Nonlinear frequency conversion in optical nanoantennas and metasurfaces:materials evolution and fabrication

Nonlinear frequency conversion is one of the most fundamental processes in nonlinear optics.It has a wide range of applications in our daily lives,including novel light sources,sensing,and information processing.It is usually assumed that nonlinear frequency conversion requires large crystals that gradually accumulate a strong effect.However,the large size of nonlinear crystals is not compatible with the miniaturisation of modern photonic and optoelectronic systems.Therefore,shrinking the nonlinear structures down to the nanoscale,while keeping favourable conversion efficiencies,is of great importance for future photonics applications.In the last decade,researchers have studied the strategies for enhancing the nonlinear efficiencies at the nanoscale,e.g.by employing different nonlinear materials,resonant couplings and hybridization techniques.In this paper,we provide a compact review of the nanomaterials-based efforts,ranging from metal to dielectric and semiconductor nanostructures,including their relevant nanofabrication techniques.

MOF/Polymer-Integrated Multi-Hotspot Mid-Infrared Nanoantennas for Sensitive Detection of CO_(2) Gas

Metal-organic frameworks(MOFs)have been extensively used for gas sorption,storage and separation owing to ultrahigh porosity,exceptional thermal stability,and wide structural diversity.However,when it comes to ultra-low concentration gas detection,technical bottlenecks of MOFs appear due to the poor adsorption capacity at ppm-/ppblevel concentration and the limited sensitivity for signal transduction.Here,we present hybrid MOF-polymer physi-chemisorption mechanisms integrated with infrared(IR)nanoantennas for highly selective and ultrasensitive CO_(2) detection.To improve the adsorption capacity for trace amounts of gas molecules,MOFs are decorated with amino groups to introduce the chemisorption while maintaining the structural integrity for physisorption.Additionally,leveraging all major optimization methods,a multi-hotspot strategy is proposed to improve the sensitivity of nanoantennas by enhancing the near field and engineering the radiative and absorptive loss.As a benefit,we demonstrate the competitive advantages of our strategy against the state-of-the-art miniaturized IR CO_(2) sensors,including low detection limit,high sensitivity(0.18%/ppm),excellent reversibility(variation within 2%),and high selectivity(against C_(2)H_(5)OH,CH_(3)OH,N_(2)).This work provides valuable insights into the integration of advanced porous materials and nanophotonic devices,which can be further adopted in ultra-low concentration gas monitoring in industry and environmental applications.

Compact and high-efficient wavelength demultiplexing coupler based on high-index dielectric nanoantennas

Wavelength demultiplexing waveguide couplers have important applications in integrated nanophotonic devices. Two of the most important indicators of the quality of a wavelength demultiplexing coupler are coupling efficiency and splitting ratio. In this study, we utilize two asymmetric high-index dielectric nanoantennas directly positioned on top of a silicon-on insulator waveguide to realize a compact wavelength demultiplexing coupler in a communication band, which is based on the interference of the waveguide modes coupled by the two nanoantennas. We add a Au substrate for further increasing the coupling efficiency. This has constructive and destructive influences on the antenna＇s in-coupling efficiency owing to the Fabry-Perot（FP） resonance in the SiO2 layer. Therefore, we can realize a wavelength demultiplexing coupler with compact size and high coupling efficiency. This coupler has widespread applications in the areas of wavelength filters,on-chip signal processing, and integrated nanophotonic circuits.

Second harmonic generation spectroscopy on hybrid plasmonic/dielectric nanoantennas

