The study of thermoelectricity in molecular junctions is of fundamental interest for the development of various technologies including cooling and heat-to-electricity conversion. Recent experimental progress in probing the Seebeck effect of molecular junctions has enabled studies of the relationship between thermoelectricity and molecular structure. However, observations of Peltier cooling—a critical step for establishing molecular-based refrigeration—have remained inaccessible. Here, we report direct observations of Peltier cooling in molecular junctions . By integrating conducting-probe atomic force microscopy with custom-fabricated picowatt-resolution microdevices, we created an experimental platform that enables the unified characterization of electrical, thermoelectric and energy dissipation characteristics of molecular junctions. Using this platform, we studied gold junctions with prototypical molecules (Au–biphenyl-4,4′-dithiol–Au, Au–terphenyl-4,4′′-dithiol–Au and Au–4,4′-bipyridine–Au) and revealed the relationship between heating or cooling and charge transmission characteristics. We expect these advances to stimulate studies of both thermal and thermoelectric transport in molecular junctions where the possibility of extraordinarily efficient energy conversion has been theoretically predicted.
 L. Cui et al., Peltier cooling in molecular junctions, Nature Nanotechnology (2017). doi:10.1038/s41565-017-0020-z