Thermodynamic and quantum bounds on nonlinear DC thermoelectric transport

I consider the non-equilibrium DC transport of electrons through a quantum system with a thermoelectric response. This system may be any nanostructure or molecule modeled by the nonlinear scattering theory which includes Hartree-like electrostatic interactions exactly, and certain dynamic interaction effects (decoherence and relaxation) phenomenologically. This theory is believed to be a reasonable model when single-electron charging effects are negligible. I derive three fundamental bounds for such quantum systems coupled to multiple macroscopic reservoirs, one of which may be superconducting. These bounds affect nonlinear heating (such as Joule heating), work and entropy production. Two bounds correspond to the first law and second law of thermodynamics in classical physics. The third bound is quantum (wavelength dependent), and is as important as the thermodynamic ones in limiting the capabilities of mesoscopic heat-engines and refrigerators. The quantum bound also leads to Nernst's unattainability principle that the quantum system cannot cool a reservoir to absolute zero in a finite time, although it can get exponentially close.Comment: 8pages (2figs) version2 (PRB version) minor improvements of earlier versio

Nonlinear thermoelectricity in point-contacts at pinch-off: a catastrophe aids cooling

We consider refrigeration and heat engine circuits based on the nonlinear thermoelectric response of point-contacts at pinch-off, allowing for electrostatic interaction effects. We show that a refrigerator can cool to much lower temperatures than predicted by the thermoelectric figure-of-merit ZT (which is based on linear-response arguments). The lowest achievable temperature has a discontinuity, called a fold catastrophe in mathematics, at a critical driving current I=I_c. For I >I_c one can in principle cool to absolute zero, when for I<I_c the lowest temperature is about half the ambient temperature. Heat back-flow due to phonons and photons stop cooling at a temperature above absolute zero, and above a certain threshold turns the discontinuity into a sharp cusp. We also give a heuristic condition for when an arbitrary system's nonlinear response means that its ZT ceases to indicate (even qualitatively) the lowest temperature to which the system can refrigerate.Comment: 7 pages 7 figs (changes in this version : Suppl. material expanded & integrated into text, more references

Quantum coherent three-terminal thermoelectrics: maximum efficiency at given power output

We consider the nonlinear scattering theory for three-terminal thermoelectric devices, used for power generation or refrigeration. Such systems are quantum phase-coherent versions of a thermocouple, and the theory applies to systems in which interactions can be treated at a mean-field level. We consider an arbitrary three-terminal system in any external magnetic field, including systems with broken time-reversal symmetry, such as chiral thermoelectrics, as well as systems in which the magnetic field plays no role. We show that the upper bound on efficiency at given power output is of quantum origin and is stricter than Carnot's bound. The bound is exactly the same as previously found for two-terminal devices, and can be achieved by three-terminal systems with or without broken time-reversal symmetry, i.e. chiral and non-chiral thermoelectrics.Comment: 22 pages (final version

Finding the quantum thermoelectric with maximal efficiency and minimal entropy production at given power output

We investigate the nonlinear scattering theory for quantum systems with strong Seebeck and Peltier effects, and consider their use as heat-engines and refrigerators with finite power outputs. This article gives detailed derivations of the results summarized in Phys. Rev. Lett. 112, 130601 (2014). It shows how to use the scattering theory to find (i) the quantum thermoelectric with maximum possible power output, and (ii) the quantum thermoelectric with maximum efficiency at given power output. The latter corresponds to a minimal entropy production at that power output. These quantities are of quantum origin since they depend on system size over electronic wavelength, and so have no analogue in classical thermodynamics. The maximal efficiency coincides with Carnot efficiency at zero power output, but decreases with increasing power output. This gives a fundamental lower bound on entropy production, which means that reversibility (in the thermodynamic sense) is impossible for finite power output. The suppression of efficiency by (nonlinear) phonon and photon effects is addressed in detail; when these effects are strong, maximum efficiency coincides with maximum power. Finally, we show in particular limits (typically without magnetic fields) that relaxation within the quantum system does not allow the system to exceed the bounds derived for relaxation-free systems, however, a general proof of this remains elusive.Comment: 20 pages 13 figures. Final version (typos fixed

Semiclassical transport in nearly symmetric quantum dots II: symmetry-breaking due to asymmetric leads

