Selective control of the emission pattern of valley-polarized excitons in monolayer transition metal dichalcogenides is essential for advancing valleytronic, quantum information, and optoelectronic devices. Although substantial progress has been made in directionally routing photoluminescence from these materials, key challenges persist: specifically, establishing how observed routing effects relate to the degree of valley polarization and distinguishing genuine valley-dependent routing from spin-momentum coupling, an optical scattering effect unrelated to the emitter. In this work, we address these challenges by experimentally and numerically demonstrating a direct link between excitonic valley polarization and the resulting farfield emission pattern, enabling quantitative evaluation of valley-selective emission routing. We report valley-dependent manipulation of the angular emission pattern of monolayer tungsten diselenide using gold nanobar dimer antennas at cryogenic temperatures. By probing the emission under opposite circularly polarized excitation, we observe a valley-selective asymmetry in the photoluminescence circular dichroism of 2%. These measurements are supported by a reciprocity-based numerical framework that enables modeling of valley-selective emission in periodic systems. Our calculations further reveal that the observed valley-dependent directionality is a symmetry-protected property of the nanoantenna array arising from its extrinsic chirality at oblique emission angles, and that it can be substantially enhanced by tailoring the emitter distribution. Together, these results establish our nanoantenna platform as a robust route toward valleytronic signal processing.
Transition metal dichalcogenides are promising quantum materials because of unique exciton-photon interactions. These interactions can be enhanced by coupling with resonant photonic structures, especially in the nonlinear light emission processes like second-harmonic generation (SHG). However, excitonic absorption may dampen SHG. Here, we demonstrate tunable SHG enhancement using virtual coupling effects between quasi-bound state in the continuum (qBIC) optical resonances and tunable excitons in high-index WS2 metasurfaces with crescent meta-atoms. These metasurfaces promote a magnetic-type qBIC resonance, enabling control over nonlinear optical processes in the visible spectrum. The used qBIC resonance at half the exciton energy increases SHG efficiency by 98-fold compared to monolayer WS2 and by four orders of magnitude relative to an unpatterned WS2 film. The enhancement is tunable with temperature and incident light polarization, allowing the dynamic control of virtual coupling and SHG efficiency, thereby paving the way for next-generation reconfigurable metaoptics devices.
Transition metal dichalcogenides (TMDCs) have demonstrated significant potential as versatile quantum materials for light absorption and emission. Their unique properties are primarily governed by exciton-photon interactions, which can be substantially enhanced through coupling with resonant photonic structures. For example, nonlinear light emission, such as second harmonic generation (SHG) is doubly enhanced when the incident wave is resonant simultaneously with the excitonic and photonic resonance. However, the excitonic absorption of incident waves can significantly dump the SHG emission. Here, we propose and demonstrate a tunable enhancement of SHG by leveraging virtual coupling effects between quasi-bound states in the continuum (qBIC) optical resonances and tunable excitons in arrays of high-index WS2 crescent metaatoms. These crescent metaatoms excites a pure magnetic type qBIC resonance, enabling dynamic control and enhancement of nonlinear optical processes in visible spectrum. Our findings demonstrate that an array of WS2 crescent metaatoms, exhibiting qBIC resonance at half the exciton energy, enhances SHG efficiency by more than 98-fold compared to monolayer WS2 (1L-WS2) and four orders of magnitude relative to unpatterned WS2 film. This substantial SHG enhancement is tunable as a function of temperature and polarization angle of incident light, allowing us to obtain control of the virtual coupling and SHG efficiency in the visible spectrum (600-650 nm). Our work opens new avenues toward next-generation reconfigurable meta-optics devices.
