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If not for its inherently weak opticalabsorption at visible andinfrared wavelengths, graphene would show exceptional promise foroptoelectronic applications. Here we show that by nanopatterning agraphene layer into an array of closely packed graphene nanodisks,its absorption efficiency can be increased from less than 3% to 30%in the infrared region of the spectrum. We examine the dependenceof the enhanced absorption on nanodisk size and interparticle spacing.By incorporating graphene nanodisk arrays into an active device, wedemonstrate that this enhanced absorption efficiency is voltage-tunable,indicating strong potential for nanopatterned graphene as an activemedium for infrared electro-optic devices. [ABSTRACT FROM AUTHOR]

When an Au nanoparticle in a liquidmedium is illuminated withresonant light of sufficient intensity, a nanometer scale envelopeof vapora “nanobubble”surrounding theparticle, is formed. This is the nanoscale onset of the well-knownprocess of liquid boiling, occurring at a single nanoparticle nucleationsite, resulting from the photothermal response of the nanoparticle.Here we examine bubble formation at an individual metallic nanoparticlein detail. Incipient nanobubble formation is observed by monitoringthe plasmon resonance shift of an individual, illuminated Au nanoparticle,when its local environment changes from liquid to vapor. The temperatureon the nanoparticle surface is monitored during this process, wherea dramatic temperature jump is observed as the nanoscale vapor layerthermally decouples the nanoparticle from the surrounding liquid.By increasing the intensity of the incident light or decreasing theinterparticle separation, we observe the formation of micrometer-sizedbubbles resulting from the coalescence of nanoparticle-“bound”vapor envelopes. These studies provide the first direct and quantitativeanalysis of the evolution of light-induced steam generation by nanoparticlesfrom the nanoscale to the macroscale, a process that is of fundamentalinterest for a growing number of applications. [ABSTRACT FROM AUTHOR]

Nanoscale antennas sandwiched between two graphene monolayersyielda photodetector that efficiently converts visible and near-infraredphotons into electrons with an 800% enhancement of the photocurrentrelative to the antennaless graphene device. The antenna contributesto the photocurrent in two ways: by the transfer of hot electronsgenerated in the antenna structure upon plasmon decay, as well asby direct plasmon-enhanced excitation of intrinsic graphene electronsdue to the antenna near field. This results in a graphene-based photodetectorachieving up to 20% internal quantum efficiency in the visible andnear-infrared regions of the spectrum. This device can serve as amodel for merging the light-harvesting characteristics of opticalfrequency antennas with the highly attractive transport propertiesof graphene in new optoelectronic devices. [ABSTRACT FROM AUTHOR]

Integrating two-dimensional (2D) transition-metal dichalcogenides (TMDCs) into dielectric plasmonic nanostructures enables the miniaturization of on-chip nanophotonic devices. Here we report on a high-quality light emitter based on the newly designed 2D h-BN/WS 2 heterostructure integrated with an array of TiO 2 nanostripes. Different from a traditional strongly coupled system such as the TMDCs/metallic plasmonic nanostructure, we first employ dielectric nanocavities and achieve a Purcell enhancement on the nanoscale at room temperature. Furthermore, we demonstrate that the light emission strength can be effectively controlled by tuning the polarization configuration. Such a polarization dependence meanwhile could be proof of the resonant energy transfer theory of dipole-dipole coupling between TMDCs and a dielectric nanostructure. This work gains experimental and simulated insights into modified spontaneous emission with dielectric nanoplasmonic platforms, presenting a promising route toward practical applications of 2D semiconducting photonic emitters on a silica-based chip.

