Hot-electron-induced photodissociation of H2 was demonstrated on small Au nanoparticles (AuNPs) supported on SiO2. The rate of dissociation of H2 was found to be almost 2 orders of magnitude higher than that observed on equivalently prepared AuNPs on TiO2. The rate of H2 dissociation was found to be linearly dependent on illumination intensity with a wavelength dependence resembling the absorption spectrum of the plasmon of the AuNPs. This result provides strong additional support for the hot-electron-induced mechanism for H2 dissociation in this photocatalytic system.
Aqueous solutions containing light-absorbing nanoparticles have recently been shown to produce steam at high efficiencies upon solar illumination, even when the temperature of the bulk fluid volume remains far below its boiling point. Here we show that this phenomenon is due to a collective effect mediated by multiple light scattering from the dispersed nanoparticles. Randomly positioned nanoparticles that both scatter and absorb light are able to concentrate light energy into mesoscale volumes near the illuminated surface of the liquid. The resulting light absorption creates intense localized heating and efficient vaporization of the surrounding liquid. Light trapping-induced localized heating provides the mechanism for low-temperature light-induced steam generation and is consistent with classical heat transfer.
Au nanoparticles with plasmon resonances in the near-infrared (NIR) region of the spectrum efficiently convert light into heat, a property useful for the photothermal ablation of cancerous tumors subsequent to nanoparticle uptake at the tumor site. A critical aspect of this process is nanoparticle size, which influences both tumor uptake and photothermal efficiency. Here, we report a direct comparative study of ∼90 nm diameter Au nanomatryoshkas (Au/SiO2/Au) and ∼150 nm diameter Au nanoshells for photothermal therapeutic efficacy in highly aggressive triple negative breast cancer (TNBC) tumors in mice. Au nanomatryoshkas are strong light absorbers with 77% absorption efficiency, while the nanoshells are weaker absorbers with only 15% absorption efficiency. After an intravenous injection of Au nanomatryoshkas followed by a single NIR laser dose of 2 W/cm2 for 5 min, 83% of the TNBC tumor-bearing mice appeared healthy and tumor free >60 days later, while only 33% of mice treated with nanoshells survived the same period. The smaller size and larger absorption cross section of Au nanomatryoshkas combine to make this nanoparticle more effective than Au nanoshells for photothermal cancer therapy.
Plasmonic nanostructures enable the generation of large electromagnetic fields confined to small volumes, potentially providing a route for the development of nanoengineered nonlinear optical media. A metal-capped hemispherical nanoparticle, also known as a nanocup, generates second harmonic light with increasing intensity as the angle between the incident fundamental beam and the nanocup symmetry axis is increased. Nanoparticle orientation also modifies the emission direction of the second harmonic light. With conversion efficiencies similar to those of inorganic SHG crystals, these structures provide a promising approach for the design and fabrication of stable, synthetic second-order nonlinear optical materials tailored for specific wavelengths.
Monolayer molybdenum disulfide (MoS 2) produced by controlled vapor-phase synthesis is a commercially promising new two-dimensional material for optoelectronics because of its direct bandgap and broad absorption in the visible and ultraviolet regimes. By tuning plasmonic core-shell nanoparticles to the direct bandgap of monolayer MoS 2 and depositing them sparsely (<1% coverage) onto the material's surface, we observe a threefold increase in photocurrent and a doubling of photoluminescence signal for both excitonic transitions, amplifying but not altering the intrinsic spectral response. V
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