Revealing the Optical Transition Properties of Interlayer Excitons in Defective WS2/WSe2 Heterobilayers.

Manipulation of physical properties in multidimensional tunable moiré superlattice systems is a key focus in nanophotonics, especially for interlayer excitons (IXs) in two-dimensional materials. However, the impact of defects on IXs remains unclear. Here, we thoroughly study the optical properties of WS2/WSe2 heterobilayers with varying defect densities. Low-temperature photoluminescence (PL) characterizations reveal that the low-energy IXs are more susceptible to defects compared to the high-energy IXs. The low-energy IXs also show much faster PL quenching rate with temperature, faster peak width broadening rate with laser power, shorter lifetime, and lower circular polarization compared to the low-energy IXs in the region with fewer defects. These effects are attributed to the combined effects of increased electron scattering, exciton-phonon interactions, and nonradiative channels introduced by the defects. Our findings aid in optimizing moiré superlattice structures.

Enhancing Light Out-coupling in Perovskite Light-Emitting Diodes through Plasmonic Nanostructures.

Perovskite light-emitting diodes (PeLEDs) have emerged as promising candidates for lighting and display technologies owing to their high photoluminescence quantum efficiency and high carrier mobility. However, the performance of planar PeLEDs is limited by the out-coupling efficiency, predominantly governed by photonic losses at device interfaces. Most notably, the plasmonic loss at the metal electrode interfaces can account for up to 60% of the total loss. Here, we investigate the use of plasmonic nanostructures to improve the light out-coupling in PeLEDs. By integrating these nanostructures with PeLEDs, we have demonstrated an effectively reduced plasmonic loss and enhanced light out-coupling. As a result, the nanostructured PeLEDs exhibit an average 1.5-fold increase in external quantum efficiency and an ∼20-fold improvement in device lifetime. This finding offers a generic approach for enhancing light out-coupling, promising great potential to go beyond existing performance limitations.

Identifying high-order plasmon modes in silver nanoparticle-over-mirror configuration.

Metallic nanoparticle-over-mirror (NPOM) represents as a versatile plasmonic configuration for surface enhanced spectroscopy, sensing and light-emitting metasurfaces. However, experimentally identifying the high-order localized surface plasmon modes in NPOM, especially for the best plasmonic material silver, is often hindered by the small scattering cross-section of high-order plasmon modes and the poor reproducibility of the spectra across different NPOMs, resulted from the polyhedral morphology of the colloidal nanoparticles or the rough surface of deposited polycrystalline metals. In this study, we identify the high-order localized surface plasmon modes in silver NPOM by using differential reflection spectroscopy. We achieved reproducible single-particle absorption spectra by constructing uniform NPOM consisting of silver nanospheres, single-crystallized silver microplates, and a self-assembled monolayer of 1,10-decanedithiol. For comparison, silver NPOM created from typical polycrystalline films exhibits significant spectral fluctuations, even when employing template stripping methods to minimize the film roughness. Identifying high-order plasmon modes in the NPOM configuration offers a pathway to construct high-quality plasmonic substrates for applications such as colloidal metasurface, surface-enhanced Raman spectroscopy, fluorescence, or infrared absorption.

Extraordinary Five-Wave Mixing in a Zinc Oxide Microwire on a Au Film.

Coherent multiwave mixing is in demand for optical frequency conversion, imaging, quantum information science, etc., but has rarely been demonstrated in solid-state systems. Here, we observed three- and five-wave mixing (5WM) in a c-axis growth zinc oxide microwire on a Au film with picosecond pulses in the near-infrared region. An output 5WM of 4.7 × 10-7 µW, only 2-3 orders smaller than the three-wave mixing, is achieved when the excitation power is as low as 1.5 mW and the peak power density as weak as ∼107 W/cm2. The excitation power dependence of 5WM agrees well with the perturbation limit under the low intensity but exhibits a strong deviation at a high pumping power. This extraordinary behavior is attributed to the cooperative resonant enhancement effect when pumping in the near-infrared range. Our study offers a potential solid-state platform for on-chip multiwave mixing and quantum nonlinear optics, such as generating many-photon entangled states or the construction of photon-photon quantum logic gates.

How to Obtain the Correct Rabi Splitting in a Subwavelength Interacting System.

