Nonequilibrium Seebeck effect and thermoelectric efficiency of Kondo-correlated molecular junctions (2301.10506v1)

Abstract: We theoretically study the nonequilibrium thermoelectric transport properties of a strongly-correlated molecule (or quantum dot) embedded in a tunnel junction. Assuming that the coupling of the molecule to the contacts is asymmetric, we determine the nonlinear current driven by the voltage and temperature gradients by using the perturbation theory. However, the subsystem consisting of the molecule strongly coupled to one of the contacts is solved by using the numerical renormalization group method, which allows for accurate description of Kondo correlations. We study the temperature gradient and voltage dependence of the nonlinear and differential Seebeck coefficients for various initial configurations of the system. In particular, we show that in the Coulomb blockade regime with singly occupied molecule, both thermopowers exhibit sign changes due to the Kondo correlations at nonequilibrium conditions. Moreover, we determine the nonlinear heat current and thermoelectric efficiency, demonstrating that the system can work as a heat engine with considerable efficiency, depending on the transport regime.