Plasmonic nanoantennas provide unprecedented opportunities to concentrate light fields in subwavelength-sized volumes.By placing a nonlinear dielectric nanoparticle in such a hot spot,one can hope to take advantage of both the field enhancement provided by nanoantennas and the large,nonlinear optical susceptibility of dielectric nanoparticles.To test this concept,we combine gold gap nanoantennas with second-order,nonlinear zinc sulfide nanoparticles,and performsecond harmonic generation(SHG)spectroscopy on the combined hybrid dielectric/plasmonic nanoantennas as well as on the individual constituents.We find that SHG from the bare gold nanoantennas,even though it should be forbidden due tosymmetry reasons,is several orders ofmagnitude larger than that of the bare zinc sulfide nanoparticles.Even stronger second harmonic signals are generated by the hybrid dielectric/plasmonic nanoantennas.Control experiments with nanoantennas containing linear lanthanumfluoride nanoparticles reveal;however,that the increasedSHG efficiency of the hybrid dielectric/plasmonic nanoantennas does not depend on the nonlinear optical susceptibility of the dielectric nanoparticles but is an effect of the modification of the dielectric environment.The combination of a hybrid dielectric/plasmonic nanoantenna,which is only resonant for the incoming pump light field,with a second nanoantenna,which is resonant for the generated second harmonic light,allows for a further increase in the efficiency of SHG.As the second nanoantenna mediates the coupling of the second harmonic light to the far field,this double-resonant approach also provides us with control over the polarization of the generated light.

Fabrication of electrically contacted plasmonic Schottky nanoantennas on silicon

We fabricate Schottky contact photodetectors based on electrically contacted Au nanoantennas on p-Si for the plasmonic detection of sub-bandgap photons in the optical communications wavelength range. Based on a physical model for the internal photoemission of hot carriers, photons coupled onto the Au nanoantennas excite resonant plasmons, which decay into energetic ＂hot＂ holes emitted over the Schottky barrier at the Au/p-Si interface, resulting in a photocurrent. In our device, the active Schottky area consists of Au/p-Si contact and is very small, whereas the probing pad for external electrical interconnection is larger but consists of Au/Ti/p-Si contact having a comparatively higher Schottky barrier, thus producing negligible photo and dark currents.We describe fabrication that involves an electron-beam lithography step overlaid with photolithography. This highly compact component is very promising for applications in high-density Si photonics.

Optical anapole modes in hybrid metal–dielectric nanoantenna for near-field enhancement and optical sensing

Metal–dielectric nanostructures in the optical anapole modes are essential for light–matter interactions due to the low material loss and high near-field enhancement. Herein, a hybrid metal–dielectric nanoantenna composed of six wedgeshaped gold(Au) nanoblocks as well as silica(SiO2) and silicon(Si) nanodiscs is designed and analyzed by the finite element method(FEM). The nanoantenna exhibits flexibility in excitation and manipulation of the anapole mode through the strong coupling between the metal and dielectrics, consequently improving the near-field enhancement at the gap. By systematically optimizing the structural parameters, the electric field enhancement factors at wavelengths corresponding to the anapole modes(AM1 and AM2) can be increased to 518 and 1482, respectively. Moreover, the nanoantenna delivers great performance in optical sensing such as a sensitivity of 550 nm/RIU. The results provide guidance and insights into enhancing the coupling between metals and dielectrics for applications such as surface-enhanced Raman scattering and optical sensing.

All-dielectric χ^(2) metasurfaces: recent progress

Optical metasurfaces,i.e.arrays of nanoantennas with sub-wavelength size and separation,enable the manipulation of light-matter interactions in miniaturized optical components with no classical counterparts.Six decades after the first ob-servation of the second harmonic generation(SHG)in bulk crystals,these devices are expected to break new ground in the field of nonlinear optics,shifting the focus from the phase matching approach achieved within long propagation dis-tances to that of near-field resonances interplay in leaky nanocavities.Here we review the recent progress in SHG with all-dielectric metasurfaces.We discuss the most used technological platforms which underpinned such advances and analyze different SHG control approaches.We finally compare their performances with other well-established technolo-gies,with the hope to delineate the current state-of-the-art and figure out a few scenarios in which these devices might soon offer unprecedented opportunities.

