Binary nanocrystal superlattices, that is, ordered structures of two sorts of nanocolloids, hold promise for a series of functional materials with novel collective properties. Here we show that based on electron tomography a comprehensive, quantitative, three-dimensional characterization of these systems down to the single nanocrystal level can be achieved, which is key in understanding the emerging materials properties. On four binary lattices composed of PbSe, CdSe, and Au nanocrystals, we illustrate that ambiguous interpretations based on two-dimensional transmission electron microscopy can be prevented, nanocrystal sizes and superlattice parameters accurately determined, individual crystallographic point and plane defects studied, and the order/disorder at the top and bottom surfaces imaged.
View Article and Find Full Text PDFThe electronic local density of states (LDOS) of single PbSe quantum dots (QDs) and QD molecules is explored using low-temperature scanning tunneling microscopy (STM) and spectroscopy (STS). Both individual PbSe QDs and molecular aggregates of PbSe QDs (dimers, trimers, etc.) are mechanically stabilized in a two-dimensional superlattice of wide band gap CdSe QDs acting as an inert matrix.
View Article and Find Full Text PDFWe use scanning tunnelling microscopy (STM) to controllably contact individual CdSe quantum dots (QDs) in a multilayer array to study electrical contacts to a model QD solid. The probability of electron injection into the QD array depends strongly on the symmetry of the QD wave functions and their response to the local electric field. Quantitative spectroscopy of the QD energy levels is possible if the potential distribution in the STM tip-QD array-substrate system is taken into account.
View Article and Find Full Text PDFThrough the mechanism of "oriented attachment", small nanocrystals can fuse into a wide variety of one- and two-dimensional nanostructures. This fusion phenomenon is investigated in detail by low-temperature annealing of a two-dimensional array of 10 nm-sized PbSe nanocrystals, in situ in the transmission electron microscope. We have revealed a complex chain of processes; after coalescence, the connected nanocrystals undergo consecutive rotations in three-dimensional space, followed by drastic interfacial relaxations whereby full fusion is obtained.
View Article and Find Full Text PDFIn this paper we show that self-organization of colloidal PbSe and CdSe semiconductor nanocrystals with a size ratio of 0.57 leads to binary structures with a AB2 or a cuboctahedral AB13 lattice. The type of superlattice formed can be regulated by the relative concentration of both nanocrystals in the suspension.
View Article and Find Full Text PDFThe optoelectronic properties of semiconductor quantum-dot (QD) solids depend on the electronic structure of the building blocks and their interactions. Disorder may affect the coupling on a local scale. We have measured the density of states of 2D arrays of PbSe QDs site by site using scanning tunneling spectroscopy.
View Article and Find Full Text PDFMolecules, supramolecular structures and semiconductor nanocrystals are increasingly used as the active components in prototype opto-electrical devices with miniaturized dimensions and novel functions. Therefore, there is a strong need to measure the electronic structure of such single, individual nano-objects. Here, we explore the potential of scanning tunnelling spectroscopy to obtain quantitative information on the energy levels and Coulomb interactions of semiconductor quantum dots.
View Article and Find Full Text PDFControl of spontaneously emitted light lies at the heart of quantum optics. It is essential for diverse applications ranging from miniature lasers and light-emitting diodes, to single-photon sources for quantum information, and to solar energy harvesting. To explore such new quantum optics applications, a suitably tailored dielectric environment is required in which the vacuum fluctuations that control spontaneous emission can be manipulated.
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