Roadmap on Label-Free Super-Resolution Imaging.

Label-free super-resolution (LFSR) imaging relies on light-scattering processes in nanoscale objects without a need for fluorescent (FL) staining required in super-resolved FL microscopy. The objectives of this Roadmap are to present a comprehensive vision of the developments, the state-of-the-art in this field, and to discuss the resolution boundaries and hurdles which need to be overcome to break the classical diffraction limit of the LFSR imaging. The scope of this Roadmap spans from the advanced interference detection techniques, where the diffraction-limited lateral resolution is combined with unsurpassed axial and temporal resolution, to techniques with true lateral super-resolution capability which are based on understanding resolution as an information science problem, on using novel structured illumination, near-field scanning, and nonlinear optics approaches, and on designing superlenses based on nanoplasmonics, metamaterials, transformation optics, and microsphere-assisted approaches.

Thermal Control of Plasmonic Surface Lattice Resonances.

Plasmonic metasurfaces exhibiting collective responses known as surface lattice resonances (SLRs) show potential for realizing flat photonic components for wavelength-selective processes, including lasing and optical nonlinearities. However, postfabrication tuning of SLRs remains challenging, limiting the applicability of SLR-based components. Here, we demonstrate how the properties of high quality factor SLRs are easily modified by breaking the symmetry of the nanoparticle surroundings.

Cross-polarized surface lattice resonances in a rectangular lattice plasmonic metasurface.

Multiresonant metasurfaces could enable many applications in filtering, sensing, and nonlinear optics. However, developing a metasurface with more than one high-quality-factor or high-Q resonance at designated resonant wavelengths is challenging. Here, we experimentally demonstrate a plasmonic metasurface exhibiting different, narrow surface lattice resonances by exploiting the polarization degree of freedom where different lattice modes propagate along different dimensions of the lattice.

Fourier-Engineered Plasmonic Lattice Resonances.

Resonances in optical systems are useful for many applications, such as frequency comb generation, optical filtering, and biosensing. However, many of these applications are difficult to implement in optical metasurfaces because traditional approaches for designing multiresonant nanostructures require significant computational and fabrication efforts. To address this challenge, we introduce the concept of Fourier lattice resonances (FLRs) in which multiple desired resonances can be chosen and used to dictate the metasurface design.

Multiply-resonant second-harmonic generation using surface lattice resonances in aluminum metasurfaces.

Nonlinear metamaterials show potential for realizing flat nonlinear optical devices but are generally lacking in terms of achievable conversion efficiencies. Recent work has focused on enhancing nonlinear processes by utilizing high quality factor resonances, such as collective responses known as surface lattice resonances (SLRs) taking place in periodic metal nanoparticle arrays. Here, we investigate how the dispersive nature of SLRs affects the nonlinear responses of SLR-supporting metasurfaces.

Ultra-high-Q resonances in plasmonic metasurfaces.

Plasmonic nanostructures hold promise for the realization of ultra-thin sub-wavelength devices, reducing power operating thresholds and enabling nonlinear optical functionality in metasurfaces. However, this promise is substantially undercut by absorption introduced by resistive losses, causing the metasurface community to turn away from plasmonics in favour of alternative material platforms (e.g.

Backward Phase-Matched Second-Harmonic Generation from Stacked Metasurfaces.

We demonstrate phase-matched second-harmonic generation (SHG) from three-dimensional metamaterials consisting of stacked metasurfaces. To achieve phase matching, we utilize a novel mechanism based on phase engineering of the metasurfaces at the interacting wavelengths, facilitating phase-matched SHG in the unconventional backward direction. Stacking up to five metasurfaces,we obtain a phase-matched SHG signal, which scales superlinearly with the number of layers.

Hyperpolarizability of Plasmonic Meta-Atoms in Metasurfaces.

Plasmonic metasurfaces are promising as enablers of nanoscale nonlinear optics and flat nonlinear optical components. Nonlinear optical responses of such metasurfaces are determined by the nonlinear optical properties of individual plasmonic meta-atoms. Unfortunately, no simple methods exist to determine the nonlinear optical properties (hyperpolarizabilities) of the meta-atoms hindering the design of nonlinear metasurfaces.