Electric Field Enhancement of Nano Gap of Silver Prisms

Using numerical calculation, we examine the effects of gap distance of a pair of nano gap silver prisms with rounded corners on the local light intensity enhancement. Two peaks due to localized surface plasmon （LSP） excitation are observed in a wavelength range from 900nm to 300nm. The results demonstrate that peaks at a longer and a shorter wavelength corresponded to dipole-like and quadrupole-like LSP resonances, respectively. It is found that a gap distance up to 20 nm provides larger light intensity enhancement than that of a single silver nano prism with rounded corners. Furthermore, nano gap silver prisms are fabricated by direct focused ion beam processing, and we measure the scattering light spectrum of a pair of nano prisms by a confocal optical system. However, the two LSP peaks are not observed in visible range because the sizes of the nano gap and prisms are too large.

Electromagnetic Analysis of Graphene Nanoparticles Operating in the TeraHertz Band

In this work electromagnetic properties of a new type of graphene nanoparticles are investigated. The particles consist of graphene circular and square rings, embedded in a dielectric environment. The electromagnetic behavior in terms of resonant frequency position, magnitude and amplitude width for the absorption cross-section and the near electric field distribution are evaluated. Moreover, the influence of the geometrical parameters is also evaluated. The electromagnetic analysis is derived through proper full-wave numerical simulations. Numerical results show that the nanoparticles can be successfully used for the development of future graphene-based antennas operating in the TeraHertz Band.

Scattering of Circularly Polarized Terahertz Waves on a Graphene Nanoantenna

We present a surface current method to model the graphene rectangular nanoantenna scattering in the terahertz band with Comsol. Compared with the equivalent thin slab method, the results obtained by the surface current method are more accurate and efficient. Then the electromagnetic scattering of circularly polarized terahertz waves on graphene nanoantennas is numerically analyzed by utilizing the surface current method. The depen- dences of the antenna resonant frequency with the circularly polarized wave on width and length are consistent with those for the linear polarized waves. These results are proved to be useful to design et^cient nanoantennas in terahertz wireless communications.

All-dielectric metasurface beam deflector at the visible frequencies

Beam deflectors are important optical elements which can control the propagation direction of the beam in free space.However,with the development of miniaturization of the optical systems,conventional reflector-based mechanical beam deflectors confront a huge challenge due to their large sizes and incompatibility to the device integration.Here we propose an all-dielectric flat metasurface beam deflector which is composed of a single layer array of TiO_2 nanoantennas resting on a fused-silica substrate.Numerical simulations are performed to demonstrate that the proposed deflectors are able to efficiently deflect the incident beam for different angles with transmission efficiency higher than 80%at visible frequencies.This ultrathin all-dielectric metasurface deflector may have great potential applications in integrated optics.

Absorption enhancement and sensing properties of Ag diamond nanoantenna arrays

Noble metal nanoantenna could effectively enhance light absorption and increase detection sensitivity. In this paper,we propose a periodic Ag diamond nanoantenna array to increase the absorption of thin-film solar cells and to improve the detection sensitivity via localized surface plasmon resonance. The effect of nanoantenna arrays on the absorption enhancement is theoretically investigated using the finite difference time domain（FDTD） method with manipulating the spectral response by geometrical parameters of nanoantennas. A maximum absorption enhancement factor of 1.51 has been achieved in this study. In addition, the relation between resonant wavelength（intensity reflectivity） and refractive index is discussed in detail. When detecting the environmental index using resonant wavelengths, a maximum detection sensitivity of about 837 nm/RIU（refractive index unit） and a resolution of about 10-3RIU can be achieved. Moreover, when using the reflectivity, the sensitivity can be as high as 0.93 AU/RIU. Furthermore, we also have theoretically studied the effectiveness of nanoantennas in distinguishing chemical reagents, solution concentrations, and solution allocation ratios by detecting refractive index. From the results presented in this paper, we conclude that this work might be useful for biosensor detection and other types of detections.

Design of Carbon Nanotube Antenna in Nanoscale Range

In this paper, new values of efficiency for coated and non-coated carbon nanotube dipole antennas are found at different ranges of length and constant radius to have an effective model in wireless communication technology, biomedical engineering, sensors and solar cells. The main issue is to get matching between the antenna and the feeding source (discreet port). To have the best value of matching impedance by optimization method through entering trials of impedance value the aim of this paper is to have the best result of efficiency in each length. A new value of efficiency is shown for coated carbon nanotube dipole antennas, it is about 59%.

