fundamental aspects of steady state heat to work...
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Fundamental Aspects of Steady State Heat to Work Conversion
Giuliano BenentiCenter for Nonlinear and Complex Systems,
Univ. Insubria, Como, ItalyINFN, Milano, Italy
In collaboration with: Giulio Casati, Vinitha Balachandran, Shunda Chen (Como),
Keiji Saito (Yokohama), Tomaz Prosen, Martin Horvat (Ljubljana),
Wang Jiao (Xiamen), Carlos Mejía-Monasterio (Madrid)
Riccardo Bosisio (Saclay-Pisa)Francesco Mazza, Stefano Valentini,
Rosario Fazio, Vittorio Giovannetti, Fabio Taddei (Pisa)
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OUTLINECoupled charge and heat flow: a dynamical system’s perspective on a fundamental problem of statistical physicsCan we learn something about microscopic mechanisms leading to high energy conversion (thermoelectric) efficiency from the study of nonlinear dynamical systems?
Part I: Interacting momentum-conserving systems Part II: Systems with time-reversal symmetry breaking: Asymmetric thermopower; Overcoming the Curzon-Ahlborn limit; Magnetic thermal switch Part III: Multi-terminal systems: heat-charge separation
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Volta and the discovery of thermoelectricity
1794-1795: letters from Volta to Vassali. “I immersed for some half-minute the end of such (iron) arc into boiling water and, without letting it to cool down, returned to experiments with two glasses of cold water. And it was then that the frog in water started contracting...”
(see Anatychuk et al, “On the discovery of thermoelectricity by A.Volta”)
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Abram Ioffe (1950s): Doped semiconductors have large thermoelectric effect
The initial excitement about semiconductors in the 1950s was due to their promise, not in electronics but in refrigeration. The goal was to build environmental benign solid state home refrigerators and power generators
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Thermoelectric (Peltier) refrigerators have poor efficiency compared to compressor-based refrigerators
Niche applications: space missions, medical applications, laboratory equipments, air conditioning in submarines (reliability and quiet operation more important than cost)
car’s seats cooler/heater Use vehicle waste heat to improve fuel economy
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Mildred Dresselhaus et al. (Adv. Materials, 2007): “a newly emerging field of low-dimensional thermoelectricity, enabled by material nanoscience and nanotechnology... Thermoelectric phenomena are expected to play an increasingly important role in meeting the energy challenge for the future...”
Small scale thermoelectricity could be relevant for cooling directly on chip, by purely electronic means. Nanoscale heat management is crucial to reduce the energy cost in many applications of microelectronics.
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Thermoelectric applications are limited due to the low conversion efficiency
Cronin Vining: limited role for thermoelectrics in the climate crisis (ZT too small to replace mechanical engines for large-scale applications)Arun Majumdar: at issue are some fundamental scientific challenges, which could be overcome by deeper understanding of charge and heat transport...
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Coupled 1D particle and heat transport
Stochastic baths: ideal gases at fixed temperature
and chemical potential
Onsager relation:
Positivity of entropy production:
X1 = ��µ
X2 = ��� = �T/T 2
� = 1/T
�µ = µL � µR
�� = �L � �R
�T = TL � TR
(we assume TL > TR, µL < µR)
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Onsager and transport coefficients
G =�
J�
�µ/e
�
�T=0
� G =e2
TL��
� =�
Jq
�T
�
J�=0
� � =1
T 2
detLL��
Note that the positivity of entropy production implies that the (isothermal) electric conductance G>0 and the thermal conductance Ξ>0
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Maximum efficiency
Find the maximum of η over X1, for fixed X2 (i.e., over the applied voltage ΔV for fixed temperature difference ΔT)
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Thermoelectric figure of merit
ZT =L2
q�
detL=
GS2
�T
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Efficiency at maximum power
Find the maximum of ω over X1, for fixed X2 (over the applied voltage ΔV for fixed ΔT)
Output power � = �TX1(L��X1 + L�qX2)
X1 = � L�q
2L��X2
Efficiency at maximum power
�(�max) =�C
2ZT
ZT + 2� �CA �
�C
2
ηCA Curzon-Ahlborn upper bound
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�max
�(�max)
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ZT diverges iff the Onsager matrix is ill-conditioned, that is, the condition number:
diverges
In such case the system is singular (strong-coupling limit):
(the ratio Jq/Jρ is independent of the applied voltage and temperature gradients)
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Charge current
Non-interacting systems, Landauer-Büttiker formalism
Heat current from reservoir α
Jq.� =1h
� �
��dE(E � µ�)�(E)[fL(E)� fR(E)]
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If transmission is possible only inside a tiny energy window around E=E✶ then
Thermoelectric efficiency
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Carnot efficiency
[Mahan and Sofo, PNAS 93, 7436 (1996); Humphrey et al., PRL 89, 116801 (2002)]
Energy filtering mechanism
Carnot efficiency obtained in the limit of reversible transport (zero entropy production) and zero output power
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Is energy-filtering necessary to get Carnot efficiency?
