Identification of vibration modes in single-molecule junctions by strong inelastic signals in noise

Conductance measurements in single-molecule junctions (SMJs) are on many occasions accompanied by inelastic spectroscopy and shot-noise measurements in order to obtain information about different vibration modes (or vibrons) and channels involved in the transport respectively. We have extended the single-molecule shot-noise measurements, which were previously performed at low bias, to high bias and we have studied the effects of these vibrons on the noise for a Deuterium (D₂) molecule between Pt leads. We report here two important findings from these measurements. First, we find in our noise measurements that at the vibron energies of the molecule, a two-level fluctuation (TLF) is excited in the junction. Second, we show that in the presence of this TLF, a form of enhanced noise spectroscopy can be performed to detect inelastic electron-vibron interactions, by studying the third derivative of the noise (d³S_I/dV³). This is possible because TLFs are insensitive to elastic scattering of electrons from defects, which nevertheless leave their signature in the usual inelastic electron tunnelling spectroscopy (IETS) measurements.