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 bulk thermoelectric refrigerator with the same $ZT$ due to suppressed local heating via the quasi-ballistic electron transport and small driving voltages. Quantum nature due to the size minimization offered by atomic-level control of properties facilitates electron cooling beyond the expectation of the conventional thermoelectric device theory.
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 investigate the thermopower of a metal-molecule-metal junction taking into account thermal effects on the junction. Based on analytical expressions and numerical simulations we show that the thermoelectric potential reveals valuable information on the mechanisms controlling the electron transfer process, including coherent transmission and thermalized hopping. We also show that at high temperatures the position of the Fermi energy relative to the molecular states can be easily deduced from the thermoelectric potential. Standard current-voltage measurements are insensitive to this informatio…
In this work, we investigate thermoelectric properties of junctions consisting of two partially overlapped graphene sheets coupled to each other in the cross-plane direction. It is shown that because of the weak van-der Waals interactions between graphene layers, the phonon conductance in these junctions is strongly reduced, compared to that of single graphene layer structures, while their electrical performance is weakly affected. By exploiting this effect, we demonstrate that the thermoelectric figure of merit can reach values higher than 1 at room temperature in junctions made of gapped gra…
The thermoelectric properties of polythiophene (PT) coupled to the Au (111) electrodes are studied based on density functional theory combined with nonequilibrium Green function formalism. Specially, the effect of Li and Cl adsorbents on the thermoelectric efficiency of the PT junction is investigated in different concentrations of the dopants for two lengths of the PT. Results show that the presence of dopants can bring the structural changes in the oligomer and modify the arrangement of the molecular levels leading to the dramatic changes in the transmission spectra of the junction. Therefor…
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…
It was recently suggested that molecular junctions would be excellent elements for efficient and high-power thermoelectric energy conversion devices. However, experimental measurements of thermoelectric conversion in molecular junctions have indicated rather poor efficiency, raising the question of whether it is indeed possible to design a setup for molecular junctions that will exhibit enhanced thermoelectric performance. Here we suggest that hybrid single-molecule nanoparticle junctions can serve as efficient thermoelectric converters. The introduction of a semiconducting nanoparticle introd…
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 Lorent…
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 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 …
It is known that Josephson junction (JJ) hosting scattering centers with energy-dependent scattering amplitudes which breaks the $ω\rightarrow-ω$ symmetry (where $ω$ is the excitation energy of electron about the Fermi level) exhibits finite thermoelectric response. In contrast, here we show that even in a ballistic JJ this symmetry is broken and it leads to a non-zero thermoelectric response when the junction length is of the order of coherence length of the superconductor and the corresponding thermoelectric coefficient confirms to the universal sinusoidal dependence on $ϕ_{12}$, where $ϕ_{1…
The miniaturization of thermoelectric nanojunctions raises a fundamental question: do the thermoelectric quantities of the bridging materials in nanojunctions remain to display material properties or show junction properties? In order to answer this question, we investigate the Seebeck coefficient $S$ and the thermoelectric figure of merit $ZT$ especially in relation to the length characteristics of the junctions from the first-principles approaches. For $S$, the metallic atomic chains reveal strong length characteristics related to strong hybridization in the electronic structures between the…
Thermoelectric transport across normal-metal/helical-multiferroic/ferromagnetic heterojunctions is theoretically investigated. We find a anisotropic charge and spin thermopower with a $C_{2v}$ symmetry. The angular dependence on the magnetization orientation of the ferromagnetic layer is substantiated by a phenomenological theory based on the symmetry of the effective spin-orbit interaction induced by the topology of the spiral magnetic order in the multiferroic barrier.