Two-dimensional nanomaterials, such as graphene and molybdenum disulfide (MoS 2 ), have recently attracted widespread attention as surface-enhanced Raman scattering (SERS) substrates. However, their SERS enhancement is of a smaller magnitude than that of noble metal nanomaterials, and therefore, the detection sensitivity still needs to be substantially improved for practical applications. Here, we present the first detailed studies on the effect of the (MoS 2 ) interlayer distances on the SERS intensity enhancement. We find that MoS 2 with smaller interlayer distances achieves an SERS enhancement factor as high as 5.31 × 10 5 , which is one of the highest enhancement factors to date among the two-dimensional nanomaterial SERS sensors. This remarkable SERS sensitivity is attributed to the highly efficient charge transfer from MoS 2 to probe molecules. The charge-transfer ability directly determines the variable quantity d z 2 orbitals of Mo elements in the MoS 2 -molecule system and then tunes the Raman intensity of probe molecules. Our work contributes to reveal the influence of MoS 2 interlayer spacing on SERS detection and to open a new way for designing a highly sensitive nonmetal SERS technology.

Devices operating with excitons have promising prospects for overcoming the dilemma of response time and integration in current generation of electron- or/and photon-based elements and devices. Although the intrinsic properties including edges, grain boundaries, and defects of atomically thin semiconductors have been demonstrated as a powerful tool to adjust the bandgap and exciton energy, investigating the intrinsic modulation of spatiotemporal dynamics still remains challenging on account of the short exciton diffusion length. Here, we achieve the attractive remote lightening phenomenon, in which the emission region could be far away (up to 14.6 μm) from the excitation center, by utilizing a femtosecond laser with ultrahigh peak power as excitation source and the edge region with high photoluminescence efficiency as a bright emitter. Furthermore, the ultrafast transition between exciton and trion is demonstrated, which provides insight into the intrinsic modulation on populations of exciton and trion states. The complete cascaded physical scenario of exciton spatiotemporal dynamics is eventually established. This work can refresh our perspective on the spatial nonuniformities of CVD-grown atomically thin semiconductors and provide important implications for developing durable and stable excitonic devices in the future.

The dangling-bond-free surfaces of van der Waals (vdW) materials make it possible to build ultrathin junctions. Fundamentally, the interfacial phenomena and related optoelectronic properties of vdW junctions are modulated by the interlayer coupling effect. However, the weak interlayer coupling of vdW heterostructures limits the interlayer charge transfer efficiency, resulting in low photoresponsivity. Here, a bilayer MoS 2 homogeneous junction is constructed by stacking the as-grown onto the self-healed monolayer MoS 2 . The homojunction barrier of ∼165 meV is obtained by the electronic structure modulation of defect self-healing. This homojunction reveals the stronger interlayer coupling effect in comparison with vdW heterostructures. This ultrastrong interlayer coupling effect is experimentally verified by Raman spectra and angle-resolved photoemission spectroscopy. The ultrafast interlayer charge transfer takes place within ∼447 fs, which is faster than those of most vdW heterostructures. Furthermore, the homojunction photodiode manifests outstanding rectifying behavior with an ideal factor of ∼1.6, perfect air stability over 12 months, and high responsivity of ∼54.6 mA/W. Moreover, the interlayer exciton peak of ∼1.66 eV is found in vdW homojunctions. This work offers an uncommon vdW junction with strong interlayer coupling and perfects the relevance of interlayer coupling and interlayer charge transfer.

The chiral state of light plays a vital role in light-matter interactions and the consequent revolution of nanophotonic devices and advanced modern chiroptics. As the light-matter interaction goes into the nano- and quantum world, numerous chiroptical technologies and quantum devices require precise knowledge of chiral electromagnetic modes and chiral radiative local density of states (LDOS) distributions in detail, which directly determine the chiral light-matter interaction for applications such as chiral light detection and emission. With classical optical techniques failing to directly measure the chiral radiative LDOS, deep-subwavelength imaging and control of circular polarization (CP) light associated phenomena are introduced into the agenda. Here, we simultaneously reveal the hidden chiral electromagnetic mode and acquire its chiral radiative LDOS distribution of a single symmetric nanostructure at the deep-subwavelength scale by using CP-resolved cathodoluminescence (CL) microscopy. The chirality of the symmetric nanostructure under normally incident light excitation, resulting from the interference between the symmetric and antisymmetric modes of the V-shaped nanoantenna, is hidden in the near field with a giant chiral distribution (∼99%) at the arm-ends, which enables the circularly polarized CL emission from the radiative LDOS hot-spot and the following active helicity control at the deep-subwavelength scale. The proposed V-shaped nanostructure as a functional unit is further applied to the helicity-dependent binary encoding and the two-dimensional display applications. The proposed physical principle and experimental configuration can promote the future chiral characterization and manipulation at the deep-subwavelength scale and provide direct guidelines for the optimization of chiral light-matter interactions for future quantum studies.

