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We fabricate artificial molecules composed of heavy atom lead on a van der Waals crystal. Pb atoms templated on a honeycomb charge-order superstructure of IrTe2 form clusters ranging from dimers to heptamers including benzene-shaped ring hexamers. Tunneling spectroscopy and electronic structure calculations reveal the formation of unusual relativistic molecular orbitals within the clusters. The spin-orbit coupling is essential both in forming such Dirac electronic states and stabilizing the artificial molecules by reducing the adatom-substrate interaction. Lead atoms are found to be ideally suited for a maximized relativistic effect. This work initiates the use of novel two dimensional orderings to guide the fabrication of artificial molecules of unprecedented properties.
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The spin-orbit interaction is a crucial element of many semiconductor spintronic technologies. Here we report the first experimental observation, by magneto-optical spectroscopy, of a remarkable consequence of the spin-orbit interaction for holes confined in the molecular states of coupled quantum dots. As the thickness of the barrier separating two coupled quantum dots is increased, the molecular ground state changes character from a bonding orbital to an antibonding orbital. This result is counterintuitive, and antibonding molecular ground states are never observed in natural diatomic molecules. We explain the origin of the reversal using a four band k.p model that has been validated by numerical calculations that account for strain. The discovery of antibonding molecular ground states provides new opportunities for the design of artificially structured materials with complex molecular properties that cannot be achieved in natural systems.
The many-body state of carriers confined in a quantum dot is controlled by the balance between their kinetic energy and their Coulomb correlation. In coupled quantum dots, both can be tuned by varying the inter-dot tunneling and interactions. Using a theoretical approach based on the diagonalization of the exact Hamiltonian, we show that transitions between different quantum phases can be induced through inter-dot coupling both for a system of few electrons (or holes) and for aggregates of electrons and holes. We discuss their manifestations in addition energy spectra (accessible through capacitance or transport experiments) and optical spectra.
Recent advancement in fabrication technologies enable the construction of nano-objects with rather rich internal structures such as double or triple quantum dots, which can then be regarded as artificial molecules. The main new ingredient in the study of the Kondo effect in such artificial (and also in natural) molecules is the internal symmetry of the nano-object, which proves to play a crucial role in the construction of the effective exchange Hamiltonian. This internal symmetry combines continuous spin symmetry SU(2) and discrete point symmetry (such as mirror reflections for double dots or discrete $C_{3v}$ rotation for equilateral triangular dots. When these artificial molecules are attached to metallic leads, the set of dot operators appearing in the effective exchange Hamiltonian generate a group which is refereed to as the dynamical symmetry group of the system dot-leads [mostly SO(n) or SU(n)], and the pertinent group parameters (such as the value of $n$) can be controlled by experiment. In this short review we clarify and expand these concepts and discuss some specific examples. In particular we concentrate on the difference between the chain geometry and the ring geometry. When a perpendicular magnetic field is applied in the ring geometry, its gauge symmetry U(1) is involved in the interplay with the spin and orbital dynamics of the dot.
The optical properties of hybrid molecules composed of semiconductor and metal nanoparticles with a weak probe in a strong pump field are investigated theoretically. Excitons in such a hybrid molecule demonstrate novel optical properties due to the coupling between exciton and plasmon. It is shown that a non-absorption hole induced by coherent population oscillation appears at the absorption spectrum of the probe field and there exists slow light effect resulting in the great change of the refractive index. The numerical results indicate that with the different center-to-center distance between the two nanopaticles the slow light effects are greatly modified in terms of exciton-plasmon couplings.
We report the Coulomb mediated hybridization of excitonic states in an optically active, artificial quantum dot molecule. By probing the optical response of the artificial molecule as a function of the static electric field applied along the molecular axis, we observe unexpected avoided level crossings that do not arise from the dominant single particle tunnel coupling. We identify a new few-particle coupling mechanism stemming from Coulomb interactions between different neutral exciton states. Such Coulomb resonances hybridize the exciton wave function over four different electron and hole single-particle orbitals. Comparisons of experimental observations with microscopic 8-band $k cdot p$ calculations taking into account a realistic quantum dot geometry show good agreement and reveal that the Coulomb resonances arise from broken symmetry in the artificial molecule.
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