Presently, solid-state Peltier coolers for electronic circuits, usage is limited by their small efficiency due to the high phononic contribution to thermal conductance. In recent years, there has been a growing experimental and theoretical interest to explore nanowires and devices where a single molecule is attached to metallic or semiconducting electrodes for thermoelectric applications.
In such devices, the dimensionality reduction and possible strong electronic correlations can make it possible to tune the electronic transport properties while keeping a low phononic thermal conductance, leaving room for further optimization of the nanodevice efficiency. In the first part of this talk, I will give a brief description of the density functional theory (DFT) and nonequilibrium Green’s function formalism (NEGF) used in the calculation of the electronic structure, charge and heat transport in nanoscale devices. Next part will be a focused discussion on a few results (theory and experiment) and challenges in single molecular thermoelectrics optimization. Finally, I will give an overview on current development with machine learning usage for electronic structure, new material discovery and quantum transport.