Excitation wavelength independent visible color emission of carbon dots.

Carbon dots (CDs) usually emit a strong blue light and excitation wavelength dependent long wavelength lights. This significantly limits their applications because one has to use a series of different excitation light sources to get different colors and the long wavelength emissions are usually very weak. We found that one type of CDs synthesized from p-phenylenediamine could emit various long wavelength lights (green to red) independent of the excitation wavelength when dispersed in different solvents. The photoluminescence quantum yields of the same CDs were 10-35% in different solvents for different color emissions. Based on this solvent-color effect, we further mixed the same CDs with different polymers to form solid CD films for various color emissions, and these film emissions were also excitation wavelength independent. Multicolor LEDs were demonstrated with the same CDs in solution and solid film states for color displays.

Plasmon-Coupled CdSe/ZnS and CdTe/CdS/ZnS Coreshells for Hybrid Light Emitting Devices.

Plasmon-coupled CdSe/ZnS and CdTe/CdS/ZnS coreshells are investigated for their optoelectronic applications because of their high color purity, wide optical tunability, large PL enhancement, and compact and easy integration into electronic devices. The quantum confinement of carriers within quantum dots (QDs) with sizes near the exciton Bohr radius (CdSe ~ 5.8 nm, CdTe ~ 7 nm) exhibits the features of discrete energy states and blue-shift from the bulk bandgap (CdSe ~718 nm, CdTe ~ 863 nm) in the optical spectrum. While the fluorescence from the QDs is attributable to the exciton carrier recombination, large PL enhancement and fast emission time is achieved through plasmon-exciton coupling via the Coulomb interaction. Large PL enhancement of QDs in the vicinity of plasmonic particles was observed and attributed to the reduction of the non-radiative decay rate and large local field enhancement. The large PL enhancement and wide optical tunability along with high color purity from plasmon-coupled QDs enables the realization of hybrid LEDs.

Hybrid optical materials of plasmon-coupled CdSe/ZnS coreshells for photonic applications.

A hybrid optical nanostructure of plasmon-coupled SQDs was developed for photonic applications. The coupling distances between the mono-layers of Au nanoparticles with a surface concentration of ~9.18 × 10-4 nm-2 and CdSe/ZnS SQDs with that of ~3.7 × 10-3 nm-2 were controlled by PMMA plasma etching. Time-resolved spectroscopy of plasmon-coupled SQDs revealed a strong shortening of the longest lifetime and ~9-fold PL enhancement. Polarization-resolved PL spectroscopy displayed linear polarization and depolarization at near- and far-field plasmon-coupling, respectively. The physical origin of PL enhancement could be attributable to both the large local field enhancement and the fast resonant energy transfer.

Stability study of PbSe semiconductor nanocrystals over concentration, size, atmosphere, and light exposure.

Infrared-emitting PbSe nanocrystals are of increasing interest in both fundamental research and technical application. However, the practical applications are greatly limited by their poor stability. In this work, absorption and photoluminescence spectra of PbSe nanocrystals were utilized to observe the stability of PbSe nanocrystals over several conventional factors, that is, particle concentration, particle size, temperature, light exposure, contacting atmosphere, and storage forms (solution or solid powder). Both absorption and luminescence spectra of PbSe nanocrystals exposed to air showed dependence on particle concentration, size, and light exposure, which caused large and quick blue-shifts in the optical spectra. This air-contacted instability arising from the destructive oxidation and subsequent collision-induced decomposition was kinetically dominated and differed from the traditional thought that smaller particles with lower concentrations shrank fast. The photoluminescence emission intensity of the PbSe nanocrystal solution under ultraviolet (UV) exposure in air increased first and then decreased slowly; without UV irradiation, the emission intensity monotonously decreased over time. However, if stored under nitrogen, no obvious changes in absorption and photoluminescence spectra of the PbSe nanocrystals were observed even under UV exposure or upon being heated up to 100 degrees C.

Size-dependent composition and molar extinction coefficient of PbSe semiconductor nanocrystals.

Atomic compositions and molar extinction coefficients of PbSe semiconductor nanocrystals were determined by atomic absorption spectrometry, UV-vis-NIR spectrophotometry, and transmission electron microscopy. The Pb/Se atomic ratio was found to be size-dependent with a systematic excess of Pb atoms in the PbSe nanocrystal system. Experimental results indicated that the individual PbSe nanocrystal was nonstoichiometric, consisting of a PbSe core and an extra layer of Pb atoms. For these nonstoichiometric PbSe semiconductor nanocrystals, we proposed a new computational approach to calculate the total number of Pb and Se atoms in different sized particles. This calculation played a key role on the accurate determination of the strongly size-dependent extinction coefficient, which followed a power law with an exponent of approximately 2.5.