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Register a new userThermoelectric efficiency of single-molecule junctions with long molecular linkers
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Added by
Natalya A. Zimbovskaya
Publication date
2018
fields
Physics
and research's language is
English
Authors
Natalya A. Zimbovskaya
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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) may noticeably affect the length-dependent ZT. Temperature dependences of ZT for various bridge lengths are analyzed. It is shown that broad minima emerge in ZT versus temperature curves whose positions are controlled by the bridge lengths.
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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 employ a sample heater in direct contact with the metallic electrodes contacting the single molecule which allows us to apply temperature biases up to $Delta T = 60$K with minimal heating of the molecular junction. This makes these devices compatible with base temperatures $T_mathrm{bath} <2$K and enables studies in the linear ($Delta T ll T_mathrm{molecule}$) and non-linear ($Delta T gg T_mathrm{molecule}$) thermoelectric transport regimes.
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 Greens 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.
In the present work we theoretically study the length dependence of thermopower of a single-molecule junction with a chain-like molecular bridge of an arbitrary length using a tight-binding model. We analyze conditions bringing a nonlinear growth of the thermopower accompanying the extension of the bridge length. Also, we show that the thermopower may decrease with increasing molecular length provided that the molecular bridge is sufficiently long.
We study the electronic contribution to the main thermoelectric properties of a molecular junction consisting of a single quantum dot coupled to graphene external leads. The system electrical conductivity (G), Seebeck coefficient ($S$), and the thermal conductivity ($kappa$), are numerically calculated based on a Greens function formalism that includes contributions up to the Hartree-Fock level. We consider the system leads to be made either of pure or gapped-graphene. To describe the free electrons in the gapped-graphene electrodes we used two possible scenarios, the massive gap scenario, and the massless gap scenario, respectively. In all cases, the Fano effect is responsible for a strong violation of the Wiedemann-Franz law and we found a substantial increase of the system figure of merit $ZT$ due to a drastic reduction of the system thermal coefficient. In the case of gapped-graphene electrodes, the system figure of merit presents a maximum at an optimal value of the energy gap of the order of $Delta/Dsim$ 0.002 (massive gap scenario) and $Delta/Dsim$ 0.0026 (massless gap scenario). Additionally, for all cases, the system figure of merit is temperature dependent.
We derive the efficiency at maximal power of a scale-invariant (critical) quantum junction in exact form. Both Fermi and Bose statistics are considered. We show that time-reversal invariance is spontaneously broken. For fermions we implement a new mechanism for efficiency enhancement above the Curzon-Ahlborn bound, based on a shift of the particle energy in each heat reservoir, proportional to its temperature. In this setting fermionic junctions can even reach at maximal power the Carnot efficiency. The bosonic junctions at maximal power turn out to be less efficient then the fermionic ones.
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