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The synthesis of epitaxially grown, wurtzite CdSe/CdS core/shell nanocrystals is reported. Shells of up to three monolayers in thickness were grown on cores ranging in diameter from 23 to 39 Å. Shell growth was controllable to within a tenth of a monolayer and was consistently accompanied by a red shift of the absorption spectrum, an increase of the room temperature photoluminescence quantum yield (up to at least 50%), and an increase in the photostability. Shell growth was shown to be uniform and epitaxial by the use of X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), high resolution transmission electron microscopy (HRTEM), and optical spectroscopy. The experimental results indicate that in the excited state the hole is confined to the core and the electron is delocalized throughout the entire structure. The photostability can be explained by the confinement of the hole, while the delocalization of the electron results in a degree of electronic accessibility that makes these nanocrystals attractive for use in optoelectronic devices.

We report experiments on bilayer light emitting diodes made with organically capped CdSe(CdS) core/shell type semiconductor nanocrystals and an electroluminescent (EL) semiconducting polymer [poly(p-phenylenevinylene) or PPV]. The devices emit from red to green with external quantum efficiencies of up to 0.22% at brightnesses of 600 cd/m2 and current densities of 1 A/cm2. They have operating voltages as low as 4 V and lifetimes under constant current flow of hundreds of hours. Most of these numbers are significant improvements over similar devices made with CdSe nanocrystals. The devices show either nanocrystal-only EL or a combination of nanocrystal and PPV EL, depending on nanocrystal layer thickness. The nanocrystal EL is dependent on nanocrystal size. Some devices show a voltage dependent spectral output. The spectral output is consistent with a field dependent electron range in the nanocrystal layer limited by carrier trapping.

A new mechanism of electron paramagnetic resonance in spherical zinc-blende semiconductor nanocrystals, based on the extended orbital motion of electrons in the entire nanocrystal, is presented. Quantum confinement plays a crucial role in making the resonance signal observable. The mechanism remains operative in nanocrystals with uniaxially distorted shape. A theoretical model based on the proposed mechanism is in good quantitative agreement with unusual ODMR spectra observed in nearly spherical CdSe nanocrystals.Comment: 4 pages, 2 figure