Thermoelectric transport with electron-phonon coupling and electron-electron interaction in molecular junctions

Jie Ren, Jian-Xin Zhu, James E. Gubernatis, Chen Wang, Baowen Li

Published 2011-06-26, updated 2012-04-25Version 3

Within the framework of nonequilibrium Green's functions, we investigate the thermoelectric transport in a single molecular junction with electron-phonon and electron-electron interactions. By transforming into a displaced phonon basis, we are able to deal with these interactions non-perturbatively. Then, by invoking the weak tunneling limit, we are able to calculate the thermoelectricity. Results show that at low temperatures, resonances of the thermoelectric figure of merit ZT occur around the sides of resonances of electronic conductance but drops dramatically to zero at exactly these resonant points. We find ZT can be enhanced by increasing electron-phonon coupling and Coulomb repulsion, and an optimal enhancement is obtained when these two interactions are competing. Our results indicate a great potential for single-molecular-junctions as good thermoelectric devices over a wide range of temperatures.