Herein, we report the successful application of hybrid Au-Ag nanoparticles (NPs) and nanochains (NCs) in the harvesting of visible light energy for selective hydrogenation reactions. For individual Au@Ag NPs with Au25 cores, the conversion and turnover frequency (TOF) are approximately 8 and 10 times higher than those of Au25 NPs, respectively. Notably, after the self-assembly of the Au@Ag NPs, the conversion and TOF of 1D NCs were approximately 2.5 and 2 times higher than those of isolated Au@Ag NPs, respectively, owing to the coupling of surface plasmon and the increase in the rate at which hot (energetic) electrons are generated with the formation of plasmonic hot spots between NPs. Furthermore, the surface-enhanced Raman scattering (SERS) activity of 1D Au@Ag NCs was strengthened by nearly 2 orders of magnitude.

Circularly polarized light is crucial for the modern physics research. Highly integrated nanophotonic device further requires the control of circularly polarized light at subnanoscale. Here, we report the tuning of chiral cathodoluminescence (CL) on single Au nanostructure under electron stimulation. The detected CL helicity is found ultrasensitive with the electron impinging position on the structure, and a helicity switch is achieved within a 1.86 nm electron-beam movement, which is applied to construct ternary notation sequence. The proposed configuration provides a delicate platform for the CL helicity control, which opens a way for the future chiral applications at subnanoscale like information coding and quantum communication.

The manipulation of light in an integrated circuit is crucial for the development of high-speed electro-optic devices. Recently, molybdenum disulfide (MoS 2 ) monolayers generated broad interest for the optoelectronics because of their huge exciton binding energy, tunable optical emission, direct electronic band-gap structure, etc. Miniaturization and multifunctionality of electro-optic devices further require the manipulation of light-matter interaction at the single-nanoparticle level. The strong exciton-plasmon interaction that is generated between the MoS 2 monolayers and metallic nanostructures may be a possible solution for compact electro-optic devices at the nanoscale. Here, we demonstrate a nanoplasmonic modulator in the visible spectral region by combining the MoS 2 monolayers with a single Au nanodisk. The narrow MoS 2 excitons coupled with broad Au plasmons result in a deep Fano resonance, which can be switched on and off by applying different gate voltages on the MoS 2 monolayers. A reversible display device that is based on this single-nanoparticle modulator is demonstrated with a heptamer pattern that is actively controlled by the external gates. Our work provides a potential application for electro-optic modulation on the nanoscale and promotes the development of gate-tunable nanoplasmonic devices in the future.

In this paper, we review nano-Raman techniques based on aperture scanning near-field optical microscopy (SNOM). Fundamentals of SNOM and aperture-tip-based near-field Raman spectroscopy and their applications in key technical issues, including Raman signal intensity and collection time, are introduced. Recent advances in the tip design are discussed, and applications of the aperture-SNOM-based nano-Raman technique are presented. We attempt to identify the most pressing open questions in this field. We believe that, by improving the power transmission efficiency and combining the local field enhancing technique with the tip-enhanced spectroscopy, the performance of aperture-SNOM can be significantly improved. Its nanometer-scale excitation volume and the consequent low background make the aperture-tip technique feasible for many important samples that cannot be measured by other optical nanospectroscopies.

