Dynamical photo-induced electronic properties of molecular junctions.

Nanoscale molecular-electronic devices and machines are emerging as promising functional elements, naturally flexible and efficient, for next-generation technologies. A deeper understanding of carrier dynamics in molecular junctions is expected to benefit many fields of nanoelectronics and power devices. We determine time-resolved charge current flowing at the donor-acceptor interface in molecular junctions connected to metallic electrodes by means of quantum transport simulations. The current is induced by the interaction of the donor with a Gaussian-shape femtosecond laser pulse. Effects of the molecular internal coupling, metal-molecule tunneling, and light-donor coupling on photocurrent are discussed. We then define the time-resolved local density of states which is proposed as an efficient tool to describe the absorbing molecule in contact with metallic electrodes. Non-equilibrium reorganization of hybridized molecular orbitals through the light-donor interaction gives rise to two phenomena: the dynamical Rabi shift and the appearance of Floquet-like states. Such insights into the dynamical photoelectronic structure of molecules are of strong interest for ultrafast spectroscopy and open avenues toward the possibility of analyzing and controlling the internal properties of quantum nanodevices with pump-push photocurrent spectroscopy.

Thermionic cooling devices based on resonant-tunneling AlGaAs/GaAs heterostructure.

We study by means of full quantum simulations the operating principle and performance of a semiconductor heterostructure refrigerator combining resonant tunneling filtering and thermionic emission. Our model takes into account the coupling between the electric and thermal currents by self-consistently solving the transport equations within the non-equilibrium Green's function framework and the heat equation. We show that the device can achieve relatively high cooling power values, while in the considered implementation, the maximum lattice temperature drop is severely limited by the thermal conductivity of the constituting materials. In such an out-of-equilibrium structure, we then emphasize the significant deviation of the phonon temperature from its electronic counterpart which can vary over several hundred Kelvin. The interplay between those two temperatures and the impact on the electrochemical potential is also discussed. Finally, viable options toward an optimization of the device are proposed.