No Arabic abstract
Recent observations of destructive quantum interference in single-molecule junctions confirm the role played by quantum effects in the electronic conductance properties of molecular systems. We show here that the destructive interference can be turned ON or OFF within the same molecular system by mechanically controlling its conformation. Using a combination of ab-initio calculations and single-molecule conductance measurements, we demonstrate the existence of a quasi-periodic destructive quantum interference pattern along the breaking traces of {pi}-{pi} stacked molecular dimers. The detection of these interferences, which are due to opposite signs of the intermolecular electronic couplings, was only made possible by a combination of wavelet transform and higher-order statistical analysis of single-breaking traces. The results demonstrate that it is possible to control the molecular conductance over a few orders of magnitudes and with a sub-angstrom resolution by exploiting the subtle structure-property relationship of {pi}-{pi} stack dimers. These large conductance changes may be beneficial for the design of single-molecule electronic components that exploit the intrinsic quantum effects occurring at the molecular scale.
The ability to detect and distinguish quantum interference signatures is important for both fundamental research and for the realization of devices including electron resonators, interferometers and interference-based spin filters. Consistent with the principles of subwavelength optics, the wave nature of electrons can give rise to various types of interference effects, such as Fabry-Perot resonances, Fano resonances and the Aharonov-Bohm effect. Quantum-interference conductance oscillations have indeed been predicted for multiwall carbon nanotube shuttles and telescopes, and arise from atomic-scale displacements between the inner and outer tubes. Previous theoretical work on graphene bilayers indicates that these systems may display similar interference features as a function of the relative position of the two sheets. Experimental verification is, however, still lacking. Graphene nanoconstrictions represent an ideal model system to study quantum transport phenomena due to the electronic coherence and the transverse confinement of the carriers. Here, we demonstrate the fabrication of bowtie-shaped nanoconstrictions with mechanically controlled break junctions (MCBJs) made from a single layer of graphene. We find that their electrical conductance displays pronounced oscillations at room temperature, with amplitudes that modulate over an order of magnitude as a function of sub-nanometer displacements. Surprisingly, the oscillations exhibit a period larger than the graphene lattice constant. Charge-transport calculations show that the periodicity originates from a combination of quantum-interference and lattice-commensuration effects of two graphene layers that slide across each other. Our results provide direct experimental observation of Fabry-Perot-like interference of electron waves that are partially reflected/transmitted at the edges of the graphene bilayer overlap region.
Twist-engineering of the electronic structure of van-der-Waals layered materials relies predominantly on band hybridization between layers. Band-edge states in transition-metal-dichalcogenide semiconductors are localized around the metal atoms at the center of the three-atom layer and are therefore not particularly susceptible to twisting. Here, we report that high-lying excitons in bilayer WSe2 can be tuned over 235 meV by twisting, with a twist-angle susceptibility of 8.1 meV/{deg}, an order of magnitude larger than that of the band-edge A-exciton. This tunability arises because the electronic states associated with upper conduction bands delocalize into the chalcogenide atoms. The effect gives control over excitonic quantum interference, revealed in selective activation and deactivation of electromagnetically induced transparency (EIT) in second-harmonic generation. Such a degree of freedom does not exist in conventional dilute atomic-gas systems, where EIT was originally established, and allows us to shape the frequency dependence, i.e. the dispersion, of the optical nonlinearity.
Nuclear polarization dynamics are measured in the nuclear spin bi-stability regime in a single optically pumped InGaAs/GaAs quantum dot. The controlling role of nuclear spin diffusion from the dot into the surrounding material is revealed in pump-probe measurements of the non-linear nuclear spin dynamics. We measure nuclear spin decay times in the range 0.2-5 sec, strongly dependent on the optical pumping time. The long nuclear spin decay arises from polarization of the material surrounding the dot by spin diffusion for long (>5sec) pumping times. The time-resolved methods allow the detection of the unstable nuclear polarization state in the bi-stability regime otherwise undetectable in cw experiments.
We report on stacked multiple quantum dots (QDs) formed inside inverted pyramidal recesses, which allow for the precise positioning of the QDs themselves. Specifically we fabricated double QDs with varying inter-dot distance and ensembles with more than two nominally highly symmetric QDs. For each, the effect of the interaction between QDs is studied by characterizing a large number of QDs through photoluminescence spectroscopy. A clear red-shift of the emission energy is observed together with a change in the orientation of its polarization, suggesting an increasing interaction between the QDs. Finally we show how stacked QDs can help influencing the charging of the excitonic complexes.
Linear in the wave-vector terms of an electron Hamiltonian play an important role in topological insulators and spintronic devices. Here we demonstrate how an external electric field controls the magnitude of a linear-in-K term in the exciton Hamiltonian in wide GaAs quantum wells. The dependence of this term on the applied field in a high quality sample was studied by means of the differential reflection spectroscopy. An excellent agreement between the experimental data and the results of calculations using semi-classical non-local dielectric response model confirms the validity of the method and paves the way for the realisation of excitonic Datta-and-Das transistors. In full analogy with the spin-orbit transistor proposed by Datta and Das [Appl. Phys. Lett. {bf 56}, 665 (1990)], the switch between positive and negative interference of exciton polaritons propagating forward and backward in a GaAs film is achieved by application of an electric field with non-zero component in the plane of the quantum well layer.