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Stephen G Hickey

Publications and source records attributed to Stephen G Hickey.

4 recordsLinked to original sources

Variable orbital coupling in a two-dimensional quantum-dot solid probed on a local scale.

The 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. It markedly differs from that of isolated QDs due to electronic coupling in the array. We observe strong local variations in the coupling strength with two prototypical cases: delocalization of the conduction electrons only, and full coupling with both hole and electron delocalization over the QD sites in the array.

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The hidden role of acetate in the PbSe nanocrystal synthesis.

Monodisperse spherical, star-shaped, and octahedral PbSe nanocrystals were synthesized via a hot injection method. We show that the shape and size of the colloidal PbSe nanocrystals are determined by the concentration of acetate and that only acetate-free reaction mixtures result in spherical nanocrystals. The presence of acetate leads to efficient oriented attachment of smaller PbSe nanoparticles along the 100 crystal axis. Comparing different synthesis procedures from the recent literature with our observations, we propose that the acetate, naturally present in insufficiently dried reaction mixtures, is responsible for many of the PbSe crystal shapes reported in the literature. In addition we show that it is possible to synthesize these star-shaped nanocrystals so monodisperse that they form ordered monolayers with crystal alignment.

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Density of states measured by scanning-tunneling spectroscopy sheds new light on the optical transitions in PbSe nanocrystals.

The density-of-states function of individual colloidal PbSe nanocrystals varying in diameter between 3 and 7 nm is measured by resonant tunneling spectroscopy. It is in semiquantitative agreement with tight-binding calculations, but the energy separation between electron (hole) levels of S and P symmetry is systematically smaller than predicted by the theory. These results provide an explanation for the second and third excitonic optical transitions, which have been debated for a long time.

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