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 controllable synthesis of uniform tungsten diselenide (WSe ) is crucial for its emerging applications due to the high sensitivity of its extraordinary physicochemical properties to its layer numbers. However, undesirable multilayer regions inevitably form during the fabrication of WSe via the traditional chemical vapor deposition process resulted from the lack of significantly energetically favorable competition between layer accumulation and size expansion. This work innovatively introduces Cu to occupy the hexagonal site positioned at the center of the six membered ring of the WSe surface, thus filtrates the undesired reaction path through precisely thermodynamical control and achieves self-limited growth WSe crystals. The as-obtained WSe crystals are characterized as strictly single-layer over the entire wafer. Furthermore, the strictly self-limited growth behavior can achieve the "win-win" cooperation with the synthesis efficiency. The fastest growth (≈15 times of the growth rate in the previous work) of strictly monolayer WSe crystals thus far is realized due to the high-efficiency simultaneous selenization process. The as-proposed ultrafast Cu-assisted self-limited growth method opens a new avenue to fabricate strictly monolayer transition metal dichalcogenides crystals and further promotes their practical applications in the future industrial applications.
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.
Recent studies of the coupling between the plasmonic excitations of metallic nanostructures with the excitonic excitations of molecular species have revealed a rich variety of emergent phenomena known as plexcitonics. Here, we use a combined experimental and theoretical approach to demonstrate new and intriguing aspects in the ultrafast nonlinear responses of strongly coupled hybrid Fano systems consisting of gold nanorods decorated with near-infrared dye molecules. We show that the severely suppressed linear absorption around the Fano dip significantly enhances the unidirectional energy transfer from the plasmons to the excitons and further allows one-photon nonlinearity to be drastically and reversibly tuned. These striking observations are interpreted within a microscopic model stressing on two competing processes: saturated plasmonic absorption and weakened destructive Fano interference from the bleached excitonic absorption. The unusually strong one-photon nonlinearity revealed here provides a promising strategy in fabricating nanoplasmonic devices with both pronounced nonlinearities and good figures of merit.
Dissipative self‐assembly of colloidal nanoparticles offers the prospect of creating reconfigurable artificial materials and systems, yet the phenomenon only occurs far from thermodynamic equilibrium. Therefore, it is usually difficult to predict and control. Here, a dissipative colloidal solution system, where anisotropic chains with different interparticle separations in two perpendicular directions transiently arise among largely disordered silver nanoparticles illuminated by a laser beam, is reported. The optical field creates a nonequilibrium dissipative state, where a disorder‐to‐order transition occurs driven by anisotropic electrodynamic interactions coupled with electrostatic interactions. Investigation of the temporal dynamics and spatial arrangements of the nanoparticle system shows that the optical binding strength and entropy of the system are two crucial parameters for the formation of the anisotropic chains and responsible for adaptive behaviors, such as self‐replication of dimer units. Formation of anisotropic nanoparticle chains is also observed among colloidal nanoparticles made from other metal (e.g., Au), polymer (e.g., polystyrene), ceramic (e.g., CeO2), and hybrid materials (e.g., SiO2@Au core–shell), suggesting that light‐driven self‐organization will provide a wide range of opportunities to discover new dissipative structures under thermal fluctuations and build novel anisotropic materials with nanoscale order.
We report the synthesis of 43-nm diameter Au nanocube dimers by using Ag(+) ions as competitive ligands to freeze L-cysteine-induced assembly process of the nanocubes to a desirable stage. Ascribed to the resonant interparticle coupling with an newly arising plasmon band at 710 nm and local field enhancement, the two-photon luminescence intensity of the Au nanocube dimers in solution was over 20 times stronger than that of the monomers in the wavelength range 555-620 nm. Furthermore, by coupling Raman tags onto the nanocube surface, a solution-based surface-enhanced Raman scattering (SERS) of the nanocube dimers had an enhancement factor of over 10 times compared to the isolated nanocubes. To sum up, with high stability in solution and attractive optical properties, the Au nanocube dimers have potential applications in in vivo bio-imaging and solution-based SERS.
Precise sorting of colloidal nanoparticles is a challenging yet necessary task for size-specific applications of nanoparticles in nanophotonics and biochemistry. Here we present a new strategy for all-optical sorting of metal nanoparticles with dynamic and tunable optical driven forces generated by phase gradients of light. Size-dependent optical forces arising from the phase gradients of optical line traps can drive nanoparticles of different sizes with different velocities in solution, leading to their separation along the line traps. By using a sequential combination of optical lines to create differential trapping potentials, we realize precise sorting of silver and gold nanoparticles in the diameter range of 70-150 nm with a resolution down to 10 nm. Separation of the nanoparticles agrees with the analysis of optical forces acting on them and with simulations of their kinetic motions. The results provide new insights into all-optical nanoparticle manipulation and separation and reveal that there is still room to sort smaller nanoparticle with nanometer precision using dynamic phase-gradient forces.
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