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…
Noble metals break preferably exposing (111)-oriented surfaces, that host Shockley type surface states (SSs). Nevertheless, the relevance of SSs on the electrical properties of gold-based molecular junctions has not been explored in detail yet. Here, we present ab initio simulations that show how the gold (111) SS, that lies approximately 0.5 eV below the Fermi energy, is key to determining correctly the electrical and thermoelectric response of the above junctions. We show how the ability to shift in a controlled way the energy position of gold SS enables us to tune the electrical and thermoe…
We present a detailed study of the non-linear thermoelectric properties of a molecular junction, represented by a dissipative Anderson-Holstein model. A single orbital level with strong Coulomb interaction is coupled to a localized vibrational mode and we account for both electron and phonon exchange with both electrodes, investigating how these contribute to the heat and charge transport. We calculate the efficiency and power output of the device operated as a heat to electric power converter and identify the optimal operating conditions, which are found to be qualitatively changed by the pre…
We investigate the optoelectronic response of a graphene interface junction, formed with bilayer and single-layer graphene, by photocurrent (PC) microscopy. We measure the polarity and amplitude of the PC while varying the Fermi level by tuning a gate voltage. These measurements show that the generation of PC is by a photo-thermoelectric effect. The PC displays a factor of ~10 increase at the cryogenic temperature as compared to room temperature. Assuming the thermoelectric power has a linear dependence on the temperature, the inferred graphene thermal conductivity from temperature dependent m…
We explore the thermoelectric properties of gold atomic chains bridging gold electrodes by means of \textit{ab initio} and semi-empirical calculations, and heuristic reasoning. We predict the thermoelectric voltage induced by a temperature difference across such junctions to oscillate, repeatedly changing sign, as a function of the number of atoms $N$ making up the atomic chain. We also predict the amplitude of the oscillations to be proportional to $N$ for long atomic chains. Further we predict the thermoelectric voltage to change sign, in some cases, if the junction is stretched without chan…
In the present work, we theoretically analyze the steady-state thermoelectric transport through a single-molecule junction with a vibrating bridge. Thermally induced charge current in the system is explored using a nonequilibrium Green's functions formalism. We study combined effects of Coulomb interactions between charge carriers on the bridge and electron-phonon interactions on the thermocurrent beyond the linear response regime. It is shown that electron-vibron interactions may significantly affect both magnitude and direction of the thermocurrent, and vibrational signatures may appear.
We consider a Josephson junction hosting a Kramers pair of helical edge states of a quantum spin Hall bar in contact with a normal-metal probe. In this hybrid system, the orbital phase induced by a small magnetic field threading the junction known as Doppler shift (DS), combines with the conventional Josephson phase difference and originates an effect akin to a Zeeman field in the spectrum. As a consequence, when a temperature bias is applied to the superconducting terminals, a thermoelectric current is established in the normal probe. We argue that this purely non-local thermoelectric effect …
We examine splitting the heat flow in a low-dimensional junction under influence an external d.c. magnetic field. The junction is a crossing between the narrow single atomic layer stripe (or a nanotube) of a semiconductor C with a metal stripe N (C/N-knot). External source of heat injects the non-equilibrium (NE) phonons, electrons, and holes into C which then propagate in direction the C/N-knot. Most of the heat is carried by NE phonons which drag additional electron and hole excitations along C. In vicinity the C/N-knot, the Lorentz force pulls the charge carriers from C to N thus inducing a…
We report results of theoretical studies of thermoelectric efficiency of single-molecule junctions with long molecular linkers. The linker is simulated by a chain of identical sites described using a tight-binding model. It is shown that thermoelectric figure of merit ZT strongly depends on the bridge length, being controlled by the lineshape of electron transmission function within the tunnel energy range corresponding to HOMO/LUMO transport channel. Using the adopted model we demonstrate that ZT may significantly increase as the linker lengthens, and that gateway states on the bridge (if any…
Motivated by recent experiments, we present here an ab initio study of the impact of the phonon transport on the thermal conductance and thermoelectric figure of merit of C$_{60}$-based single-molecule junctions. To be precise, we combine density functional theory with nonequilibrium Green's function techniques to compute these two quantities in junctions with either a C$_{60}$ monomer or a C$_{60}$ dimer connected to gold electrodes, taking into account the contributions of both electrons and phonons. Our results show that for C$_{60}$ monomer junctions phonon transport plays a minor role in …