Metasurfaces have long served as a cornerstone technique to enhance nonlinear processes, enabling frequency conversion, efficient light manipulation and integrated photonic devices. However, traditional bulk materials often suffer from high absorption losses, hindering the second harmonic generation (SHG) efficiency. Here, we develop a novel approach exploiting quasi-bound state in continuum (qBIC) to achieve giant SHG efficiency in metasurfaces utilizing 3R-MoS_2, with high index, superior damage threshold and inherent nonlinearity. The high refractive index of 3R-MoS_2, facilitates the high-quality factor (Q) metasurfaces, leading to reduced radiation leakage and localized light confinement within qBIC resonances, with which a remarkable 2000-fold enhancement in SHG intensity has been experimentally demonstrated. Additionally, the twist angle between the lattice orientation and the metasurface unit geometry exhibits a 120^∘ periodicity in its influence on SHG behaviour. By strategically designing to realize the qBIC and exciton dual resonances and optimized twist angle (30^∘), SHG conversion efficiency was boosted to 1 than those of the best metasurfaces on traditional bulk materials. This approach enables potential applications in various areas of nonlinear optics, including frequency conversion, light manipulation, integrated photonics, and quantum communications.
Transition metal dichalcogenides are promising quantum materials because of unique exciton-photon interactions. These interactions can be enhanced by coupling with resonant photonic structures, especially in the nonlinear light emission processes like second-harmonic generation (SHG). However, excitonic absorption may dampen SHG. Here, we demonstrate tunable SHG enhancement using virtual coupling effects between quasi-bound state in the continuum (qBIC) optical resonances and tunable excitons in high-index WS 2 metasurfaces with crescent meta-atoms. These metasurfaces promote a magnetic-type qBIC resonance, enabling control over nonlinear optical processes in the visible spectrum. The used qBIC resonance at half the exciton energy increases SHG efficiency by 98-fold compared to monolayer WS 2 and by four orders of magnitude relative to an unpatterned WS 2 film. The enhancement is tunable with temperature and incident light polarization, allowing the dynamic control of virtual coupling and SHG efficiency, thereby paving the way for next-generation reconfigurable metaoptics devices.
Recently, InGaAs/InP multiple quantum well nanowires grown by selective area epitaxy have been demonstrated with uniform morphology and high optical quality. The InGaAs quantum wells wrapping around the nanowire core are formed with both axial and radial components. As such the radial quantum well configuration presents a unique advantage for the realization of intraband absorption of normal-incidence light in the nanowires, which cannot be achieved in conventional planar quantum well structures due to polarization selection rules. We report here mid-infrared intraband transitions within the atmospheric window (3–5 μm) in InP nanowire arrays embedded with five InGaAs quantum wells under normal-incidence light. The light absorption coefficient of the quantum wells is modeled, and the absorption peak indicates a bound-to-continuum transition. The intraband photocurrent shows a linear dependence on the incident power, while the interband photoresponse is sublinear due to the surface states of the nanowires. These nanowires with radial quantum wells open up great opportunities for developing next-generation mid- to long-wavelength infrared photodetectors and focal plane arrays.
In its 60 years of existence, the field of nonlinear optics (NLO) has witnessed tremendous growth, and it has been gaining additional momentum over the past two decades thanks to major breakthroughs in materials science and technology. However, a data table providing an overview of these post-2000 developments in NLO has not yet been presented. Here, we introduce a new set of NLO data tables based on a representative collection of experimental works published since 2000 for different material categories (bulk materials, solvents, 0D-1D-2D materials, metamaterials, fiber waveguiding materials, on-chip waveguiding materials, hybrid waveguiding systems, and THz NLO materials) [1]. The data tables are mostly focused on experimental papers that not only provided NLO coefficients, but also reported experimental parameters that give the context and limits of validity for using the quoted coefficient values. In this regard, we decided to also include in our work a list of best practices for performing and reporting NLO experiments [1].
The field of nonlinear optics (NLO), launched about 60 years ago, has gained considerable momentum over the past two decades, resulting in an enormous growth in NLO publications for a wide range of material categories, including bulk materials, 0D-1D-2D materials, metamaterials, fiber waveguiding materials, on-chip waveguiding materials, and hybrid waveguiding systems. However, a convenient summary of NLO data collected since 2000 for these different material types has been lacking and would be a valuable resource for researchers in the field. Here, we present a new set of data tables showcasing a representative list of NLO properties taken from the literature since 2000 on the above-mentioned material categories. Furthermore, we provide best practices for performing and reporting NLO experiments. These best practices underpin the selection process that we used for including papers in the tables, and also form the foundation for a more adequate comparison, interpretation, and use of the NLO parameters published today and those that will be published in the future.
