graphene antidot lattices (GALs) connected to perfect graphene leads. We use an atomistic approach based on the $π$-tight-binding model, the Brenner potential, and employing recursive Green's functions. We consider the effect of random disorder on the electronic and thermal transport properties, and examine the potential gain of thermoelectric merit by tailoring of the disorder. We propose several routes to optimize the transport properties of the GAL systems. Finally, we illustrate how quantum thermal tran…
Molecular junctions are a versatile test bed for investigating thermoelectricity on the nanoscale1-10 and contribute to the design of new cost-effective environmentally-friendly organic thermoelectric materials11. It has been suggested that transport resonances associated with the discrete molecular levels would play a key role in the thermoelectric performance12,13, but no direct experimental evidence has been reported. Here we study single-molecule junctions of the endohedral fullerene Sc3N@C80 connected to gold electrodes using a scanning tunnelling microscope (STM). We find that the magnit…
Molecular junctions and similar devices described by an energy dependent transmission coefficient can have a high linear response thermoelectric figure of merit. Since such devices are inherently non-linear, the full thermodynamic efficiency valid for any temperature and chemical potential difference across the leads is calculated. The general features in the energy dependence of the tranmission function that lead to high efficiency and also high power output are determined. It is shown that the device with the highest efficiency does not necessarily lead to large power output. To illustrate t…
Solid-state thermoelectric devices are currently used in applications ranging from thermocouple sensors to power generators in satellites, to portable air-conditioners and refrigerators. With the ever-rising demand throughout the world for energy consumption and CO2 reduction, thermoelectric energy conversion has been receiving intensified attention as a potential candidate for waste-heat harvesting as well as for power generation from renewable sources. Efficient thermoelectric energy conversion critically depends on the performance of thermoelectric materials and devices. In this review, we …
The possibility of electrically exciting and detecting magnon currents in magnetic insulators has opened exciting perspectives for transporting spin information in electronic devices. However, the role of the magnetic field and the nonlocal thermal gradients on the magnon transport remain unclear. Here, by performing nonlocal harmonic voltage measurements, we investigate magnon transport in perpendicularly magnetized ultrathin Tm3Fe5O12 (TmIG) films coupled to Pt electrodes. We show that the first harmonic nonlocal voltage captures spin-driven magnon transport in TmIG, as expected, and the sec…
The energy dependent thermoelectric response of a single molecule contains valuable information about its transmission function and its excited states. However, measuring it requires devices that can efficiently heat up one side of the molecule while being able to tune its electrochemical potential over a wide energy range. Furthermore, to increase junction stability devices need to operate at cryogenic temperatures. In this work we report on a new device architecture to study the thermoelectric properties and the conductance of single molecules simultaneously over a wide energy range. We empl…
Graphene is known to show a significant photo-thermoelectric effect that can exceed its photovoltaic contribution. Here, by utilizing this effect, we demonstrate a photovoltage measurement of cyclotron resonance in a double-back-gated h-BN/graphene/h-BN two-terminal device. A graphite local bottom gate was fabricated in addition to a p-doped Si global back gate. By tuning the two gate voltages, an in-plane graphene junction having an asymmetric carrier-doping profile was created. With the help of this asymmetric structure, the photo-thermoelectric voltage generated in the vicinity of the metal…
Recent developments in nanoscale experimental techniques made it possible to utilize single molecule junctions as devices for electronics and energy transfer with quantum coherence playing an important role in their thermoelectric characteristics. Theoretical studies on the efficiency of nanoscale devices usually employ rate (Pauli) equations, which do not account for quantum coherence. Therefore, the question whether quantum coherence could improve the efficiency of a molecular device cannot be fully addressed within such considerations. Here, we employ a nonequilibrium Green function approac…
Quantum dots are useful model systems for studying quantum thermoelectric behavior because of their highly energy-dependent electron transport properties, which are tunable by electrostatic gating. As a result of this strong energy dependence, the thermoelectric response of quantum dots is expected to be nonlinear with respect to an applied thermal bias. However, until now this effect has been challenging to observe because, first, it is experimentally difficult to apply a sufficiently large thermal bias at the nanoscale and, second, it is difficult to distinguish thermal bias effects from pur…
Spin-related effects in thermoelectricity can be used to design more efficient refrigerators and offer novel promising applications for the harvesting of thermal energy. The key challenge is to design structural and compositional magnetic material systems with sufficiently high efficiency and power output for transforming thermal energy into electric energy and vice versa. Here, the fabrication of large-area 3D interconnected Co/Cu nanowire networks is demonstrated, thereby enabling the controlled Peltier cooling of macroscopic electronic components with an external magnetic field. The flexibl…
The silicon (Si) based spin-MOSFET (metal-oxide semiconductor field-effect transistor) is considered to be the building block of low-power-consumption electronics, utilizing spin-degrees of freedom in semiconductor devices. In this paper, we review the latest results on the spin transport in nanoscale Si-based spin-valve devices, which is important to realize the nanoscale spin-MOSFET. Our results demonstrate the importance of ballistic transport in obtaining high spin-dependent output voltage in nanoscale Si spin-valve devices.
We consider a single level quantum dot interacting with a phonon mode and weakly coupled to metallic leads which are subjected to a time dependent gate voltage. Electrical conductance, thermopower, and figure of merit are investigated in detail using a Tien-Gordon-type rate equation. In the presence of the microwave field, the electrical conductance exhibits extra peaks whose height is controlled by the magnitude of the microwave field. Furthermore, the oscillation of the thermopower increases in the presence of the time-dependent gate voltage or the electron-phonon interaction. Influence of t…
The role of dimensionality on the electronic performance of thermoelectric devices is clarified using the Landauer formalism, which shows that the thermoelectric coefficients are related to the transmission, T(E), and how the conducing channels, M(E), are distributed in energy. The Landauer formalism applies from the ballistic to diffusive limits and provides a clear way to compare performance in different dimensions. It also provides a physical interpretation of the "transport distribution," a quantity that arises in the Boltzmann transport equation approach. Quantitative comparison of thermo…
We present a method, based on characterizing efficiency fluctuations, to asses the performance of nanoscale thermoelectric junctions. This method accounts for effects typically arising in small junctions, namely, stochasticity in the junction's performance, quantum effects, and nonequilibrium features preventing a linear response analysis. It is based on a nonequilibrium Green's function (NEGF) approach, which we use to derive the full counting statistics (FCS) for heat and work, and which in turn allows us to calculate the statistical properties of efficiency fluctuations. We simulate the lat…
Recent breakthroughs in quantum-dot circuit-quantum-electrodynamics (circuit-QED) systems are important both from a fundamental perspective and from the point of view of quantum photonic devices. However, understanding the applications of such setups as potential thermoelectric diodes and transistors has been missing. In this paper, via the Keldysh nonequilibrium Green's function approach, we show that cavity-coupled double quantum-dots can serve as excellent quantum thermoelectric diodes and transistors. Using an enhanced perturbation approach based on polaron-transformations, we find non-mon…