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…
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…
We investigate the electron transport and thermoelectric property of twisted bilayer graphene nanoribbon junction (TBGNRJ) in $0^o$, $21.8^o$, $38.2^o$ and $60^o$ rotation angles by first principles calculation with Landauer-Buttiker and Boltzmann theories. It is found that TBGNRJs exhibit negative differential resistance (NDR) in $21.8^o$ and $38.2^o$ rotation angles under $\pm$ 0.2 V bias voltage. More importantly, three peak ZT values of 2.0, 2.7 and 6.1 can be achieved in the $21.8^o$ rotation angle at 300K. The outstanding ZT values of TBGNRJs are interpreted as the combination of the red…
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…
We show that a molecular junction can give large values of the thermoelectric figure of merit $ZT$, and so could be used as a solid state energy conversion device that operates close to the Carnot efficiency. The mechanism is similar to the Mahan-Sofo model for bulk thermoelectrics -- the Lorenz number goes to zero violating the Wiedemann-Franz law while the thermopower remains non-zero. The molecular state through which charge is transported must be weakly coupled to the leads, and the energy level of the state must be of order $k_B T$ away from the Fermi energy of the leads. In practice, the…
The thermoelectric transport through a molecular bridge is discussed, with an emphasis on the effects of inelastic processes of the transport electrons caused by the coupling to the vibrational modes of the molecule. In particular it is found that when the molecule is strongly coupled to a thermal bath of its own, which may be at a temperature different from those of the electronic reservoirs, a heat current between the molecule and the electrons can be converted into electric current. Expressions for the transport coefficients governing this conversion and similar ones are derived, and a poss…
The energy dissipation and heat flows associated with the particle current in a system with a molecular junction are considered. In this connection, we determine the effective temperature of the molecular oscillator that is compatible with the existence of a steady state. The calculations based on the Kadanov-Baym nonequilibrium Green function formalism are carried out supposing a strong coupling of the dot electrons with the molecular vibrations. Accordingly, the representation given by the Lang-Firsov polaron transformation is used and the dependence of results on the electron-phonon interac…
Molecular junctions comprise small molecules on the order of one or a few nanometers in length, chemically attached to two electrodes of metal or semiconductors. They have recently been identified as promising candidates for materials/devices for thermoelectric energy conversion. Molecules have the potential to act as sharp energy filters for electrical currents and could outperform other materials considered for thermoelectric energy conversion so far, thereby providing a wide-spread technological relevance thermoelectrics could not achieve to date. However, there is a clear gap between predi…
We study the use of a thermoelectric junction as a thermal radiation detector in the calorimetric regime, where single radiation bursts can be separated in time domain. We focus especially on the case of a large thermoelectric figure of merit $ZT$ affecting significantly for example the relevant thermal time scales. This work is motivated by the use of hybrid superconductor/ferromagnet systems in creating an unprecedentedly high low-temperature $ZT$ even exceeding unity. Besides constructing a very general noise model which takes into account cross correlations between charge and heat noise, w…
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…
We investigate the electrical and thermal transport properties of the $α-T_3$ based normal metal-insulator-superconductor (NIS) junction using Blonder-Tinkham-Klapwijk (BTK) theory. We show that the tunneling conductance of the NIS junction is an oscillatory function of the effective barrier potential ($χ$) of the insulating region upto a thin barrier limit. The periodicity and the amplitudes of the oscillations largely depend on the values of $α$ and the gate voltage of the superconducting region, namely, $U_0$. Further, the periodicity of the oscillation changes from $π$ to $π/2$ as we incre…
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…
Here we present a theoretical study of the thermoelectric transport through {[}2,2{]}para\-cyclo\-phane-based single-molecule junctions. Combining electronic and vibrational structures, obtained from density functional theory (DFT), with nonequilibrium Green's function techniques, allows us to treat both electronic and phononic transport properties at a first-principles level. For the electronic part, we include an approximate self-energy correction, based on the DFT+$Σ$ approach. This enables us to make a reliable prediction of all linear response transport coefficients entering the thermoele…
Interference represents one of the most striking manifestation of quantum physics in low-dimensional systems. Despite evidences of quantum interference in charge transport have been known for a long time, only recently signatures of interference induced thermal properties have been reported, paving the way for the phase-coherent manipulation of heat in mesoscopic devices. In this work we show that anomalous thermoelectric properties and efficient heat rectification can be achieved by exploiting the phase-coherent edge states of quantum Hall systems. By considering a tunneling geometry with mul…