Zeptomole Imaging of Cytosolic MicroRNA Cancer Biomarkers with A Light-Controlled Nanoantenna

Detecting and quantifying intracellular microRNAs(miRNAs)are a critical step in resolving a cancer diagnostic and resolving the ensemble of gene products that orchestrate the living state of cells.However,the nanoprobe for detecting low abundance miRNAs in cell cytosol is restricted by either the"one-to-one"signaltrigger model or di culty for cytosol delivery.To address these challenges,we designed a lightharvesting nanoantenna-based nanoprobe,which directs excitation energy to a single molecule to sensitively detect cytosolic miRNA.With light irradiation,the light-harvesting nanoantenna e ectively disrupted lysosomal structures by generationof reactive oxygen species,substantially achieved cytosol delivery.The nanoantenna containing>4000 donor dyes can e ciently transfer excitation energy to one or two acceptors with 99%e ciency,leading to unprecedented signal amplification and biosensing sensitivity.The designed nanoantenna can quantify cytosolic miR-210 at zeptomolar level.The fluorescence lifetime of the donor exhibited good relationship with miR-210 concentration in the range of 0.032 to 2.97 amol/ngRNA.The zeptomole sensitivity of nanoantenna provides accurate bioimaging of miR-210 both in multiple cell lines and in vivo assay,which creates a pathway for the creation of miRNA toolbox for quantitative epigenetics and personalized medicine.

Babinet-Inverted Optical Nanoantenna Analogue of Electromagnetically Induced Transparency

A Babinet-inverted optical nanoantenna analogue of electromagnetically induced transparency based on the coupling between two magnetic dipole antennas and a magnetic octupole antenna in a Au film waveguide is demonstrated. Simulation results indicate that a pronounced elimination occurs in the radiating spectrum due to the coupling-induced radiation suppression. A two-oscillator electromagnetically induced transparency model is used to describe the antenna. The coupling coefficient between the magnetic dipole antennas and the magnetic octupole antenna is calculated using the model and is found to decline exponentially with the increase of the distance between them. Such an antenna can be directly integrated with optical waveguides or transmission lines,thus is of fundamental significance for the applications in nano-optics, such as the optical device miniaturizations and photonic circuit integrations.

Nanoplasmonic mid-infrared biosensor for in vitro protein secondary structure detection

Plasmonic nanoantennas offer new applications in mid-infrared(mid-IR)absorption spectroscopy with ultrasensitive detection of structural signatures of biomolecules,such as proteins,due to their strong resonant near-fields.The amide I fingerprint of a protein contains conformational information that is greatly important for understanding its function in health and disease.Here,we introduce a non-invasive,label-free mid-IR nanoantenna-array sensor for secondary structure identification of nanometer-thin protein layers in aqueous solution by resolving the content of plasmonically enhanced amide I signatures.We successfully detect random coil to crossβ-sheet conformational changes associated withα-synuclein protein aggregation,a detrimental process in many neurodegenerative disorders.Notably,our experimental results demonstrate high conformational sensitivity by differentiating subtle secondary-structural variations in a nativeβ-sheet protein monolayer from those of crossβ-sheets,which are characteristic of pathological aggregates.Our nanoplasmonic biosensor is a highly promising and versatile tool for in vitro structural analysis of thin protein layers.

Tailoring magnetic and electric resonances with dielectric nanocubes for broadband and high-efficiency unidirectional scattering

The interference of optically induced electric and magnetic resonances in high-refractive-index dielectric nanoparticles provides a new approach to control and shape the scattering patterns of light in the field of nanophotonics. In this Letter, we spectrally tune the electric and magnetic resonances by varying the geometry of a single isolated lead telluride （PbTe） dielectric nanocube. Then, we overlap the electric dipole resonance and magnetic dipole resonance to suppress backward scattering and enhance forward scattering in the resonance region. Furthermore, a broadband unidirectional scattering is achieved by structuring the dielectric nanocuboids as a trimer antenna.