We unambiguously extract the individual decay channels of a coupled plasmon-exciton system by using correlated single-particle absorption and scattering measurements. A remarkable difference in the two channels is present─clear Rabi splitting in the plasmon channel but no Rabi splitting in the exciton channel. Discordance in the absorption and scattering spectra are mainly originated from the distinct contributions of plasmon and exciton channels in the absorption and scattering process. Our findings provide insights into plasmon-exciton interaction in an open cavity and can impact the design of plexcitonic devices for ultrafast nonlinear nanophotonics.

Self-Modulation-Guided Growth of 2D Tellurides with Ultralow Thermal Conductivity.

Ultralow thermal conductivity materials have triggered much interest due to diverse applications in thermal insulation, thermal barrier coating, and especially thermoelectrics. Two dimensional (2D) indium tellurides with ultralow thermal conductivity provide a versatile platform for tailoring the heat transfer, exploring new candidates for thermoelectrics, and achieving miniature, lightweight, and highly integrated devices. Unfortunately, their nanostructure and structure-related heat transfer properties at a 2D scale are much less studied due to difficulties in material fabrication. The ionic character between interlayers and strong covalent bonds in 3D directions impede the anisotropic growth of indium telluride flakes; meanwhile, the low environmental stability and chemical reactivity of tellurium also limit the fabrication of high-quality tellurides, thus hindering the exploration of thermal transport properties. Here, a self-modulation-guided growth strategy to synthesize high-quality 2D In4 Te3 single crystals with ultralow thermal conductivity (0.47 W m-1  K-1 ) is developed. This strategy can also be extended to synthesize a series of highly crystallized metal tellurides, providing excellent candidates for further application in thermoelectrics.

Merging Bound States in the Continuum at Off-High Symmetry Points.

Bound states in the continuum (BICs) confine resonances embedded in a continuous spectrum by eliminating radiation loss. Merging multiple BICs provides a promising approach to further reduce the scattering losses caused by fabrication imperfections. However, to date, BIC merging has been limited to only the Γ point, which constrains potential application scenarios such as beam steering and directional vector beams. Here, we propose a new scheme to construct merging BICs at almost an arbitrary point in reciprocal space. Our approach utilizes the topological features of BICs on photonic crystal slabs, and we merge a Friedrich-Wintgen BIC and an accidental BIC. The Q factors of the resulting merging BIC are enhanced for a broad wave vector range compared with both the original Friedrich-Wintgen BIC and the accidental BIC. Since Friedrich-Wintgen BICs and accidental BICs are quite common in the band structure, our proposal provides a general approach to realize off-Γ merging BICs with superhigh Q factors that can substantially enhance nonlinear and quantum effects and boost the performance of on-chip photonic devices.

Unified treatment of scattering, absorption, and luminescence spectra from a plasmon-exciton hybrid by temporal coupled-mode theory.

Plasmonic nanostructures are capable of tailoring the emission of a nearby emitter by increasing (or reducing) the brightness, shortening (or prolonging) the lifetime, and shaping the spectrum. Experimental characterization of such coupled plasmon-exciton (plexciton) systems usually relies on the acquisition and comparison of scattering, absorption, or luminescence spectra. However, theoretical accounts of these optical spectra, which are key to distinguishing between the coupling regimes and to standardizing the coupling criteria, often scatters in different frameworks, varying from classical to quantum-mechanical. Therefore, developing a unified and simple formalism that can simultaneously compare all these spectral signatures in different coupling regimes is nontrivial. Here, we use a temporal coupled-mode formalism to reproduce the scattering, absorption, and luminescence spectra of a plexciton system and find that its luminescence reaches a maximum at a critical coupling point, featuring a light-emitting plexciton with intense brightness and ultrafast lifetime. This simple approach provides a unified and phenomenological treatment of these spectra by simply including or excluding an external driving term. It therefore allows for a direct comparison of different spectroscopic signatures from the plexciton system and provides an easy-to-use guidance for the design of broadband light-emitting devices.

ZnO@ZIF-8 Core-Shell Structure Gas Sensors with Excellent Selectivity to H2.

