Controlling molecular heat conduction using temperature modulations

Over the past decade, there has been growing interest in the field of nanoscale heat transfer, particularly in context of molecular heat conduction. Recently, this interest has sharply increased due to experiments that have measured molecular thermal conductance at the single-molecule level. The broad class of molecular structures that can be realized through advanced molecular synthesis techniques in inorganic, organic, and material chemistry provide possibilities for fabricating molecular structures that could be used to advance the field phononics, that is, using phononic heat transfer to perform complex logic operations. To control these phononic molecular devices, we propose manipulating the heat current through the device by modulating its temperature. Specifically, we explore how modifying thermal transport properties by periodically modulating temperatures of thermal reservoirs in contact with the device can be used to control heat currents at the molecular level. Our theoretical framework includes Langevin dynamics and Nonequilibrium Green's function approaches. Using stochastic molecular dynamics simulations, we confirm the validity of our theoretical approach for examining thermal transport in driven systems. Our results indicate that controlling molecular heat currents using time-periodic temperature modulations could be used to advance the design of molecule-based thermal devices.