Particle exchange heat engines are a novel class of cyclic heat engines that are all-electrical, contain no moving parts and can therefore be scaled down to nanometer size. At the center of their operation is the manipulation of a particle flow between a hot and a cold reservoir through energy filtering mechanisms, where their efficiency depends primarily on the sharpness of the energy filter. In this study, we investigate the efficiency enhancement of such engines by utilizing ultra-sharp transmission resonances formed by magnetic impurities interacting with superconductors, known as Yu-Shiba-Rusinov bound states. To this end, we couple a neutral and stable diradical molecule to superconducting break-junction electrodes, and study its thermoelectric properties at ultra-low temperatures. By driving the molecular heat engine through a phase transition from a Kondo state into the Yu-Shiba-Rusinov regime, we observe a five fold increase in the thermoelectric power factor. This observation could pave the way for practical applications such as cryogenic waste heat recovery and efficient spot-cooling for future quantum computing architectures.

Heat-to-charge conversion efficiency of thermoelectric materials is closely linked to the entropy per charge carrier. Thus, magnetic materials are promising building blocks for highly efficient energy harvesters as their carrier entropy is boosted by a spin degree of freedom. In this work, we investigate how this spin-entropy impacts heat-to-charge conversion in the A-type antiferromagnet CrSBr. We perform simultaneous measurements of electrical conductance and thermocurrent while changing magnetic order using the temperature and magnetic field as tuning parameters. We find a strong enhancement of the thermoelectric power factor at around the Néel temperature. We further reveal that the power factor at low temperatures can be increased by up to 600% upon applying a magnetic field. Our results demonstrate that the thermoelectric properties of 2D magnets can be optimized by exploiting the sizable impact of spin-entropy and confirm thermoelectric measurements as a sensitive tool to investigate subtle magnetic phase transitions in low-dimensional magnets.

Thermocurrent flowing through a single-molecule device contains valuable information about the quantum properties of the molecular structure and, in particular, on its electronic and phononic excitation spectra and entropy. Furthermore, accessing the thermoelectric heat-to-charge conversion efficiency experimentally can help to select suitable molecules for future energy conversion devices, which - predicted by theoretical studies - could reach unprecedented efficiencies. However, one of the major challenges in quantifying thermocurrents in nanoscale devices is to determine the exact temperature bias applied to the junction. In this work, we have incorporated a superconductor-normal metal-superconductor Josephson junction thermometer into a single-molecule device. The critical current of the Josephson junction depends accurately on minute changes in the electronic temperature in a wide temperature range from 100 mK to 1.6 K. Thus, we present a device architecture which can enable thermoelectric experiments on single molecules down to millikelvin temperatures with high precision.