As the energy crisis becomes worse, hydrogen as a clean energy source is more and more widely used in industrial production and people's daily life. However, there are hidden dangers in hydrogen storage and transportation, because of its flammable and explosive features. Gas detection is the key to solving this problem. High quality sensors with more practical and commercial value must be able to accurately detect target gases in the environment. Emerging porous metal-organic framework (MOF) materials can effectively improve the selectivity of sensors as a result of high surface area and coordinated pore structure. The application of MOFs for surface modification to improve the selectivity and sensitivity of metal oxides sensors to hydrogen has been widely investigated. However, the influence of MOF modified film thickness on the selectivity of hydrogen sensors is seldom studied. Moreover, the mechanism of the selectivity improvement of the sensors with MOF modified film is still unclear. In this paper, we prepared nano-sized ZnO particles by a homogeneous precipitation method. ZnO nanoparticle (NP) gas sensors were prepared by screen printing technology. Then a dense ZIF-8 film was grown on the surface of the gas sensor by hydrothermal synthesis. The morphology, the composition of the elements and the characters of the product were analyzed by X-ray diffraction analysis (XRD), transmission electron microscope (TEM), scanning electron microscope (SEM), energy dispersive spectrometer (EDS), Brunauer-Emmett-Teller (BET) and differential scanning calorimetry (DSC). It is found that the ZIF-8 film grown for 4 h cannot form a dense core-shell structure. The thickness of ZIF-8 reaches 130 nm at 20 h. Through the detection and analysis of hydrogen (1000 ppm), ethanol (100 ppm) and acetone (50 ppm) from 150 °C to 290 °C, it is found that the response of the ZnO@ZIF-8 sensors to hydrogen has been significantly improved, while the response to ethanol and acetone was decreased. By comparing the change of the response coefficient, when the thickness of ZIF-8 is 130 nm, the gas sensor has a significantly improved selectivity to hydrogen at 230 °C. The continuous increase of the thickness tends to inhibit selectivity. The mechanism of selectivity improvement of the sensors with different thickness of the ZIF-8 films is discussed.

Enhancing Formaldehyde Selectivity of SnO2 Gas Sensors with the ZSM-5 Modified Layers.

High performance formaldehyde gas sensors are widely needed for indoor air quality monitoring. A modified layer of zeolite on the surface of metal oxide semiconductors results in selectivity improvement to formaldehyde as gas sensors. However, there is insufficient knowledge on how the thickness of the zeolite layer affects the gas sensing properties. In this paper, ZSM-5 zeolite films were coated on the surface of the SnO2 gas sensors by the screen printing method. The thickness of ZSM-5 zeolite films was controlled by adjusting the numbers of screen printing layers. The influence of ZSM-5 film thickness on the performance of ZSM-5/SnO2 gas sensors was studied. The results showed that the ZSM-5/SnO2 gas sensors with a thickness of 19.5 µm greatly improved the selectivity to formaldehyde, and reduced the response to ethanol, acetone and benzene at 350 °C. The mechanism of the selectivity improvement to formaldehyde of the sensors was discussed.

Selectively Depopulating Valley-Polarized Excitons in Monolayer MoS2 by Local Chirality in Single Plasmonic Nanocavity.

Transition metal dichalcogenides, whose valley degrees of freedom are characterized by the degree of circular polarization (DCP) of the photoluminescence, draw broad interests due to their potential applications in information storage and processing. However, this DCP is usually low at room temperature due to the phonon-assisted intervalley scattering, severely degrading the fidelity of the valley-stored signals. Therefore, achieving high DCP at room temperature is vital for valley-encoded nanophotonic devices. In this work, we demonstrate a high DCP of 48.7% at room temperature by embedding monolayer MoS2 into a compact plasmonic nanocavity. Such a high DCP is proven to originate from the prominent chiral Purcell effect owing to the degeneracy-lifted circularly polarized local density of states in the nanocavity. In addition, the DCP can be further manipulated by an in situ plasmon-scanned technique. This highly compact system provides possibilities for developing versatile valley-encoded light-emitting devices at room temperature.

Efficient Frequency Mixing of Guided Surface Waves by Atomically Thin Nonlinear Crystals.

Monolayer transition metal dichalcogenides possess considerable second-order nonlinear coefficients but a limited efficiency of frequency conversion due to the short interaction length with light under the typical direct illumination. Here, we demonstrate an efficient frequency mixing of the guided surface waves on a monolayer tungsten disulfide (WS2) by simultaneously lifting the temporal and spatial overlap of the guided wave and the nonlinear crystal. Three orders-of-magnitude enhancement of the conversion efficiency was achieved in the counter-propagating excitation configuration. Also, the frequency-mixing signals are highly collimated, with the emission direction and polarization controlled, respectively, by the pump frequencies and the rotation angle of WS2 relative to the propagation direction of the guided waves. These results indicate that the rules of nonlinear frequency conversion are applicable even when the crystal is scaled down to the ultimate single-layer limit. This study provides a versatile platform to enhance the nonlinear optical response of 2D materials and favor the scalable generation of a coherent light source and entangled photon pairs.

