Molecular Electronic Junctions Achieved High Thermal Switch Ratios in Atomistic Simulations.

Abstract

The development of devices that improve thermal energy management requires thermal regulation with efficiency comparable to the ratios R ∼ 105 in electric regulation. Unfortunately, current materials and devices in thermal regulators have only been reported to achieve R ∼ 10. We use atomistic simulations to demonstrate that Ferrocenyl (Fc) molecules under applied external electric fields can alter charge states and achieve high thermal switch ratios R = Gq/G0, where Gq and G0 are the high and low limiting conductances. When an electric field is applied, Fc molecules are positively charged, and the SAM-Au interfacial interaction is strong, leading to high heat conductance Gq. On the other hand, with no electric field, the Fc molecules are charge neutral and the SAM-Au interfacial interaction is weak, leading to low heat conductance G0. We optimized various design parameters for the device performance, including the Au-to-Au gap distance L, the system operation temperature T, the net charge on Fc molecules q, the Au surface charge number Z, and the SAM number N. We find that Gq can be very large and increases with increasing q, Z, or N, while G0 is near 0 at L > 3.0 nm. As a result, R > 100 was achieved for selected parameter ranges reported here.