For future on-chip communication schemes, it is essential to integrate nanoscale materials with an ultrafast optoelectronic functionality into high-frequency circuits. The atomically thin graphene has been widely demonstrated to be suitable for photovoltaic and optoelectronic devices because of its broadband optical absorption and its high electron mobility. Moreover, the ultrafast relaxation of photogenerated charge carriers has been verified in graphene. Here, we show that dual-gated graphene junctions can be functional parts of THz-circuits. As the underlying optoelectronic process, we expl…
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 consider theoretically a wide graphene ribbon, that on both ends is attached to electronic reservoirs which generally have different temperatures. The graphene ribbon is assumed to be deposited on a substrate, that leads to a spin-orbit coupling of Rashba type. We calculate the thermally induced charge current in the ballistic transport regime as well as the thermoelectric voltage (Seebeck effect). Apart from this, we also consider thermally induced spin current and spin polarization of the graphene ribbon. The spin currents are shown to have generally two components; one parallel to the te…
We investigate the noise current in a thermally biased tunnel junction between two superconductors with different zero-temperature gaps. When the Josephson effect is suppressed, this structure can support a nonlinear thermoelectric effect due to the spontaneous breaking of electron-hole symmetry, as we recently theoretically predicted. We discuss the possibly relevant role played by the noise in the junction. While a moderate noise contribution assists the generation of the thermoelectric signal, further unveiling the spontaneous nature of the electron-hole symmetry breaking, a large noise con…
Electronic and Thermoelectric Properties of Molecular Junctions Incorporating Organometallic Complexes: Implications for Thermoelectric Energy Conversion
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…
We report on large thermoelectric effects in superconductor-ferromagnet tunnel junctions in proximity contact with the ferromagnetic insulator europium sulfide. The combination of a spin-splitting field and spin-polarized tunnel conductance in these systems breaks the electron-hole symmetry and leads to spin-dependent thermoelectric currents. We show that the exchange splitting induced by the europium sulfide boosts the thermoelectric effect in small applied fields and can therefore eliminate the need to apply large magnetic fields, which might otherwise impede applications in thermometry or c…
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.
Quantization of the magneto-thermoelectric transport is studied when an external d.c. magnetic field is applied to the C/N-knot formed as crossing between a narrow stripe of conducting atomic monolayer C on the one hand and metal stripe N on the other hand. The temperature gradient in C is created by injecting the non-equilibrium electrons, holes and phonons from the heater H thereby directing them toward the C/N-knot. A non-linear coupling between electron states of the C/N-knot counter electrodes causes splitting of the heat flow into several fractions owing to the Lorentz force acting in th…
We studied the thermoelectric coefficients (Seebeck and thermal conductance)of FeCo|MgO|FeCo(001) magnetic tunnel junctions (MTJs) from first principles using a generalized Landauer-Büttiker formalism. FeCo|MgO|FeCo(001) MTJs usually yield smaller thermoelectric effects compared with epitaxial Fe|MgO|Fe(001) MTJs. The (magneto-) Seebeck effect is sensitive to the details of the FeCo$|$MgO interfaces. Interfacial oxygen vacancies (OVs) can enhance the thermoelectric effects in MTJs greatly. We also compute angular dependent Seebeck coefficients that provide more information about the transport …
The electrical conductance, thermal conductance, thermal power and figure of merit (ZT) of semiconductor quantum dots (QDs) embedded into an insulator matrix connected with metallic electrodes are theoretically investigated in the Coulomb blockade regime. The multilevel Anderson model is used to simulate the multiple QDs junction system. The charge and heat currents in the sequential tunneling process are calculated by the Keldysh Green function technique. In the linear response regime the ZT values are still very impressive in the small tunneling rates case, although the effect of electron Co…
We report on the experimental observation of thermoelectric currents in superconductor-ferromagnet tunnel junctions in high magnetic fields. The thermoelectric signals are due to a spin-dependent lifting of particle-hole symmetry, and are found to be in excellent agreement with recent theoretical predictions. The maximum Seebeck coefficient inferred from the data is about $-100~\mathrm{μV/K}$, much larger than commonly found in metallic structures. Our results directly prove the coupling of spin and heat transport in high-field superconductors.
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…
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…
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…
