Nonequilibrium electron-vibration coupling and conductance fluctuations in a C-60 junction

TL;DR: In this article, the authors investigated chemical bond formation and conductance in a molecular C${}_{60}$ junction under finite bias voltage using first-principles calculations based on density functional theory and nonequilibrium Green's functions.

Abstract: We investigate chemical bond formation and conductance in a molecular C${}_{60}$ junction under finite bias voltage using first-principles calculations based on density functional theory and nonequilibrium Green's functions (DFT-NEGF). At the point of contact formation we identify a remarkably strong coupling between the C${}_{60}$ motion and the molecular electronic structure. This is only seen for positive sample bias, although the conductance itself is not strongly polarity dependent. The nonequilibrium effect is traced back to a sudden shift in the position of the voltage drop with a small C${}_{60}$ displacement. Combined with a vibrational heating mechanism we construct a model from our results that explain the polarity-dependent two-level conductance fluctuations observed in recent scanning tunneling microscopy (STM) experiments [N. N\'eel et al., Nano Lett. 11, 3593 (2011)]. These findings highlight the significance of nonequilibrium effects in chemical bond formation/breaking and in electron-vibration coupling in molecular electronics.