Fano resonance arising from the interaction between a broad "bright" mode and a narrow "dark" mode has been widely investigated in symmetry-breaking structures made of noble metals such as plasmonic asymmetric oligomers or other well-designed nanostructures. However, Fano resonance in nanoscale all-dielectric dimers has not been experimentally demonstrated so far. We report the first experimental observation of directional Fano resonance in silicon nanosphere dimers (both homodimer and heterodimer) and clarify that the coupling between magnetic and electric dipole modes can easily generate Fano resonance in all-dielectric oligomers, distinctly differing from conventional Fano resonances based on electric responses or artificial optical magnetism. A silicon nanosphere dimer, exhibiting a strong magnetic response inside and an electric enhancement in the gap, is an excellent structure to support magnetic-based Fano scattering. Interactions between magnetic and electric dipoles can suppress backward scattering and enhance forward scattering at Fano wavelengths. This directional scattering is much more prominent than that from a single silicon sphere and shows promising applications in areas such as directional nanoantenna or optical switching, opening up avenues for developing all-dielectric low-loss metamaterials or nanophotonic devices at visible wavelengths.
Amorphous materials are usually evaluated as photocatalytically inactive due to the amorphous nature-induced self-trapping of tail states, in spite of their achievements in electrochemistry. NiO crystals fail to act as an individual reactor for photocatalytic H2 evolution because of the intrinsic hole doping, regardless of their impressive cocatalytic ability for proton/electron transfer. Here we demonstrate that two-dimensional amorphous NiO nanostructure can act as an efficient and robust photocatalyst for solar H2 evolution without any cocatalysts. Further, the antenna effect of surface plasmon resonance can be introduced to construct an incorporate antenna-reactor structure by increasing the electron doping. The solar H2 evolution rate is improved by a factor of 19.4 through the surface plasmon resonance-mediated charge releasing. These findings thus open a door to applications of two-dimensional amorphous NiO as an advanced photocatalyst.
α-Ag2WO4 (AWO) has been studied extensively due to its H2 evolution and organic pollution degradation ability under the irradiation of UV light. However, the band gap of AWO is theoretically calculated to be 3.55 eV, resulting in its sluggish reaction to visible light. Herein, we demonstrated that, by using the electronic reconstruction of AWO nanorods upon a unique process of laser irradiation in liquid, these nanorods performed good visible-light photocatalytic organics degradation and H2 evolution. Using commercial AWO powders as the starting materials, we achieved the electronic reconstruction of AWO by a recrystallization of the starting powders upon laser irradiation in liquid and synthesized AWO nanorods. Due to the weak bond energy of AWO and the far from thermodynamic equilibrium process created by laser irradiation in liquid, abundant cluster distortions, especially [WO6] cluster distortions, are introduced into the crystal lattice, the defect density increases by a factor of 2.75, and uneven intermediate energy levels are inset into the band gap, resulting in a 0.44 eV decrease of the band gap, which modified the AWO itself by electronic reconstruction to be sensitive to visible light without the addition of others. Further, the first-principles calculation was carried out to clarify the electronic reconstruction of AWO, and the theoretical results confirmed the deduction based on the experimental measurements.
The reduced TiO 2 -graphene oxide heterostructure as an alternative broad spectrum-driven efficient water splitting photocatalyst has become a really interesting topic, however, its syntheses has many flaws, e.g., tedious experimental steps, time-consuming, small scale production, and requirement of various additives, for example, hydrazine hydrate is widely used as reductant to the reduction of graphene oxide, which is high toxicity and easy to cause the second pollution. For these issues, herein, we reported the synthesis of the reduced TiO 2 -graphene oxide heterostructure by a facile chemical reduction agent-free one-step laser ablation in liquid (LAL) method, which achieves extended optical response range from ultraviolet to visible and composites TiO 2−x (reduced TiO 2 ) nanoparticle and graphene oxide for promoting charge conducting. 30.64% Ti 3+ content in the reduced TiO 2 nanoparticles induces the electronic reconstruction of TiO 2 , which results in 0.87 eV decrease of the band gap for the visible light absorption. TiO 2−x -graphene oxide heterostructure achieved drastically increased photocatalytic H 2 production rate, up to 23 times with respect to the blank experiment. Furthermore, a maximum H 2 production rate was measured to be 16 mmol/h/g using Pt as a cocatalyst under the simulated sunlight irradiation (AM 1.5G, 135 mW/cm 2 ), the quantum efficiencies were measured to be 5.15% for wavelength λ = 365 ± 10 nm and 1.84% for λ = 405 ± 10 nm, and overall solar energy conversion efficiency was measured to be 14.3%. These findings provided new insights into the broad applicability of this methodology for accessing fascinate photocatalysts.
Copper(I) oxide (Cu2O) is an attractive photocatalyst because of its abundance, low toxicity, environmental compatibility, and narrow direct band gap, which allows efficient light harvesting. However, Cu2O exhibits poor photocatalytic performance and photostability because of its short electron diffusion length and low hole mobility. Here, it is demonstrated that nanodiamond (ND) can greatly improve the photocatalytic hydrogen evolution reaction (HER) of the p‐type photocatalyst Cu2O nanocrystals by nanocomposition. Compared with pure Cu2O nanocrystals, this composite shows a tremendous improvement in HER performance and photostability. HER rates of 100.0 mg NDs‐Cu2O nanocrystals are 1597 μmol normalh−1 normalg−1 and 824 μmol normalh−1 normalg−1 under the simulated solar light irradiation (AM 1.5, 100 mW cm−2) and visible light irradiation (420–760 nm, 77.5 mW cm−2), respectively. The solar‐to‐hydrogen conversion efficiency of this composite is 0.85%, which is nearly ten times higher than that of pure Cu2O. The quantum efficiency of the composite is high, with values of 0.17% at λ = 780 nm and 0.23% at λ = 850 nm. The broad spectral response of ND provides numerous carriers for the subsequent reactions. The electron‐donating ability of ND and suitable band structures of the two components promote electron injection from ND to Cu2O. These results suggest the broad applicability of ND to ameliorate the photoelectric properties of semiconductors.
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