Gustavo Grinblat

Enhanced Third Harmonic Generation in Single Germanium Nanodisks Excited at the Anapole Mode

We present an all-dielectric germanium nanosystem exhibiting a strong third order nonlinear response and efficient third harmonic generation in the optical regime. A thin germanium nanodisk shows a pronounced valley in its scattering cross section at the dark anapole mode, while the electric field energy inside the disk is maximized due to high confinement within the dielectric. We investigate the dependence of the third harmonic signal on disk size and pump wavelength to reveal the nature of the anapole mode. Each germanium nanodisk generates a high effective third order susceptibility of χ((3)) = 4.3 × 10(-9) esu, corresponding to an associated third harmonic conversion efficiency of 0.0001% at an excitation wavelength of 1650 nm, which is 4 orders of magnitude greater than the case of an unstructured germanium reference film. Furthermore, the nonlinear conversion via the anapole mode outperforms that via the radiative dipolar resonances by about 1 order of magnitude, which is consistent with our numerical simulations. These findings open new possibilities for the optimization of upconversion processes on the nanoscale through the appropriate engineering of suitable dielectric materials.

Giant photoluminescence enhancement in tungsten-diselenide–gold plasmonic hybrid structures

Impressive properties arise from the atomically thin nature of transition metal dichalcogenide two-dimensional materials. However, being atomically thin limits their optical absorption or emission. Hence, enhancing their photoluminescence by plasmonic nanostructures is critical for integrating these materials in optoelectronic and photonic devices. Typical photoluminescence enhancement from transition metal dichalcogenides is 100-fold, with recent enhancement of 1,000-fold achieved by simultaneously enhancing absorption, emission and directionality of the system. By suspending WSe2 flakes onto sub-20-nm-wide trenches in gold substrate, we report a giant photoluminescence enhancement of ∼20,000-fold. It is attributed to an enhanced absorption of the pump laser due to the lateral gap plasmons confined in the trenches and the enhanced Purcell factor by the plasmonic nanostructure. This work demonstrates the feasibility of giant photoluminescence enhancement in WSe2 with judiciously designed plasmonic nanostructures and paves a way towards the implementation of plasmon-enhanced transition metal dichalcogenide photodetectors, sensors and emitters.

High-Efficiency Second Harmonic Generation from a Single Hybrid ZnO Nanowire/Au Plasmonic Nano-Oligomer

We introduce a plasmonic-semiconductor hybrid nanosystem, consisting of a ZnO nanowire coupled to a gold pentamer oligomer by crossing the hot-spot. It is demonstrated that the hybrid system exhibits a second harmonic (SH) conversion efficiency of ∼3 × 10(-5)%, which is among the highest values for a nanoscale object at optical frequencies reported so far. The SH intensity was found to be ∼1700 times larger than that from the same nanowire excited outside the hot-spot. Placing high nonlinear susceptibility materials precisely in plasmonic confined-field regions to enhance SH generation opens new perspectives for highly efficient light frequency up-conversion on the nanoscale.

Efficient Third Harmonic Generation and Nonlinear Subwavelength Imaging at a Higher-Order Anapole Mode in a Single Germanium Nanodisk

Benefiting from large intrinsic nonlinearities, low absorption, and high field enhancement abilities, all-dielectric nanoantennas are considered essential for efficient nonlinear processes at subwavelength volumes. In particular, when the dielectric nanoantenna supports the nonradiating anapole mode, characterized by a minimum in the extinction cross section and a maximum electric energy within the material, third harmonic generation (THG) processes can be greatly enhanced. In this work, we demonstrate that a higher-order anapole mode in a 200 nm thick germanium nanodisk delivers the highest THG efficiency on the nanoscale at optical frequencies. By doubling the diameter of a disk supporting the fundamental anapole mode, we discover the emergence of an anapole mode of higher order, with a valley in the extinction cross section significantly narrower than that of the fundamental anapole. Under this condition, we observe a highly improved electric field confinement effect within the dielectric disk, leading to THG conversion efficiencies as large as 0.001% at a third harmonic wavelength of 550 nm. In addition, by mapping the THG emission across the nanodisk, we are able to unveil the anapole near-field intensity distributions, which show excellent agreement with numerical simulations. Our findings remarkably expand contemporary knowledge on localized modes in dielectric nanosystems, revealing crucial elements for the elaboration of highly efficient frequency upconversion nanodevices.

Bridging the Gap between Dielectric Nanophotonics and the Visible Regime with Effectively Lossless Gallium Phosphide Antennas

We present all-dielectric gallium phosphide (GaP) nanoantennas as an efficient nanophotonic platform for surface-enhanced second harmonic generation (SHG) and fluorescence (SEF), showing negligible losses in the visible range. Employing single GaP nanodisks, we observe an increase of more than 3 orders of magnitude in the SHG conversion signal in comparison with the bulk. This constitutes an SHG efficiency as large as 0.0002%, which is to the best of our knowledge the highest yet achieved value for a single nano-object in the optical region. Furthermore, we show that GaP dimers with 35 nm gap can enhance up to 3600 times the fluorescence emission of dyes located in the gap of the nanoantenna. This is accomplished by a fluorescence lifetime reduction of at least 22 times, accompanied by a high-intensity field confinement in the gap region. These results open new avenues for low-loss nanophotonics in the optical regime.