No, for interacting systems with momentum conservation
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Interacting systems, Green-Kubo formulaThe Green-Kubo formula expresses linear response transport coefficients in terms of dynamic correlation functions of the corresponding current operators, cal- culated at thermodynamic equilibrium
Non-zero generalized Drude weights signature of ballistic transport
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Conservation laws and thermoelectric efficiencySuzuki’s formula (which generalizes Mazur’s inequality) for finite-size Drude weights
Qn relevant (i.e., non-orthogonal to charge and thermal currents), mutually orthogonal conserved quantities
Assuming commutativity of the two limits,
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Momentum-conserving systems
Consider systems with a single relevant constant of motion, notably momentum conservation
Ballistic contribution to det(L) vanishes as
k � detLL��
� ��, � < 1
� � L�� � �
S � L�q
L��� �0
ZT =�S2
�T � �1�� �� when ���
(G.B., G. Casati, J. Wang, PRL 110, 070604 (2013))
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For systems with more than a single relevant constant of motion, for instance for integrable systems, due to the Schwarz inequality
Equality arises only in the exceptional case when the two vectors are parallel; in general
detL � L2, � � �, ZT � �0
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Example: 1D interacting classical gas
Consider a one dimensional gas of elastically colliding particles with unequal masses: m, M
injection rates
ZT depends on the system size
(integrable model)ZT = 1 (at µ = 0)
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Non-decaying correlation functions
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D��(�) =TN2
2�(mN1 + MN2),
Duu(�) =9T 3N2
8�(mN1 + MN2),
D�u(�) =3T 2N2
4�(mN1 + MN2).
m + M
Finite-size Drude weights: analytical results vs. numerics
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Ballistic behavior of Onsager coefficients
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Anomalous thermal transport
ZT =�S2
kT
(G.B., G. Casati, J. Wang, PRL 110, 070604 (2013))
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Energy-filtering mechanism?At a given position x compute:
Density of particles crossing x from left
Density of particles crossing x from right
“transmission function”
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There is no sign of narrowing of D(E) with increasing the system size L
A mechanism for increasing ZT different from energy filtering is needed
(K. Saito, G.B., G. Casati, Chem. Phys. 375, 508 (2010))
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1D Coulomb gas model
Fourier-like behavior
(S. Chen, J. Wang , G. Casati, G.B., preprint)
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Multiparticle collision dynamics (Kapral model)
Streaming step: free propagation during a time τ
Collision step: random rotations of the velocities of the particles in cells of linear size a with respect to the center of mass velocity:
Momentum is conserved
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The range of linear response shrinks with the system size: Carnot efficiency achieved at zero power
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A free gas of charged interacting particles (electrons,..) has diverging ZT at the thermodynamic limit
2D simulations (Kapral model)
(G.B., G. Casati, C. Mejía-Monasterio, New J. Phys. 16, 015014 (2014))
� = 0
� = 1/5� = 1/2
� = �/4� = �/2
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Noise mimicking disorder effects breaking momentum conservations; correlations decay and ZT saturates
Breaking of momentum conservation
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New mechanism for achieving Carnot efficiency in extended interacting systems, provided:
1) Overall momentum is the only relevant constant of motion (translational invariance of interactions, absence of on-site pinning potential)
2) Absence of dissipative channels
Summary
Mechanism fundamentally different from energy filtering
No dimensionality restrictions, argument applicable also to quantum systems
Possible implementations in high-mobility 2D electron gases? (elastic mean free paths up to tens of microns)
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And when time-reversal is broken?
B applied magnetic field or any parameter breaking time-reversibility
such as the Coriolis force, etc.
X1 = ��µ
X2 = ��� = �T/T 2
� = 1/T
�µ = µL � µR
�� = �L � �R
�T = TL � TR
(we assume TL > TR, µL < µR)
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Constraints from thermodynamics
ONSAGER-CASIMIR RELATIONS:
POSITIVITY OF THE ENTROPY PRODUCTION:
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EFFICIENCY AT MAXIMUM POWER
Output power
maximum when
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Efficiency at maximum power depends on two parameters
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MAXIMUM EFFICIENCY
Maximum efficiency achieved for
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(G.B., K. Saito, G. Casati, PRL 106, 230602 (2011) )
The CA limit can be overcome within linear response
When |x| is large the figure of merit y required to get Carnot efficiency becomes small
Carnot efficiency could be obtained far from the strong coupling condition
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OUTPUT POWER AT MAXIMUM EFFICIENCY
When time-reversibility is broken, within linear response is it possible to have simultaneously Carnot
efficiency and non-zero power.Terms of higher order in the entropy production, beyond linear response, will generally be non-zero. However, irrespective how close we are to the Carnot efficiency, we can find small enough forces such that the linear theory holds.
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Reversible part of the currents
J revi � Lij � Lji
2Xj , i = �, q
J irri � LiiXi +
Lij + Lji
2Xj
S = J�X1 + JqX2 = J irr� X1 + J irr
q X2
The reversible part of the currents do not contribute to entropy production
Possibility of dissipationless transport?
(K. Brandner, K. Saito, U. Seifert, PRL 110, 070603 (2013))
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How to obtain asymmetry in the Seebeck coefficient?
