Control 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. Photonic crystals provide such an environment: they strongly modify the vacuum fluctuations, causing the decay of emitted light to be accelerated or slowed down, to reveal unusual statistics, or to be completely inhibited in the ideal case of a photonic bandgap. Here we study spontaneous emission from semiconductor quantum dots embedded in inverse opal photonic crystals. We show that the spectral distribution and time-dependent decay of light emitted from excitons confined in the quantum dots are controlled by the host photonic crystal. Modified emission is observed over large frequency bandwidths of 10%, orders of magnitude larger than reported for resonant optical microcavities. Both inhibited and enhanced decay rates are observed depending on the optical emission frequency, and they are controlled by the crystals' lattice parameter. Our experimental results provide a basis for all-solid-state dynamic control of optical quantum systems.
Through 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.
Molecules, 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. We discuss the conditions under which shell-tunnelling, shell-filling and bipolar spectroscopy can be performed, and illustrate this with spectra acquired on individual CdSe and PbSe quantum dots. We conclude that quantitative information on the energy levels and Coulomb interactions can be obtained if the physics of the tip/quantum dot/substrate double-barrier tunnel junction is well understood.
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