Second-harmonic generation (SHG) offers a convenient approach for infrared-to-visible light conversion in tunable nanoscale light sources and optical communication. Semiconductor nanostructures offer rich possibilities to tailor their nonlinear optical properties. In this study, strong second-harmonic generation in InP nanomembranes with InAsP quantum well (QW) is demonstrated. Compared with bulk InP, up to 100 times enhancement of SHG is achieved in the short-wave infrared range. This enhancement is shown to be predominantly induced by the resonance-enhanced absorption and quantum confinement of fundamental wavelengths in the InAsP QW. The thin nanomembrane structure will also provide nanocavity enhancement for second-harmonic wavelengths. The enhanced SHG peak wavelengths can also be tuned by changing the QW composition. These findings provide an effective strategy for enhancing and manipulating the second-harmonic generation in semiconductor quantum-confined nanostructures for on-chip all-optical applications.
On the occasion of 60 years of nonlinear-optical research, we present new data tables listing nonlinear- optical properties for different material categories as reported in the literature since 2000, and provide best practices for performing experiments.
In its 60 years of existence, the field of nonlinear optics has gained momentum especially over the past two decades thanks to major breakthroughs in material science and technology. In this article, we present a new set of data tables listing nonlinear-optical properties for different material categories as reported in the literature since 2000. The papers included in the data tables are representative experimental works on bulk materials, solvents, 0D-1D-2D materials, metamaterials, fiber waveguiding materials, on-chip waveguiding materials, hybrid waveguiding systems, and materials suitable for nonlinear optics at THz frequencies. In addition to the data tables, we also provide best practices for performing and reporting nonlinear-optical experiments. These best practices underpin the selection process that was used for including papers in the tables. While the tables indeed show strong advancements in the field over the past two decades, we encourage the nonlinear-optics community to implement the identified best practices in future works. This will allow a more adequate comparison, interpretation and use of the published parameters, and as such further stimulate the overall progress in nonlinear-optical science and applications.
Lead iodide (PbI2) is a van der Waals layered semiconductor with a direct bandgap in its bulk form and a hexagonal layered crystalline structure. The recently developed PbI2 nanosheets have shown great promise for high-performance optoelectronic devices, including nanolasers and photodetectors. However, despite being widely used as a precursor for perovskite materials, the optical properties of PbI2 nanomaterials remain largely unexplored. Here, we determine the nonlinear optical properties of PbI2 nanosheets by utilising nonlinear microscopy as a non-invasive optical technique. We demonstrate the nonlinearity enhancement dependent on excitonic resonances, crystalline orientation, thickness, and influence of the substrate. Our results allow for estimating the second- and third-order nonlinear susceptibilities of the nanosheets, opening new opportunities for the use of PbI2 nanosheets as nonlinear and quantum light sources.
We experimentally investigate the coupling of spontaneous emission from monolayer tungsten diselenide to resonant plasmonic nanoantennas at cryogenic temperatures. The low temperature conditions enable preserved chiral polarization states of the spontaneous emission with a valley-selective handedness. By back-focal plane imaging of the scattered spontaneous emission we demonstrate a valley-selective directional emission pattern.
We experimentally investigate the coupling of spontaneous emission from monolayer tungsten diselenide to resonant plasmonic nanoantennas at cryogenic temperatures. The low temperature conditions enable preserved chiral polarization states of the spontaneous emission with a valleyselective handedness. By back-focal plane imaging of the scattered spontaneous emission we demonstrate a valley-selective directional emission pattern.
Nonlinear light sources are central to a myriad of applications, driving a quest for their miniaturisation down to the nanoscale. In this quest, nonlinear metasurfaces hold a great promise, as they enhance nonlinear effects through their resonant photonic environment and high refractive index, such as in high-index dielectric metasurfaces. However, despite the sub-diffractive operation of dielectric metasurfaces at the fundamental wave, this condition is not fulfilled for the nonlinearly generated harmonic waves, thereby all nonlinear metasurfaces to date emit multiple diffractive beams. Here, we demonstrate the enhanced single-beam second- and third-harmonic generation in a metasurface of crystalline transition-metal-dichalcogenide material, offering the highest refractive index. We show that the interplay between the resonances of the metasurface allows for tuning of the unidirectional second-harmonic radiation in forward or backward direction, not possible in any bulk nonlinear crystal. Our results open new opportunities for metasurface-based nonlinear light-sources, including nonlinear mirrors and entangled-photon generation.