Efficient Third Harmonic Generation from Metal–Dielectric Hybrid Nanoantennas

High refractive index dielectric nanoantennas are expected to become key elements for nonlinear nano-optics applications due to their large nonlinearities, low energy losses, and ability to produce high electric field enhancements in relatively large nanoscale volumes. In this work, we show that the nonlinear response from a high-index dielectric nanoantenna can be significantly improved by adding a metallic component to build a metal-dielectric hybrid nanostructure. We demonstrate that the plasmonic resonance of a Au nanoring can boost the anapole mode supported by a Si nanodisk, strongly enhancing the electric field inside the large third-order susceptibility dielectric. As a result, a high third harmonic conversion efficiency, which reaches 0.007% at a third harmonic wavelength of 440 nm, is obtained. In addition, by suitably modifying geometrical parameters of the hybrid nanoantenna, we tune the enhanced third harmonic emission throughout the optical regime. Coupling metallic and dielectric nanoantennas to expand the potential of subwavelength structures opens new paths for efficient nonlinear optical effects in the visible range on the nanoscale.

Slow cooling and efficient extraction of C-exciton hot carriers in MoS2 monolayer.

In emerging optoelectronic applications, such as water photolysis, exciton fission and novel photovoltaics involving low-dimensional nanomaterials, hot-carrier relaxation and extraction mechanisms play an indispensable and intriguing role in their photo-electron conversion processes. Two-dimensional transition metal dichalcogenides have attracted much attention in above fields recently; however, insight into the relaxation mechanism of hot electron-hole pairs in the band nesting region denoted as C-excitons, remains elusive. Using MoS2 monolayers as a model two-dimensional transition metal dichalcogenide system, here we report a slower hot-carrier cooling for C-excitons, in comparison with band-edge excitons. We deduce that this effect arises from the favourable band alignment and transient excited-state Coulomb environment, rather than solely on quantum confinement in two-dimension systems. We identify the screening-sensitive bandgap renormalization for MoS2 monolayer/graphene heterostructures, and confirm the initial hot-carrier extraction for the C-exciton state with an unprecedented efficiency of 80%, accompanied by a twofold reduction in the exciton binding energy.

Hierarchical ZnO nanostructures: Growth mechanisms and surface correlated photoluminescence

ZnO nanowires were grown by vapor-transport and deposition on Au nanocluster covered fused and thermal silica and c-Si. The nanowire size and density depended strongly on the substrate type. By decreasing the O2 to local Zn partial pressure ratio, the growth pattern changed to nanocombs and nanosheets. ZnO nanohedgehogs were found on bare c-Si. We observe a remarkable correlation between the defect to exciton photoluminescence intensity ratio and the nanostructures specific surface areas. These results indicate that changes in strain and O deficiency defects at surfaces are behind the observed morphology changes, one to two-dimensional growth transition, and corresponding luminescence.

Luminescence and electrical properties of single ZnO/MgO core/shell nanowires

To neutralise the influence of the surface of ZnO nanowires for photonics and optoelectronic applications, we have covered them with insulating MgO film and individually contacted them for electrical characterisation. We show that such a metal-insulator-semiconductor-type nanodevice exhibits a high diode ideality factor of 3.4 below 1 V. MgO shell passivates ZnO surface states and provides confining barriers to electrons and holes within the ZnO core, favouring excitonic ultraviolet radiative recombination, while suppressing defect-related luminescence in the visible and improving electrical conductivity. The results indicate the potential use of ZnO/MgO nanowires as a convenient building block for nano-optoelectronic devices.

Homoepitaxial Growth of Large‐Scale Highly Organized Transition Metal Dichalcogenide Patterns

Controllable growth of highly crystalline transition metal dichalcogenide (TMD) patterns with regular morphology and unique edge structure is highly desired and important for fundamental research and potential applications. Here, single-crystalline MoS2 flakes are reported with regular trigonal symmetric patterns that can be homoepitaxially grown on MoS2 monolayer via chemical vapor deposition. The highly organized MoS2 patterns are rhombohedral (3R)-stacked with the underlying MoS2 monolayer, and their boundaries are predominantly terminated by zigzag Mo edge structure. The epitaxial MoS2 crystals can be tailored from compact triangles to fractal flakes, and the pattern formation can be explained by the anisotropic growth rates of the S and Mo edges under low sulfur chemical potential. The 3R-stacked MoS2 pattern demonstrates strong second and third-harmonic-generation signals, which exceed those reported for monolayer MoS2 by a factor of 6 and 4, correspondingly. This homoepitaxial growth approach for making highly organized TMD patterns is also demonstrated for WS2 .