Long-lived electron emission reveals localized plasmon modes in disordered nanosponge antennas

We report long-lived,highly spatially localized plasmon states on the surface of nanoporous gold nanoparticles—nanosponges—with high excitation efficiency.It is well known that disorder on the nanometer scale,particularly in two-dimensional systems,can lead to plasmon localization and large field enhancements,which can,in turn,be used to enhance nonlinear optical effects and to study and exploit quantum optical processes.Here,we introduce promising,three-dimensional model systems for light capture and plasmon localization as gold nanosponges that are formed by the dewetting of gold/silver bilayers and dealloying.We study light-induced electron emission from single nanosponges,a nonlinear process with exponents of n≈5...7,using ultrashort laser pulse excitation to achieve femtosecond time resolution.The long-lived electron emission process proves,in combination with optical extinction measurements and finite-difference time-domain calculations,the existence of localized modes with lifetimes of more than 20 fs.These electrons couple efficiently to the dipole antenna mode of each individual nanosponge,which in turn couples to the far-field.Thus,individual gold nanosponges are cheap and robust disordered nanoantennas with strong local resonances,and an ensemble of nanosponges constitutes a meta material with a strong polarization independent,nonlinear response over a wide frequency range.

Antenna-assisted picosecond control of nanoscale phase transition in vanadium dioxide

Nanoscale devices in which the interaction with light can be configured using external control signals hold great interest for next-generation optoelectronic circuits.Materials exhibiting a structural or electronic phase transition offer a large modulation contrast with multi-level optical switching and memory functionalities.In addition,plasmonic nanoantennas can provide an efficient enhancement mechanism for both the optically induced excitation and the readout of materials strategically positioned in their local environment.Here,we demonstrate picosecond all-optical switching of the local phase transition in plasmonic antenna-vanadium dioxide(VO_(2))hybrids,exploiting strong resonant field enhancement and selective optical pumping in plasmonic hotspots.Polarization-and wavelength-dependent pump–probe spectroscopy of multifrequency crossed antenna arrays shows that nanoscale optical switching in plasmonic hotspots does not affect neighboring antennas placed within 100 nm of the excited antennas.The antenna-assisted pumping mechanism is confirmed by numerical model calculations of the resonant,antenna-mediated local heating on a picosecond time scale.The hybrid,nanoscale excitation mechanism results in 20 times reduced switching energies and 5 times faster recovery times than a VO_(2) film without antennas,enabling fully reversible switching at over two million cycles per second and at local switching energies in the picojoule range.The hybrid solution of antennas and VO_(2) provides a conceptual framework to merge the field localization and phase-transition response,enabling precise,nanoscale optical memory functionalities.

Fano resonance boosted cascaded optical field enhancement in a plasmonic nanoparticle-in-cavity nanoantenna array and its SERS application

Cascaded optical field enhancement(CFE)can be realized in some specially designed multiscale plasmonic nanostructures,in which the generation of extremely strong fields at nanoscale volume is crucial for many applications,for example,surface-enhanced Raman spectroscopy(SERS).In this paper,we propose a strategy for realizing a high-quality plasmonic nanoparticle-in-cavity(PIC)nanoantenna array,in which strong coupling between a nanoparticle(NP)dark mode with a high-order nanocavity bright mode can produce strong Fano resonance at the target wavelength.The Fano resonance can effectively boost the CFE in a PIC.A cost-effective and reliable nanofabrication method is developed using room temperature nanoimprinting lithography to manufacture high-quality PIC arrays.This technique guarantees the generation of only one gold NP at the bottom of each nanocavity,which is crucial for the generation of the expected CFE.To demonstrate the performance and application of the PIC array,the PIC array is employed as an active SERS substrate for detecting 4-aminothiophenol molecules.An experimental SERS enhancement factor of 2×10^(7) is obtained,which verifies the field enhancement and the potential of this device.