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The Role of Particle Morphology in Interfacial Energy Transfer in CdSe/CdS Heterostructure Nanocrystals

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Science  03 Dec 2010:
Vol. 330, Issue 6009, pp. 1371-1374
DOI: 10.1126/science.1198070

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An Upside of Asymmetry

Advances in synthetic techniques have enabled the preparation of nanometer-scale semiconductors in a wide range of precise shapes and sizes, including core-shell morphologies that layer several different materials in the same particle. Such two-in-one motifs are promising for light-harvesting applications because they allow optically induced charge separation across the internal interface. Borys et al. (p. 1371) studied a series of rod-shaped cadmium sulfide–cadmium selenide hybrid particles using single-particle–resolved optical spectroscopy and found that smooth versus bulbous geometries produced distinct emission spectra. Further analysis of more complex, tetrapodal particles (with four arms aligned tetrahedrally) suggested that nonuniform geometries facilitate interfacial charge transfer by reducing the likelihood of electronic band misalignment.

Abstract

Nanoscale semiconductor heterostructures such as tetrapods can be used to mimic light-harvesting processes. We used single-particle light-harvesting action spectroscopy to probe the impact of particle morphology on energy transfer and carrier relaxation across a heterojunction. The generic form of an action spectrum [in our experiments, photoluminescence excitation (PLE) under absorption in CdS and emission from CdSe in nanocrystal tetrapods, rods, and spheres] was controlled by the physical shape and resulting morphological variation in the quantum confinement parameters of the nanoparticle. A correlation between single-particle PLE and physical shape as determined by scanning electron microscopy was demonstrated. Such an analysis links local structural non-uniformities such as CdS bulbs forming around the CdSe core in CdSe/CdS nanorods to a lower probability of manifesting excitation energy–dependent emission spectra, which in turn is probably related to band alignment and electron delocalization at the heterojunction interface.

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