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- Fei Zhan

Fei
Zhan

Heat transport in molecular junctions

Supervisor: Prof. Dr. Peter Hänggi
[Theoretical physics I]

Date of oral examination:
12/16/2011

69 pages,
english
In this thesis we consider heat transport in molecular junctions. We analyze the fluctuations of an electronic heat current across a molecular wire. The wire is composed of a single energy level, which connects two leads that are held at different temperatures. By use of the Green function method we derive an explicit expression for the power spectral density of the emerging heat noise. This result assumes a form that is quite distinct from the power spectral density of the accompanying electric current noise. The complex expression simplifies considerably in the limit of zero frequency, yielding the heat noise intensity. The heat noise spectral density still depends on the frequency in the zero-temperature limit, assuming different asymptotic behaviors in the low- and high-frequency regions. These findings evidence that heat transport across molecular junctions can exhibit a rich structure beyond the common behavior that emerges in the linear response limit. To control the heat current, we design a quantum heat ratchet. We explore heat transport in molecular junctions between two leads in the absence of a finite net thermal bias. The application of an unbiased time-periodic temperature modulation of the leads entails a dynamical breaking of reflection symmetry, such that a directed heat current may emerge (ratchet effect). In particular, we consider two cases of adiabatically slow driving, namely, (i) periodic temperature modulation of only one lead and (ii) temperature modulation of both leads with an ac driving that contains a second harmonic, thus, generating harmonic mixing. Both scenarios yield sizeable directed heat currents, which should be detectable with present techniques. Adding a static thermal bias allows one to compute the heat current-thermal load characteristics, which includes the ratchet effect of negative thermal bias with positive-valued heat flow against the thermal bias, up to the thermal stop load. The ratchet heat flow in turn generates also an electric current. An applied electric stop voltage, yielding effective zero electric current flow, then mimics a solely heat-ratchet-induced thermopower (%93ratchet Seebeck effect%94), although no net thermal bias is acting. Moreover, we find that the relative phase between the two harmonics in scenario (ii) enables steering the net heat current into a direction of choice.

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