Nonequilibrium electron-vibration coupling and conductance fluctuations in a C60-junction

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We investigate chemical bond formation and conductance in a molecular C60-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 C60-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 a sudden shift in the position of the voltage drop with a small C60-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. Néel 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.