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Plasmonic nanostructures have a capability to control the photoluminescence (PL) emission properties of optical species and thus can dramatically enhance the performances of diverse optical systems and devices. Lanthanide ions typically exhibit multiple PL emission lines. Systematic studies on the plasmon-enabled selective enhancement for the different emission lines of lanthanide ions are still highly desired in order to achieve the fine manipulation on the spectral profile and luminescence intensity ratio (LIR). Herein we report on the synthesis and PL emission properties of monodisperse spherical (Au core)@(Y(V,P)O4:Eu) nanostructures, which integrate the plasmonic and luminescent units into an individual core@shell structure. The localized surface plasmon resonance adjusted through control of the size of the Au nanosphere core enables the systematic modulation of the selective emission enhancement of Eu3+. As revealed by single-particle scattering and PL measurements, the five luminescence emission lines of Eu3+originating from the 5D0,1excitation states are affected by the localized plasmon resonance to different extents, which are dependent on both the dipole transition nature and the intrinsic quantum yield of the emission line. Based on the plasmon-enabled tunable LIR, high-level anticounterfeiting and optical temperature measurements for photothermal conversion are further demonstrated. Our architecture design and PL emission tuning results offer many possibilities for constructing multifunctional optical materials by integrating plasmonic and luminescent building blocks into hybrid nanostructures with different configurations.

Excitons in a transition-metal dichalcogenide (TMDC) monolayer can be modulated through strain with spatial and spectral control, which offers opportunities for constructing quantum emitters for applications in on-chip quantum communication and information processing. Strain-localized excitons in TMDC monolayers have so far mainly been observed under cryogenic conditions because of their subwavelength emission area, low quantum yield, and thermal-fluctuation-induced delocalization. Herein, we demonstrate both generation and detection of strain-localized excitons in WS2monolayer through a simple plasmonic structure design, where WS2monolayer covers individual Au nanodisks or nanorods. Enhanced emission from the strain-localized excitons of the deformed WS2monolayer near the plasmonic hotspots is observed at room temperature with a photoluminescence energy redshift up to 200 meV. The emission intensity and peak energy of the strain-localized excitons can be adjusted by the nanodisk size. Furthermore, the excitation and emission polarization of the strain-localized excitons are modulated by anisotropic Au nanorods. Our results provide a promising strategy for constructing nonclassical integrated light sources, high-sensitivity strain sensors, or tunable nanolasers for future dense nanophotonic integrated circuits.

Optical excitation, subsequent energy transfer, and emission are fundamental to many physical problems. Optical antennas are ideal candidates for manipulating these processes. We extend energy transfer to second- and third-harmonic (SH and TH) fields through the collaborative susceptibility χ(n)(n= 1, 2, 3) resonances of nonlinear optical antennas. Hollow gold stars, with a broadband response covering the fundamental, SH, and TH frequencies, are synthesized as nonlinear antennas. Harmonic resonance energy transfer through a χ(3)→ χ(1)collaboration is revealed. A χ(3)→ χ(2)collaboration is uncovered, with largely enhanced SH radiation demonstrated by exciting the three resonances at the fundamental, SH, and TH frequencies. A theoretical model of the effective nonlinear susceptibilities is proposed to calculate the efficiencies of the two nonlinear energy transfer processes.