For non-interacting systems, due to the symmetry properties of the scattering matrix
This symmetry does not apply when electron-phonon and electron-electron interactions are taken into account
Let us consider the case of partially coherent transport, with ine las t ic processes s imula ted by “conceptual probes” (Buttiker, 1988).
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Non-interacting three-terminal model
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Three-terminal Onsager matrixEquation connecting fluxes and thermodynamic forces:Equation connecting fluxes and thermodynamic forces:
In block-matrix form:
Zero-particle and heat current condition through the probe terminal:
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Two-terminal Onsager matrix for partially coherent transport
Reduction to 2x2 Onsager matrix when the third terminal is a probe terminal mimicking phase-breaking.
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Illustrative three-dot example
Asymmetric structure, e.g..
First-principle exact calculation within the Landauer-Büttiker multi-terminal approach
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Asymmetric Seebeck coefficient
(K. Saito, G. B., G. Casati, T. Prosen, PRB 84, 201306(R) (2011) )(see also D. Sánchez, L. Serra, PRB 84, 201307(R) (2011) )
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Asymmetric power generation and refrigeration
When a magnetic field is added, the efficiencies of power generation and refrigeration are no longer equal:
To linear order in the applied magnetic field:
A small magnetic field improves either power generation or refrigeration, and vice versa if we reverse the direction of the field
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The large-field enhancement of efficiencies is model-dependent, but the small-field asymmetry is generic
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Optimized efficiency
Optimization by means of simulated annealing
The Curzon-Ahlborn limit can be overcome (within linear response)
(V. Balachandran, G. B., G. Casati, PRB 87, 165419 (2013))
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Transmission windows model
(V. Balachandran, G. B., G. Casati, PRB 87, 165419 (2013));
se also M. Horvat, T. Prosen, G. B., G. Casati, PRE 86, 052102 (2012))
�
i
�ij(E) =�
j
�ij(E) = 1
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Saturation of bounds from the unitarity of S-matrix
Bounds recently obtained for non-interacting 3-terminal transport (K. Brandner, K. Saito, U. Seifert, PRL 110, 070603 (2013))
�(⇥max) =47
�C at x =43
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Magnetic thermal switch (n-terminal setup)
Set voltages (for fixed thermal affinities) to obtain conditions on the currents from a subset K of the n terminals:
(R. Bosisio, S. Valentini, F. Mazza, G.B., V. Giovannetti, R. Fazio, F. Taddei, arXiv:1504.01486 )
J(B) = J(r)(B) + J(i)(B) 56
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Heat current multiplier:
Heat path selector:
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Fully reversible heat:
Heat current swap:
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Example: interferometer model
Fully reversible heat:
(R. Bosisio, S. Valentini, F. Mazza, G.B., V. Giovannetti, R. Fazio, F. Taddei, arXiv:1504.01486 )
Heat path selector:
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Switch also applicable to phononic currents
(O. Entin-Wolman, A. Aharony, PRB 85, 085401 (2012))
Due to electron-phonon coupling the thermal current from the bosonic terminal has a reversible component
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When time-reversal symmetry is broken new thermodynamic bounds on thermoelectric efficiencies are needed.
The CA limit can be overcome within linear response
Carnot efficiency in principle achievable far from the tight coupling regime and with finite power (within linear response)
For partially coherent transport in asymmetric structures the Seebeck coefficient is not an even function of the fieldAsymmetric efficiencies of power generation and refrigeration
The non-interacting cases studied so far exhibit strongly asymmetric thermopower but with low efficiencies. Is this result generic, also beyond linear response and for interacting systems?
Summary
Magnetic thermal switch for heat management
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Multi-terminal thermoelectricityPossibility to exploit additional terminals to decouple charge and heat flows and improve thermoelectric efficiency?
The third terminal is not necessarily a probe
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Multi-terminalt ransport coefficients
Nonlocal thermopowers
Electrical and thermal conductances
�ij
Peltier coefficients
(F. Mazza, R. Bosisio, G. B., V. Giovannetti, R. Fazio, F. Taddei, New J. Phys. 16, 085001 (2014))
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Thermoelectric efficiency
The sum in the denominator is restricted to positive heat currents only
Various instances are possible and for all of them, in the three-terminal case, explicit formulas for the efficiency at maximum power have been worked out
(F. Mazza, R. Bosisio, G. B., V. Giovannetti, R. Fazio, F. Taddei, New J. Phys. 16, 085001 (2014))
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Illustrative example: single dot
Terminal 2 is at temperature between T1 and T3
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Improving power and/or efficiency
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Illustrative example: double dot
In this simple model non-local thermopowers are different from zero
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Heat-charge separation
(F. Mazza, S. Valentini, R. Bosisio, G.B., R. Fazio, V. Giovannetti, F. Taddei, arXiv:1503.01601 )
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Improved thermoelectric performancesStatistics of scattering matrices (within the Sommerfeld regime)
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The third terminal can be useful to improve the thermoelectric performances of a system with respect to the two-terminal case
Possible extensions: - systems with a magnetic field breaking time-reversibility, - bosonic terminals,- systems with time-dependent driving (microscopic thermodynamic cycles)
Summary (part III)
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