We demonstrate a nonlinear microscopy-based non-invasive technique for characterisation of PbI2 nanosheets. By using the polarisation, wavelength and thickness dependences of the harmonic emissions we can precisely determine their thickness, strain and crystalline orientation. 160.4236 160.4330 Lead iodide (PbI2) is a layered material with unique optical and electrical properties, including direct bandgap in the bulk and a layered crystalline structure, consisting of close-packed Pb atoms sandwiched between two layers of Iodine atoms [1]. Compared to the widely-studied TMDCs, 2D PbI2 is a halide semiconductors with a larger visible bandgap (Eg ∼ 2.4 eV) which endows its distinct optical properties. Despite being extensively studied in its bulk form and being used as a precursor for perovskite materials, the recently developed PbI2 nanosheets have shown a great promise for high-performance optoelectronic devices, such as flexible photodetectors [2] and nanolasers [3]. However, such novel applications of PbI2 nanosheets require careful characterization of their crystalline structure, thickness, strain and nonlinearity. Here we deploy a nonlinear optical microscopy as a non-invasive technique to investigate PbI2 nanosheets and fully determine their crystalline properties. To achieve such complete characterisation we analyse the polarisation, thickness and strain dependence of the second harmonic generation (SHG) and third harmonic generation (THG) from solution-grown PbI2 nanosheets. Our experimental results are also compared with numerical simulations of the conversion efficiency of the nonlinear harmonic generation with different thickness and wavelength, revealing the influence of the layered crystalline structure. Our measurements allow, for the first time, to precisely determine their thickness, crystalline orientation and strain with a non-invasive optical technique.
Two-dimensional semiconductors such as monolayer transition metal dichalcogenides (TMDs) exhibits remarkable optical properties such as robust valley polarization, making them ideal for optoelectronic and valleytronic devices. Manipulating the valley polarization by optical method is the key to realize valleytronic devices. Here, we demonstrate a resonant plasmonic nanostructure designed to spatially separate the emissions from different valleys of the WSe2 monolayer at cryogenic temperature. By changing the helicity of excitation, we show the directionality control of valley-based emission. Our hybrid nanostructure exhibits the possibility to realise the valleytronic devices.
We demonstrate enhanced second -harmonic generation from a single -crystal transition-metal-dichalcogenide metasurface of high refractive index. By manipulating the Mie-resonances at the second -harmonic wavelength, we show the control of intensity and radiation of the second -harmonic signal.
The development of a miniaturised device that provides efficient beam manipulation with high transmittance is extremely desirable for the broad range of applications including holography, metalens, and imaging. Recently, the potential of dielectric metasurfaces has been unleashed to efficiently manipulate the beam with full 2π-phase control by overlapping the electric and magnetic dipole resonances. However, in the visible range for available materials, it comes with the price of higher absorption that reduces efficiency. Here, we have considered dielectric amorphous silicon (a-Si) nanodisk and engineered them in such a way which provides minimal absorption loss in the visible range. We have experimentally demonstrated meta-deflector with high transmittance which operates in the visible wavelengths. The supercell of proposed meta-deflector consists of 15 amorphous silicon nanodisks numerically shows the transmission efficiency of 95% and deflection efficiency of 95% at operating wavelength of 715 nm. However, experimentally measured transmission and deflection efficiencies are 83% and 71%, respectively, having the experimental deflection angle of 8.40°. Nevertheless, by reducing the supercell length, the deflection angle can be controlled, and the value 15.50° was experimentally achieved using eight disks supercell. Our results suggest a new way to realise the highly transmittance metadevice with full 2π-phase control operating with the visible light which could be applicable in the imaging, metalens, holography, and display applications.