The design of new functional materials with excellent hydrogen production activity under visible‐light irradiation has critical significance for solving the energy crisis. A well‐controlled synthesis strategy is developed to prepare an Au–Pt–CdS hetero‐nanostructure, in which each component of Au, Pt, and CdS has direct contact with the other two materials; Pt is on the tips and a CdS layer along the sides of an Au nanotriangle (NT), which exhibits excellent photocatalytic activity for hydrogen production under light irradiation (λ > 420 nm). The sequential growth and surfactant‐dependent deposition produce the three‐component Au–Pt–CdS hybrids with the Au NT acting as core while Pt and CdS serve as a co‐shell. Due to the presence of the Au NT cores, the Au–Pt–CdS nanostructures possess highly enhanced light‐harvesting and strong local‐electric‐field enhancement. Moreover, the intimate and multi‐interface contact generates multiple electron‐transfer pathways (Au to CdS, CdS to Pt and Au to Pt) which guide photoexcited electrons to the co‐catalyst Pt for an efficient hydrogen reduction reaction. By evaluating the hydrogen production rate when aqueous Na2SO3–Na2S solution is used as sacrificial agent, the Au–Pt–CdS hybrid exhibits excellent photocatalytic activity that is about 2.5 and 1.4 times larger than those of CdS/Pt and Au@CdS/Pt, respectively.
Localized surface plasmon resonances (LSPRs) of metal nanostructures are highly related to the shape, which could greatly enhance the light−matter interaction at nanoscale. Here, we investigate the LSPRs of gold nanostars corresponding to the unique morphology and demonstrate surface-enhanced Raman scattering (SERS) activities and nonlinear refraction properties of two typical structures. By adjusting the synthesis condition, the main plasmon resonance could be tuned from 557 to 760 nm. The plasmon modes and intense field enhancement near the sharp tips are revealed by finite-difference timed-domain (FDTD) simulations. The nonlinear refractive index |γ| reaches to the maximum value when the excitation wavelength is resonant to the LSPRs wavelength. The maximum value of |γ| for long-branched nanostars (λ SP = 706 nm) is 5.843 × 10 −4 cm 2 / GW, which is about 1.5 times larger than that of spherical-like nanostars with λ SP = 563 nm. The SERS activity of long-branched nanostars is about 15 times larger than that of spherical-like gold nanostars.
The magnetic plasmons of three-dimensional nanostructures have unique optical responses and special significance for optical nanoresonators and nanoantennas. In this study, we have successfully synthesized colloidal Au and AuAg nanocups with a well-controlled asymmetric geometry, tunable opening sizes, and normalized depths (h/ b, where h is depth and b is the height of the templating PbS nanooctahedrons), variable magnetic plasmon resonance, and largely enhanced second-harmonic generation (SHG). The most-efficient SHG of the bare Au nanocups is experimentally observed when the normalized depth h/b is adjusted to ∼0.78−0.79. We find that the average magnetic field enhancement is maximized at h/b = ∼0.65 and reveal that the maximal SHG can be attributed to the joint action of the optimized magnetic plasmon resonance and the "lightning-rod effect" of the Au nanocups. Furthermore, we demonstrate for the first time that the AuAg heteronanocups prepared by overgrowth of Ag on the Au nanocups can synergize the magnetic and electric plasmon resonances for nonlinear enhancement. By the tailoring of the dual resonances at the fundamental excitation and second-harmonic wavelengths, the far-field SHG intensity of the AuAg nanocups is enhanced 21.8fold compared to that of the bare Au nanocups. These findings provide a strategy for the design of nonlinear optical nanoantennas based on magnetic plasmon resonances and can lead to diverse applications ranging from nanophotonics to biological spectroscopy.
The metallic nanostructures with unique properties of tunable plasmon resonance and large field enhancement have been cooperated with semiconductor to construct hetero‐nanostructures for various applications. Herein, a general and facile approach to synthesize uniform dumbbell‐like gold–sulfide core–shell hetero‐nanostructures is reported. The transformation from Au nanorods (NRs) to dumbbell‐like Au NRs and coating of metal sulfide shells (including Bi2S3, CdS, CuxS, and ZnS) are achieved in a one‐pot reaction. Due to the reshaping of Au core and the deposition of sulfide shell, the plasmon resonances of Au NRs are highly enhanced, especially the about 2 times enhancement for the visible transverse plasmon resonance compared with the initial Au NRs. Owing to the highly enhanced visible light absorption and strong local electric field, we find the photocatalytic activity of dumbbell‐like Au–Bi2S3 NRs is largely enhanced compared with pure Bi2S3 and normal Au–Bi2S3 NRs by testing the photodegradation rate of Rhodamine B (RhB). Moreover, the second‐layer sulfide can be coated and the double‐shell Au–Bi2S3–CdS hetero‐nanostructures show further improved photodegradation rate, especially about 2 times than that of Degussa P25 TiO2 (P25) ascribing to the optimum band arrangement and then the prolonged lifetime of photo‐generated carriers.
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