Valleytronics is a promising paradigm to explore the emergent degree of freedom for charge carriers on the energy band edges. Using ab initio calculations, we reveal that the honeycomb boron nitride (h-BN) monolayer shows a pair of inequivalent valleys in the vicinities of the vertices of hexagonal Brillouin zone even without the protection of the C 3 symmetry. The inequivalent valleys give rise to a 2-fold degree of freedom named the valley pseudospin. The valley pseudospin with a tunable bandgap from deep ultraviolet to far-infrared spectra can be obtained by doping h-BN monolayer with carbon atoms. For a low-concentration carbon periodically doped h-BN monolayer, the subbands with constant valley Hall conductance are predicted due to the interaction between the artificial superlattice and valleys. In addition, the valley pseudospin can be manipulated by visible light for high-concentration carbon doped h-BN monolayer. In agreement with our calculations, the circularly polarized photoluminescence spectra of the B 0.92 NC 2.44 sample show a maximum valley-contrasting circular polarization of 40% and 70% at room temperature and 77 K, respectively. Our work demonstrates a class of valleytronic materials with a controllable bandgap.

Molybdenum disulfide (MoS 2 ) monolayer as one of the atomic thickness two-dimensional materials has remarkable electronic and optical properties, which is an ideal candidate for a wide range of optoelectronic applications. However, the atomic monolayer thickness poses a significant challenge in MoS 2 photoluminescence emission due to weak light-matter interaction. Here, we investigate the MoS 2 exciton-plasmon interaction with spin-orbit coupling of light. The plasmonic spiral rings with subwavelength dimensions are designed and fabricated on hybrid substrates. MoS 2 photoluminescence enhancement can be actively controlled by changing the incident optical spin states, laser powers, and the nanospiral geometries, which is arising from the change of field enhancement at near-field region. Planar light-emitting devices based on spin-orbit coupling (SOC) effect were further realized and flexibly controlled by changing the polarization of light. The SOC effect is discussed by the accumulation of geometric and dynamic phases, which can be demonstrated and elaborated by the Majorana sphere model. Our results provide a way to manipulate MoS 2 light-matter interaction actively and can be further applied in the spin-dependent light-emitting devices at the nanoscale.

Flexible ZnO thin film UV sensors with 3 orders of magnitude improvement in sensitivity and 2 orders of magnitude acceleration in speed are realized via light absorption efficiency enhancement and surface encapsulation. Devices are constructed on polyethylene substrate incorporating morphology controlled ZnO nanorod arrays (NRAs) as absorbing antireflection layers. By adjusting the morphology of ZnO NRAs, the light absorptance exceeds 99% through effectively trapping incident photons. As a result, the sensitivity of the UV sensor reaches 109 000. Moreover, a mechanism of competitive chemisorption between O2 and H2O at oxygen vacancy sites is proposed to explain the phenomenon of the speed acceleration in moist environment. A new approach of humectant encapsulation is used to make H2O participant rapid processes dominant for speed acceleration. Two orders of magnitude speed enhancement in reset time is achieved by polyethylene glycol encapsulation. After a total 3000 cycles bending test, the decay in the responsivity of UV sensor is within 20%, indicating good mechanical stability. All these results not only demonstrate a simple, effective and scalable approach to fabricate high sensitive and fast response flexible ZnO UV sensors, but also provide meaningful references for performance boosting of photoelectronic devices based on other oxide semiconductors.

Plasmonic excitation of Au nanoparticles deposited on a MoS2 monolayer changes the absorption and photoluminescence characteristics of the material. Hot electrons generated from the Au nanoparticles are transferred into the MoS2 monolayers, resulting in n-doping. The doping effect of plasmonic hot electrons modulates the dielectric permittivity of materials, resulting in a red shift of both the absorption and the photoluminescence spectrum. This spectroscopic tuning was further investigated experimentally by using different Au nanoparticle concentrations, excitation laser wavelengths, and intensities. An analytical model for the photoinduced modulation of the MoS2 dielectric function and its exciton binding energy change is developed and used to estimate the doping density of plasmonic hot electrons. Our approach is important for the development of photonic devices for active control of light by light.

