Full thermoelectric characterization of a single molecule.

Molecules are predicted to be chemically tunable towards high thermoelectric efficiencies and they could outperform existing materials in the field of energy conversion. However, their capabilities at the more technologically relevant temperature of 300 K are yet to be demonstrated. A possible reason could be the lack of a comprehensive technique able to measure the thermal and (thermo)electrical properties, including the role of phonon conduction. Here, by combining the break junction technique with a suspended heat-flux sensor, we measured the total thermal and electrical conductance of a single molecule, at room temperature, together with its Seebeck coefficient. We used this method to extract the figure of merit zT of a tailor-made oligo(phenyleneethynylene)-9,10-anthracenyl molecule with dihydrobenzo[b]thiophene anchoring groups (DHBT-OPE3-An), bridged between gold electrodes. The result is in excellent agreement with predictions from density functional theory and molecular dynamics. This work represents the first measurement, within the same setup, of experimental zT of a single molecule at room temperature and opens new opportunities for the screening of several possible molecules in the light of future thermoelectric applications. The protocol is verified using SAc-OPE3, for which individual measurements for its transport properties exist in the literature.

Ultra-stable dry cryostat for variable temperature break junction.

We present the design of a variable temperature setup that uses a pulse tube cryocooler to perform break-junction experiments at variable temperatures ranging from 12 K to room temperature. The use of pulse tube coolers is advantageous because they are easy to use, can be highly automatized, and used to avoid wastage of cryogenic fluids. This is the reason why dry cryostats are conquering more and more fields in cryogenic physics. However, the main drawback is the level of vibration that can be up to several micrometers at the cold-head. The vibrations make the operation of scanning probe-based microscopes challenging. We implemented vibration-damping techniques that allow obtaining a vibration level of 12 pm between the tip and sample. With these adaptations, we show the possibility to perform break junction measurements in a cryogenic environment and keep in place atomic chains of a few nanometers between the two electrodes.