Photocatalytic H2O2production has attracted much attention as an alternative way to the industrial anthraquinone oxidation process but is limited by the weak interaction between the catalysts and reactants as well as inefficient proton transfer. Herein, we report on a hydrogen-bond-broken strategy in carbon nitride for the enhancement of H2O2photosynthesis without any sacrificial agent. The H2O2photosynthesis is promoted by the hydrogen bond formation between the exposed N atoms on hydrogen-bond-broken carbon nitride and H2O molecules, which enhances proton-coupled electron transfer and therefore the photocatalytic activity. The exposed N atoms serve as proton buffering sites for the proton transfer from H2O molecules to carbon nitride. The H2O2photosynthesis is also enhanced through the enhanced adsorption and reduction of O2gas toward H2O2on hydrogen-bond-broken carbon nitride because of the formation of nitrogen vacancies (NVs) and cyano groups after the intralayer hydrogen bond breaking on carbon nitride. A high light-to-chemical conversion efficiency (LCCE) value of 3.85% is achieved. O2and H2O molecules are found to undergo a one-step two-electron reduction pathway by photogenerated hot electrons and a four-electron oxidation process to produce O2gas, respectively. Density functional theory (DFT) calculations validate the O2adsorption and reaction pathways. This study elucidates the significance of the hydrogen bond formation between the catalyst and reactants, which greatly increases the proton tunneling dynamics.

The integration of two-dimensional transition metal dichalcogenides with plasmonic nanostructures is extremely attractive for the investigation of the resonance coupling between plasmons and excitons, which offers a framework for the study of cavity quantum electrodynamics and is of great potential for exploring diverse quantum technologies. Herein we report on the coupling between the magnetic plasmons supported by individual asymmetric Au nanocups and the excitons in WS2monolayer and multilayer. Resonance coupling with the strength varying from weak to strong regimes is realized by adjusting the orientation of the individual Au nanocups on WS2monolayer. Different energy detunings between the magnetic plasmons and the excitons are achieved by varying the size of the Au nanocup. The Rabi splitting energies extracted at zero detuning are up to 106 meV. The anticrossing feature is observed in the measured scattering spectra and simulated absorption spectra, which indicates that the resonance coupling between the magnetic plasmons in the Au nanocup and the excitons in WS2monolayer enters the strongly coupled regime. A dependence of the coupling strength on the layer number is further observed when the Au nanocups are coupled with WS2multilayer. Our study suggests a promising approach toward the realization of different coupling regimes in a simple hybrid system made of individual Au nanocups and two-dimensional materials.

Gold nanocubes demonstrate unique optical properties of the high photoluminescence (PL) quantum yield and a remarkably enhanced extinction band at 544 nm. The 4 × 10−2PL yield, which is about 200 times higher than that of gold nanorods, allows gold nanocubes to be successfully used in cell imaging of human liver cancer cells (QGY) and human embryo kidney cells (293T) with a common method of single-photon excitation. The high extinction coefficients of gold nanocubes also facilitate them carrying out the photothermal therapy of QGY and 293T cells, showing similar photokilling efficiency as compared to gold nanorods.

A high-quality plasmon–fiber cavity in a doubly resonant configuration can exhibit second-harmonic generation (SHG) with over 5 orders of magnitude enhancement compared to gold nanoparticles on a fused silica substrate. Through coupling to a fiber cavity with the proper diameter, a high-quality (Q≈ 160) resonance can be achieved in combination with a single gold nanoparticle. In a classical picture, where the incident electric field travels coherently Qtimes around the fiber during the nonlinear process, the high Qof the coupled mode aids in highly efficient SHG. We accomplish two feats: First, we analyze the Qfactor dependence of the SHG efficiency, proving the expected Q4dependence and thus confirming coherent E-field amplification in the fiber cavity. Second, we carefully adjust the fiber size further and tune the plasmon response of a gold nanoparticle to a high-Qcavity mode. We make sure that the second harmonic wavelength is simultaneously in resonance with a higher order fiber cavity mode, fulfilling the doubly resonantcondition. As a result, a giant SH response with conversion efficiency up to 1.6 × 10–5is detected upon a pump intensity of 5 × 108W/cm2for 100 fs pump pulses around 840 nm incident wavelength. Additionally, the importance of the doubly resonant condition is proven by detuning the size of the fiber, which leads to a drastic drop in SHG efficiency. This disparity of the SHG efficiency can be observed even by eye, when monitoring the intensity changes of the visible SH light during detuning.