Coupled electronic states in CdTe quantum dot assemblies fabricated by utilizing chemical bonding between ligands.

Semiconductor quantum dot superlattices (QDSLs) have attracted much attention as key materials for realizing new optoelectronic devices such as solar cells with high conversion efficiency and thermoelectric elements with high electrical conductivity. To improve the charge transport properties of QDSL-based optoelectronic devices, it is important that the QD structures form minibands, which are the coupled electronic states between QDs. A shorter inter-QD distance and a periodic arrangement of QDs are the essential conditions for the formation of minibands. In this study, we use CdTe QDs capped with short ligands of N-acetyl-l cysteine (NAC) to fabricate three-dimensional QD assemblies by utilizing chemical bonding between NACs. Absorption spectra clearly display the quantum resonance phenomenon originating from the coupling of the wave functions between the adjacent QDs in CdTe QD assemblies. Furthermore, we demonstrate the formation of minibands in CdTe QD assemblies by examining both, the excitation energy dependence of photoluminescence (PL) spectra and the detection energy dependence of PL excitation spectra. The fabrication method of QD assemblies utilizing chemical bonding between NACs can be applied to all QDs capped with NAC as a ligand.

Surface modification effects on defect-related photoluminescence in colloidal CdS quantum dots.

We investigated the effects of surface modification on the defect-related photoluminescence (PL) band in colloidal CdS quantum dots (QDs). A size-selective photoetching process and a surface modification technique with a Cd(OH)2 layer enabled the preparation of size-controlled CdS QDs with high PL efficiency. The Stokes shift of the defect-related PL band before and after the surface modification was ∼1.0 eV and ∼0.63 eV, respectively. This difference in the Stokes shifts suggests that the origin of the defect-related PL band was changed by the surface modification. Analysis by X-ray photoelectron spectroscopy revealed that the surface of the CdS QDs before and after the surface modification was S rich and Cd rich, respectively. These results suggest that Cd-vacancy acceptors and S-vacancy donors affect PL processes in CdS QDs before and after the surface modification, respectively.

Temperature dependence of photoluminescence dynamics of self-assembled monolayers of CdSe quantum dots: the influence of the bound-exciton state.

We have investigated the temperature dependence of photoluminescence (PL) dynamics of self-assembled monolayers (SAMs) of CdSe quantum dots (QDs). The PL decay profiles become slower with an increase in temperature up to 160 K, contrary to an ordinary behavior due to thermal quenching. Such anomalous temperature dependence of the PL-decay profile is explained using a four-state model which introduces a bound-exciton state into a conventional three-state model consisting of a ground state and two excited states: a lower-lying dark-exciton state and a higher-lying bright-exciton state. Furthermore, it is proposed that the radiative decay time of QDs is strongly influenced by the presence or absence of the bound-exciton state.

Hydrothermal synthesis of thiol-capped CdTe nanoparticles and their optical properties.

Water soluble nanoparticles (NPs) with a high emission property were synthesized via hydrothermal routes. In this report, we chose thiol ligand N-acetyl-L-cysteine as the ideal stabilizer and have successfully employed it to synthesize readily size-controllable CdTe NPs in a reaction of only one step. Hydrothermal synthesis of CdTe NPs has been carried out in neutral or basic conditions so far. We found out that the pH value of precursor solutions plays an important role in the uniformity of the particle size. Actually, high quality CdTe NPs were synthesized under mild acidic conditions of pH 5. The resultant NPs indicated good visible light-emitting properties and stability. Further, the experimental results showed that the reaction temperature influenced significantly the growth rate and the maximum size of the NPs. The CdTe NPs with a high photoluminescence quantum yield (the highest value: 57%) and narrower half width at half maximum (the narrowest value: 33 nm) were attained in very short time, within 40 minutes, reaching diameters of 2.3 to 4.3 nm. The PL intensity was increased with an increase in the reaction time, reflecting the suppression of nonradiative recombination processes. Furthermore, the formation of CdTe/CdS core-shell structures was discussed from the viewpoint of PL dynamics and X-ray diffraction studies.