Duplicating Plasmonic Hotspots by Matched Nanoantenna Pairs for Remote Nanogap Enhanced Spectroscopy.

Plasmonic nanoantennas are capable of reversibly interconverting free-space radiation with localized modes at the nanoscale. However, optical access to a single nanoantenna, through a laser beam, is always accompanied by disruptive background perturbations and heating effects. Remote spectroscopy is one promising route to overcome these effects. Here, we demonstrate excitation-collection-separated enhanced spectroscopy using a matched nanoantenna pair. The receiving and transmitting antennas are geometrically separated but bridged by the propagating surface plasmon polaritons (SPPs) on the metal film. The receiving antenna, consisting of a silver nanowire on a mirror, ensures a high light-to-plasmon conversion efficiency. The transmitting antenna consists of a silver nanocube over a mirror and is impedance matched to free space photons and the propagating SPPs. As a proof-of-principle, we demonstrate remote surface-enhanced Raman scattering with a high signal-to-noise ratio. This matched nanoantenna pair may have applications for remote entanglement of quantum emitters, biochemistry detection, or optical interconnects.

Plasmon Waveguiding in Nanowires.

Nanowires supporting propagating surface plasmons can function as nanowaveguides to realize the light guiding with field confinement beyond the diffraction limit, providing fundamental building blocks for nanophotonic integrated circuits. This review covers the recent developments of plasmon waveguiding in nanowires, mainly including plasmon waveguiding in metal nanowires, coupling of nanowire plasmons and emitters, hybrid nanowire waveguides and plasmonic gain, and nanowire photonic devices. We first introduce the main techniques for fabricating metal nanowires, the plasmon modes in metal nanowires and the excitation/detection methods. We then discuss the fundamental properties of plasmon propagation and emission, including zigzag, chiral and spin-dependent propagation, mode conversion, loss and propagation length, group velocity, terminal emission, and leaky radiation. Then the interactions between nanowires and emitters are reviewed, especially the coupling of single nanowires and single quantum emitters. Finally, we briefly introduce the hybrid nanowire waveguide composed of a semiconductor nanowire and a metal film with an intervening thin insulator and highlight a few nanophotonic devices based on plasmonic nanowire networks or plasmonic-photonic hybrid nanowire structures.

Simultaneous Surface-Enhanced Resonant Raman and Fluorescence Spectroscopy of Monolayer MoSe2: Determination of Ultrafast Decay Rates in Nanometer Dimension.

The fact that metallic nanostructures are an excellent light receiver and transmitter connects the underlying principles of two widely applied optical processes: surface-enhanced Raman scattering (SERS) and surface-enhanced fluorescence (SEF). A comparative study of SERS and SEF can eliminate the typical unknown quantities of the system and reveal important parameters that cannot be accessed by conventional techniques. Here, we use this simultaneous SERS and SEF technique in a monolayer MoSe2 coupled plasmonic nanocavity. After optimizing the spatial and the spectral overlaps between excitonic and plasmonic resonances, the SERS and SEF enhancement factors can exceed 107 and 6000, respectively, at the same time on the same nanocube. The comparison of the SERS and SEF enhancements allows the estimation of the ultrafast total decay rate of the bright exciton in monolayer MoSe2 in the nanocavity down to tens of femtoseconds, which is otherwise hard to realize using time-resolved techniques.

Efficient Second Harmonic Generation in a Hybrid Plasmonic Waveguide by Mode Interactions.

Developing highly efficient nanoscale coherent light sources is essential for advances in technological applications such as integrated photonic circuits, bioimaging, and sensing. An on-chip wavelength convertor based on second harmonic generation (SHG) would be a crucial step toward this goal, but the light-conversion efficiency would be low for small device dimensions. Here we demonstrate strongly enhanced SHG with a high conversion efficiency of 4 × 10-5 W-1 from a hybrid plasmonic waveguide consisting of a CdSe nanowire coupled with a Au film. The strong spatial overlap of the waveguide mode with the nonlinear material and momentum conservation between the incident and reflected modes are the key factors resulting in such high efficiency. The SHG emission angles vary linearly with excitation wavelength, indicating a nonlinear steering of coherent light emission at the subwavelength scale. Our work is promising for the realization of efficient and tunable nonlinear coherent sources and opens new approaches for efficient integrated nonlinear nanophotonic devices.

