Radical enhancement of molecular thermoelectric efficiency

Abstract

There is a worldwide race to find materials with high thermoelectric efficiency to convert waste heat to useful energy in consumer electronics and server farms. Here, we propose a radically new method to enhance simultaneously the electrical conductance and thermopower and suppress heat transport through ultra-thin materials formed by single radical molecules. This leads to a significant enhancement of room temperature thermoelectric efficiency. The proposed strategy utilises the formation of transport resonances due to singly occupied spin orbitals in radical molecules. This enhances the electrical conductance by a couple of orders of magnitude in molecular junctions formed by nitroxide radicals compared to the non-radical counterpart. It also increases the Seebeck coefficient to high values of 200 μV K⁻¹. Consequently, the power factor increases by more than two orders of magnitude. In addition, the asymmetry and destructive phonon interference that was induced by the stable organic radical side group significantly decreases the phonon thermal conductance. The enhanced power factor and suppressed thermal conductance in the nitroxide radical lead to the significant enhancement of room temperature ZT to values ca. 0.8. Our result confirms the great potential of stable organic radicals to form ultra-thin film thermoelectric materials with unprecedented thermoelectric efficiency.