Graphene has emerged as an outstanding material for optoelectronic applications due to its high electronic mobility and unique doping capabilities. Here we demonstrate electrical tunability and hybridization of plasmons in graphene nanodisks and nanorings down to 3.7 μm light wavelength. By electrically doping patterned graphene arrays with an applied gate voltage, we observe radical changes in the plasmon energy and strength, in excellent quantitative agreement with rigorous analytical theory. We further show evidence of an unexpected increase in plasmon lifetime with growing energy. Plasmon hybridization and electrical doping in nanorings of suitably chosen nanoscale dimensions are key elements for bringing the optical response of graphene closer to the near-infrared, where it can provide a robust, integrable platform for light modulation, switching, and sensing.

A metallic nanoantenna, under resonant illumination, injects nonequilibrium hot electrons into a nearby graphene structure, effectively doping the material. A prominent change in carrier density was observed for a plasmonic antenna-patterned graphene sheet following laser excitation, shifting the Dirac point, as determined from the gate-controlled transport characteristic. The effect is due to hot electron generation resulting from the decay of the nanoantenna plasmon following resonant excitation. The effect is highly tunable, depending on the resonant frequency of the plasmonic antenna, as well as on the incident laser power. Hot electron-doped graphene represents a new type of hybrid material that shows great promise for optoelectronic device applications.

A wide variety of complex, multicomponent plasmonic nanostructures have been shown to possess Fano resonances. Here we introduce a remarkably simple planar nanostructure, a single metallic nanodisk with a missing wedge-shaped slice, that also supports a Fano resonance. In this geometry, the Fano line shape arises from the coupling between a hybridized plasmon resonance of the disk and a narrower quadrupolar mode supported by the edge of the missing wedge slice. As a consequence, both disk size and wedge angle control the properties of the resonance. A semianalytical description of plasmon hybridization proves useful for analyzing the resulting line shape.

Ag nanowire with the receiving and transmitting Ag bow tie antenna pairs at its incident and emission ends was patterned on the SiO(2) substrate to realize an enhanced surface plasmon emission with a factor of 45 compared to the single Ag nanowire without antenna pairs. The receiving and transmitting bow tie antenna pairs enhanced the plasmon coupling and emission efficiencies of the Ag nanowire. And the maximum plasmon emission sensitively depended on the length of Ag nanowire, the arm length of bow tie antennas, and the incident angle of optical excitation. This enhanced plasmon emission was confirmed by finite-difference time-domain simulations and explored with analytical calculations using the impedance matching theory at optical frequency.

Plasmonic focusing was investigated in symmetry broken nanocorrals under linearly polarized illumination. Near-field optical measurements of the perpendicular electric field show that a single subwavelength spot size of 320 nm can be generated. The interference pattern within the corral can be controlled by changing the polarization of optical excitation and the degree of symmetry breaking. The intensity enhancement factor was investigated using finite-difference time-domain simulations and confirmed by analytical calculations taking into account the plasmon damping and multiple reflections against the corral wall.

Planar plasmonic focusing of surface plasmon polaritons (SPPs) by an in-plane nanostructure consisting of Ag-column arrays and an in-plane Fresnel zone plate (FZP) with a Cu grating underneath for energy compensation was demonstrated. The CdS-based hybrid plasmonic waveguide generated in the Ag-column arrays was characterized with a scanning near-field optical microscope. By using the FZP focusing structure, the SPP modes were separated from the CdS photoluminescence background and focused at the FZP focus area, and in this way, were used as the source for the SPP waveguide. Finite-difference time-domain simulations correspond with the experimental observations, suggesting that this is indeed an effective approach to control SPP coupling within the dielectric nanoribbon waveguide.