In this work - the second of a pair of articles - we consider transport through spatially symmetric quantum dots with leads whose widths or positions do not obey the spatial symmetry. We use the semiclassical theory of transport to find the symmetry-induced contributions to weak localization corrections and universal conductance fluctuations for dots with left-right, up-down, inversion and four-fold symmetries. We show that all these contributions are suppressed by asymmetric leads, however they remain finite whenever leads intersect with their images under the symmetry operation. For an up-down symmetric dot, this means that the contributions can be finite even if one of the leads is completely asymmetric. We find that the suppression of the contributions to universal conductance fluctuations is the square of the suppression of contributions to weak localization. Finally, we develop a random-matrix theory model which enables us to numerically confirm these results.Comment: (18pages - 9figures) This is the second of a pair of articles (v3 typos corrected - including in equations

Suppression of Shot-Noise in Quantum Cavities: Chaos vs. Disorder

We investigate the behavior of the shot-noise power through quantum mechanical cavities in the semiclassical limit of small electronic wavelength. In the absence of impurity scattering, the Fano factor $F$, giving the noise to current ratio, was previously found to disappear as more and more classical, hence deterministic and noiseless transmission channels open up. We investigate the behavior of $F$ as diffractive impurities are added inside the cavity. We find that $F$ recovers its universal value provided (i) impurities cover the full cavity so that only a set of zero measure of classical trajectories may avoid them, and (ii) the impurity scattering rate exceeds the inverse dwell time through the cavity. If condition (i) is not satisfied, $F$ saturates below its universal value, even in the limit of strong scattering. Our results corroborate the validity of the two-phase fluid model according to which the electronic flow splits into two well separated components, a classical deterministic fluid and a stochastic quantum-mechanical fluid. Only the latter carries shot-noise.Comment: 6 pages, 3 figures, to appear in the proceedings of the fourth conference on ``Unsolved Problems of Noise and Fluctuations in Physics, Biology and High Technology'

Thermoelectric coefficients and the figure of merit for large open quantum dots

We consider the thermoelectric response of chaotic or disordered quantum dots in the limit of phase-coherent transport, statistically described by random matrix theory. We calculate the full distribution of the thermoelectric coefficients (Seebeck $S$ and Peltier $\Pi$), and the thermoelectric figure of merit $ZT$, for large open dots at arbitrary temperature and external magnetic field, when the number of modes in the left and right leads ($N_{\rm L}$ and $N_{\rm R}$) are large. Our results show that the thermoelectric coefficients and $ZT$ are maximal when the temperature is half the Thouless energy, and the magnetic field is negligible. They remain small, even at their maximum, but they exhibit a type of universality at all temperatures, in which they do not depend on the asymmetry between the left and right leads $(N_{\rm L}-N_{\rm R})$, even though they depend on $(N_{\rm L}+N_{\rm R})$.Comment: 25 pages [final version - minor typos fixed

Suppression of weak-localization (and enhancement of noise) by tunnelling in semiclassical chaotic transport

We add simple tunnelling effects and ray-splitting into the recent trajectory-based semiclassical theory of quantum chaotic transport. We use this to derive the weak-localization correction to conductance and the shot-noise for a quantum chaotic cavity (billiard) coupled to $n$ leads via tunnel-barriers. We derive results for arbitrary tunnelling rates and arbitrary (positive) Ehrenfest time, $\tau_{\rm E}$. For all Ehrenfest times, we show that the shot-noise is enhanced by the tunnelling, while the weak-localization is suppressed. In the opaque barrier limit (small tunnelling rates with large lead widths, such that Drude conductance remains finite), the weak-localization goes to zero linearly with the tunnelling rate, while the Fano factor of the shot-noise remains finite but becomes independent of the Ehrenfest time. The crossover from RMT behaviour ($\tau_{\rm E}=0$) to classical behaviour ($\tau_{\rm E}=\infty$) goes exponentially with the ratio of the Ehrenfest time to the paired-paths survival time. The paired-paths survival time varies between the dwell time (in the transparent barrier limit) and half the dwell time (in the opaque barrier limit). Finally our method enables us to see the physical origin of the suppression of weak-localization; it is due to the fact that tunnel-barriers ``smear'' the coherent-backscattering peak over reflection and transmission modes.Comment: 20 pages (version3: fixed error in sect. VC - results unchanged) - Contents: Tunnelling in semiclassics (3pages), Weak-localization (5pages), Shot-noise (5pages