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Single molecules are nanoscale thermodynamic systems with few degrees of freedom. Thus, the knowledge of their entropy can reveal the presence of microscopic electron transfer dynamics, that are difficult to observe otherwise. Here, we apply thermocurrent spectroscopy to directly measure the entropy of a single free radical molecule in a magnetic field. Our results allow us to uncover the presence of a singlet to triplet transition in one of the redox states of the molecule, not detected by conventional charge transport measurements. This highlights the power of thermoelectric measurements which can be used to determine the difference in configurational entropy between the redox states of a nanoscale system involved in conductance without any prior assumptions about its structure or microscopic dynamics.
Controlling electronic transport through a single-molecule junction is crucial for molecular electronics or spintronics. In magnetic molecular devices, the spin degree-of-freedom can be used to this end since the magnetic properties of the magnetic i
It is known that the quantum-mechanical ground state of a nano-scale junction has a significant impact on its electrical transport properties. This becomes particularly important in transistors consisting of a single molecule. Due to strong electron-
Single-molecule break junction measurements deliver a huge number of conductance vs. electrode separation traces. Along such measurements the target molecules may bind to the electrodes in different geometries, and the evolution and rupture of the si
The solid-state structures of organic charge transfer (CT) salts are critical in determining their mode of charge transport, and hence their unusual electrical properties, which range from semiconducting through metallic to superconducting. In contra
Using photoemission spectroscopy, we determine the relationship between electronic energy level alignment at a metal-molecule interface and single-molecule junction transport data. We measure the position of the highest occupied molecular orbital (HO