Routing a Chiral Raman Signal Based on Spin-Orbit Interaction of Light.

Spontaneous Raman scattering is a second-order perturbation process with two photons linking the internal structures of the matter. The frequency-shifted Raman peaks are sharp and carry rich information about the internal structures. However, encoding and manipulating this information have been barely explored up to now. Here, we report the high-fidelity routing of a chiral Raman signal into propagating surface plasmon polaritons along a silver nanowire based on spin-orbit interaction of light. A directionality up to 91.5±0.5% is achieved and can be quantitatively controlled by tuning the polarization of the incident laser and the position of excitation. The deterministic routing of the Raman signal is sensitively dependent on the local spin density of the plasmon field and the polarization of the Raman modes. This study extends the spin-orbit interaction of light to the Raman scattering regime and proposes a new perspective for the remote readout of local optical chirality, helicity-related directional sorting, and quantum information processing.

The Enhanced H2 Selectivity of SnO2 Gas Sensors with the Deposited SiO2 Filters on Surface of the Sensors.

This paper reports a study on the enhanced H2 selectivity of SnO2 gas sensors with SiO2 on the surface of the sensors obtained via chemical vapor deposition using dirthoxydimethylsilane as the Si source. The gas sensors were tested for sensing performance towards ethanol, acetone, benzene, and hydrogen at operating temperatures from 150 °C to 400 °C. Our experimental results show that higher selectivity and responses to hydrogen were achieved by the deposition of SiO2 on the surface of the sensors. The sensor with SiO2 deposited on its surface at 500 °C for 8 h exhibited the highest response (Ra/Rg = 144) to 1000 ppm hydrogen at 350 °C, and the sensor with SiO2 deposited on its surface at 600 °C for 4 h attained the maximum response variation coefficient (D = 69.4) to 1000 ppm hydrogen at 200 °C. The mechanism underlying the improvement in sensitivity and the higher responses to hydrogen in the sensors with SiO2 on their surface is also discussed.

Transversely Divergent Second Harmonic Generation by Surface Plasmon Polaritons on Single Metallic Nanowires.

Coherently adding up signal wave from different locations are a prerequisite for realizing efficient nonlinear optical processes in traditional optical configurations. While nonlinear optical processes in plasmonic waveguides with subwavelength light confinement are in principle desirable for enhancing nonlinear effects, so far it has been difficult to improve the efficiency due to the large momentum mismatch. Here we demonstrate, using remotely excited surface plasmon polaritons (SPPs), axial collimated but transversely divergent second harmonic (SH) generation in a single silver nanowire-monolayer molybdenum disulfide hybrid system. Fourier imaging of the generated SH signal confirms the momentum conservation conditions between the incident and reflected SPPs and reveals distinct features inherent to the 1D plasmonic waveguides: (i) the SH photons are collimated perpendicular to the nanowire axis but are divergent within the perpendicular plane; (ii) the collimation (divergence) is inversely proportional to the length of the active region (lateral confinement of the SPPs); and (iii) the SH emission pattern resembles that of an aligned dipole chain on top of the substrate with an emission peak at the critical angle. Our results pave the way to generate and manipulate SH emission around subwavelength waveguides and open up new possibilities for realizing high efficiency on-chip nonlinear optics.

Manipulating Coherent Plasmon-Exciton Interaction in a Single Silver Nanorod on Monolayer WSe2.

Strong coupling between plasmons and excitons in nanocavities can result in the formation of hybrid plexcitonic states. Understanding the dispersion relation of plexcitons is important both for fundamental quantum science and for applications including optoelectronics and nonlinear optics devices. The conventional approach, based on statistics over different nanocavities, suffers from large inhomogeneities from the samples, owing to the nonuniformity of nanocavities and the lack of control over the locations and orientations of the excitons. Here we report the first measurement of the dispersion relationship of plexcitons in an individual nanocavity. Using a single silver nanorod as a Fabry-Pérot nanocavity, we realize strong coupling of plasmon in single nanocavity with excitons in a single atomic layer of tungsten diselenide. The plexciton dispersion is measured by in situ redshifting the plasmon energy via successive deposition of a dielectric layer. Room-temperature formation of plexcitons with Rabi splittings as large as 49.5 meV is observed. The realization of strong plasmon-exciton coupling by in situ tuning of the plasmon provides a novel route for the manipulation of excitons in semiconductors.