Intramolecular single electron transfer plays important role in many processes in nature and it is frequently accompanied by energy dissipation to environment [1]. Detailed mechanism of such processes depends on electron transfer rates, internal molecular relaxation and energy dissipation to environment. However, studies of electron transfer and accompanied energy dissipation processes in a single molecule represent still the challenge [2]. Here we demonstrate that atomic force microscopy (AFM) can control mixed valence state [3] and the electron transfer between different redox centers within a single molecule. What is more, it allows to detect underlying energy dissipation to its environment. Back action of single electron tunneling between two redox centers on oscillating scanning probe allows us to determine average switching rate [4] and dissipated energy as function of temperature. We found the dependence of switching rate on temperature to be negligible. This demonstrates that the continuous intramolecular electron transfer drives the molecule out of its thermal equilibrium. We anticipate our work may open new possibilities to study mixed valence state molecular systems and the quantum dissipation out of equilibrium on single molecular level using atomic force microscopy. For example, it may reveal influence of distinct functional molecular groups on dissipation processes on atomic scale. Strong coupling between the single electron transfer within single molecule and dynamics of macroscopic probe may also define novel single molecular nanoelectromechanical systems.

Quantum dissipation driven by electron transfer within a single molecule investigated by means of atomic force microscopy

2019 Fall National Meeting

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