Solid state light sources based on integrating commercial near-UV LED chips with encapsulated CdS quantum dots are demonstrated. Blue, blue-green, and white quantum dot LEDs were fabricated with luminous efficiencies of 9.8, 16.6, and 3.5 lm/W, respectively. These are the highest efficiencies reported for quantum dot LEDs. Quantum dots have advantages over conventional micron-sized phosphors for solid state lighting, such as strong absorption of near-UV to blue wavelengths, smaller Stokes shift, and a range of emission colors based on their size and surface chemistry. Alkylthiol-stabilized CdS quantum dots in tetrahydrofuran solvent with quantum yields (QYs) up to 70% were synthesized using room temperature metathesis reactions. A variety of emission colors and a white spectrum from monodisperse CdS quantum dots (D~2 nm) have been demonstrated. The white emission was obtained from the CdS quantum dots directly, by altering the surface chemistry. When incorporated into an epoxy, the high solution phase QY was preserved. In contrast to other approaches, the white LED contains monodisperse CdS quantum dots, rather than a blend of different-size blue, green, and red-emitting quantum dots. The concentration of CdS quantum dots in epoxy can be increased to absorb nearly all of the incident near-UV light of the LED.
Solid state lighting devices that utilize semiconducting nanoparticles (quantum dots) as the sole source of visible light emission have recently been fabricated. The quantum dots in these devices have been demonstrated to have quantum efficiencies similar to those of conventional phosphors. The dispersion and concentration of the nanoparticles within a suitable polymeric matrix was found to be critical to device performance. Yet achieving suitable concentrations and adequate dispersion implies chemical compatibility between the nanoparticles and the matrix, which must be achieved without detrimental effect on either the physical/optical properties of the matrix or the stability/surface state of the quantum dots. A number of encapsulation strategies have been identified and are discussed with regard to their effect on nanoparticle dispersion and concentration within silicone and epoxy matrices.
The optical properties of both II-VI (direct gap) and type IV (indirect gap) nanosize semiconductors are significantly affected not only by their size, but by the nature of the chemical interface of the cluster with the embedding medium. This affects the light conversion efficiency and can alter the shape and position (i.e. the color) of the photoluminescence (PL). As the goal of our work is to embed nanoclusters into either organic or inorganic matrices for use as near UV, LED-excited phosphor thin films, understanding and controlling this interface is very important for preserving the high Q.E. of nanoclusters known for dilute solution conditions.
We describe a room temperature synthesis of semiconductor nanoclusters which employs inexpensive, less toxic ionic precursors (metal salts), and simple coordinating solvents (e.g. tetrahydrofuran). This allows us to add passivating agents, ions, metal or semiconductor coatings to identical, highly dispersed bare clusters, post-synthesis. We can also increase the cluster size by heterogeneous growth on the seed nanoclusters.
One of the most interesting observations for our II-VI nanomaterials is that both the absorbance excitonic features and the photoluminescence (PL) energy and intensity depend on the nature of the surface as well as the average size. In CdS, for example, the presence of electron traps (i.e Cd(II) sites) decreases the exciton absorbance peak amplitude but increases the PL nearly two-fold. Hole traps (i.e. S(II)) have the opposite effect. In the coordinating solvents used for the synthesis, the PL yield for d~2 nm, blue emitting CdSe clusters increases dramatically with sample age as the multiple absorbance features sharpen.
Liquid chromatographic (LC) separation of the nanoclusters from other chemicals and different sized clusters is used to investigate the intrinsic optical properties of the purified clusters and identify which clusters are contributing most strongly to the PL. Both LC and dynamic light scattering, show that as the nanocluster concentration approaches 1 x 10-4M and above, a large loss in light emission occurs due to association or "clumping" of clusters. Overcoming this natural tendency toward aggregation may be the most significant technical obstacle to the use of nanoclusters in thin film phosphors.
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