The development of optical gain in chemically synthesized semiconductor nanoparticles (nanocrystal quantum dots) has been intensely studied as the first step toward nanocrystal quantum dot lasers. We examined the competing dynamical processes involved in optical amplification and lasing in nanocrystal quantum dots and found that, despite a highly efficient intrinsic nonradiative Auger recombination, large optical gain can be developed at the wavelength of the emitting transition for close-packed solids of these dots. Narrowband stimulated emission with a pronounced gain threshold at wavelengths tunable with the size of the nanocrystal was observed, as expected from quantum confinement effects. These results unambiguously demonstrate the feasibility of nanocrystal quantum dot lasers.

We have resolved single-exponential relaxation dynamics of the 2-, 3-, and 4-electron-hole pair states in nearly monodisperse cadmium selenide quantum dots with radii ranging from 1 to 4 nanometers. Comparison of the discrete relaxation constants measured for different multiple-pair states indicates that the carrier decay rate is cubic in carrier concentration, which is characteristic of an Auger process. We observe that in the quantum-confined regime, the Auger constant is strongly size-dependent and decreases with decreasing the quantum dot size as the radius cubed.

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An elusive goal for systemic drug delivery is to provide both spatial and temporal control of drug release. Liposomes have been evaluated as drug delivery vehicles for decades 1-5 , but their clinical significance has been limited by slow release or poor availability of the encapsulated drug 6 . Here we show that near-complete liposomal release can be initiated within seconds by irradiating hollow gold nanoshells (HGNs) with a near-infrared (NIR) pulsed laser. Our findings reveal that different coupling methods, such as having the HGNs tethered to, encapsulated within, or suspended freely outside the liposomes, all triggered liposomal release but with different levels of efficiency. For the underlying content release mechanism, our experiments suggest that microbubble formation and collapse due to the rapid temperature increase of the HGN is responsible for liposome disruption, as evidenced by the formation of solid gold particles after NIR irradiation and the coincidence of a laser power threshold for both triggered release and pressure fluctuations in the solution associating with cavitations. These effects are similar to those induced by ultrasound and our approach is conceptually analogous to use optically triggered nano-"sonicators" deep inside the body for drug delivery. We expect HGNs can be coupled with any nanocarriers to promote spatially and temporally controlled drug release. In addition, the capability of external HGNs to permeabilize lipid membranes can facilitate the cellular uptake of macromolecules, including proteins and DNA and allow for promising applications in gene therapy.One major challenge for current drug delivery is to control the drug release both spatially and temporally. Liposomes have been evaluated as drug delivery vehicles for decades 1-5 , but their clinical significance has been limited by slow release or poor availability of the encapsulated drug 6 . Here we show that near-complete liposomal release can be initiated within seconds ("burst" kinetics) by irradiating hollow gold nanoshells (HGNs) with a near-infrared (NIR) pulsed laser. Tissues are relatively transparent to NIR light which penetrates into body up to 10 cm 7 . This allows these HGN/liposome complexes to be addressed non-invasively within a significant fraction of the human body. Our findings on the underlying release mechanism reveal that this approach is conceptually analogous to using optically triggered nano-"sonicators" deep inside the body for drug delivery. Email: gorilla@engineering.ucsb Liposomes optimized to be highly stable and resistant to drug leakage in the circulation 8,9 are hampered by suboptimal drug release to serve as drug carriers. Current endogenous strategies in drug release have focused on incorporating components into liposomes to achieve either thermal, pH, enzymatically triggered or receptor-targeted liposomes 3-5 , however, none of them has led to marketed drugs 10 . It is difficult to include a destabilizing agent into the liposomes to promote release without compromising their ...

A series of organic- and water-soluble distyrylbenzene-based two-photon absorption (TPA) fluorophores containing dialkylamino donor groups at the termini was designed, synthesized, and characterized. The central core was systematically substituted to modulate intramolecular charge transfer (ICT). These molecules allow an examination of solvent effects on the TPA cross section (delta) and on the TPA action cross section. In toluene, the delta values follow the order of ICT strength. The effect of solvent on delta is nonmonotonic: maximum delta was measured in an intermediate polarity solvent (THF) and was lowest in water. We failed to find a correlation between the observed solvent effect and previous theoretical predictions. Hydrogen bonding to the donor groups and aggregation of the optical units in water, which are not included in calculational analysis, may be responsible for the discrepancies between experimental results and theory.

The orthosilicate phosphors Sr x Ba2–x SiO4:Eu2+ have now been known for over four decades and have found extensive recent use in solid-state white lighting. It is well-recognized in the literature and in practice that intermediate compositions in the solid-solutions between the orthosilicates Sr2SiO4 and Ba2SiO4 yield the best phosphor hosts when the thermal stability of luminescence is considered. We employ a combination of synchrotron X-ray diffraction, total scattering measurements, density functional theory calculations, and low-temperature heat capacity measurements, in conjunction with detailed temperature- and time-resolved studies of luminescence properties to understand the origins of the improved luminescence properties. We observe that in the intermediate compositions, the two cation sites in the crystal structure are optimally bonded as determined from bond valence sum calculations. Optimal bonding results in a more rigid lattice, as established by the intermediate compositions possessing the highest Debye temperature, which are determined experimentally from low-temperature heat capacity measurements. Greater rigidity in turn results in the highest luminescence efficiency for intermediate compositions at elevated temperatures.

We study different emission regimes in close-packed films of chemically synthesized CdSe nanoparticles [nanocrystal quantum dots (NQDs)]. We observe that the NQD photoluminescence is dominated by excitons and biexcitons, respectively, before and after the threshold for stimulated emission. Furthermore, we demonstrate the regime of microring lasing into sharp, whispering-gallery modes using NQD solids incorporated into microcapillary tubes. This result indicates a feasibility of miniature, solid-state laser devices based on chemically synthesized NQDs.

A solid solution strategy helps increase the efficiency of Ce3+ oxyfluoride phosphors for solid‐state white lighting. The use of a phosphor‐capping architecture provides additional light extraction. The accompanying image displays electroluminescence spectra from a 434‐nm InGaN LED phosphor that has been capped with the oxyfluoride phosphor.