Multiphoton microscopy of the dermoepidermal junction and automated identification of dysplastic tissues with deep learning.

Histopathological image analysis performed by a trained expert is currently regarded as the gold-standard for the diagnostics of many pathologies, including cancers. However, such approaches are laborious, time consuming and contain a risk for bias or human error. There is thus a clear need for faster, less intrusive and more accurate diagnostic solutions, requiring also minimal human intervention.

Multiresonant High- Plasmonic Metasurfaces.

Resonant metasurfaces are devices composed of nanostructured subwavelength scatterers that generate narrow optical resonances, enabling applications in filtering, nonlinear optics, and molecular fingerprinting. It is highly desirable for these applications to incorporate such devices with multiple high-quality-factor resonances; however, it can be challenging to obtain more than a pair of narrow resonances in a single plasmonic surface. Here, we demonstrate a multiresonant metasurface that operates by extending the functionality of surface lattice resonances, which are the collective responses of arrays of metallic nanoparticles.

Less Is More: Enhancement of Second-Harmonic Generation from Metasurfaces by Reduced Nanoparticle Density.

We investigate optical second-harmonic generation (SHG) from metasurfaces where noncentrosymmetric V-shaped gold nanoparticles are ordered into regular array configurations. In contrast to expectations, a substantial enhancement of the SHG signal is observed when the number density of the particles in the array is reduced. More specifically, by halving the number density, we obtain over 5-fold enhancement in SHG intensity.

Automated classification of multiphoton microscopy images of ovarian tissue using deep learning.

Histopathological image analysis of stained tissue slides is routinely used in tumor detection and classification. However, diagnosis requires a highly trained pathologist and can thus be time-consuming, labor-intensive, and potentially risk bias. Here, we demonstrate a potential complementary approach for diagnosis.

Rapid visualization of grain boundaries in monolayer MoS by multiphoton microscopy.

Grain boundaries have a major effect on the physical properties of two-dimensional layered materials. Therefore, it is important to develop simple, fast and sensitive characterization methods to visualize grain boundaries. Conventional Raman and photoluminescence methods have been used for detecting grain boundaries; however, these techniques are better suited for detection of grain boundaries with a large crystal axis rotation between neighbouring grains.

Ultra-strong polarization dependence of surface lattice resonances with out-of-plane plasmon oscillations.

The interplay between localized surface plasmon (LSP) resonances and their collective responses, known as surface lattice resonances (SLRs), in metal nanoparticle arrays can lead to resonances with high Q-factors (∼100). These responses have in the past usually been studied for LSP resonances in the plane of the array of the nanoparticles (assumed to be nonmagnetic), thus restricting efficient coupling to particles separated along a specific direction. In the present study, we demonstrate that LSPs oscillating perpendicular to the plane of the surface can lead to stronger inter-particle coupling, which enhances the SLRs.

Hybrid plasmonic lattices with tunable magneto-optical activity.

We report on the optical and magneto-optical response of hybrid plasmonic lattices that consist of pure nickel and gold nanoparticles in a checkerboard arrangement. Diffractive far-field coupling between the individual emitters of the lattices results in the excitation of two orthogonal surface lattice resonance modes. Local analyses of the radiation fields indicate that both the nickel and gold nanoparticles contribute to these collective resonances and, thereby, to the magneto-optical activity of the hybrid arrays.

Second-harmonic generation imaging of semiconductor nanowires with focused vector beams.

We use second-harmonic generation (SHG) with focused vector beams to investigate individual vertically aligned GaAs nanowires. Our results provide direct evidence that SHG from oriented nanowires is mainly driven by the longitudinal field along the nanowire growth axis. Consequently, focused radial polarization provides a superior tool to characterize such nanowires compared to linear polarization, also allowing this possibility in the native growth environment.

Polarized THG microscopy identifies compositionally different lipid droplets in mammalian cells.

Cells store excess lipids as two major compounds, triacylglycerols (TAGs) and cholesteryl esters (CEs), inside lipid droplets (LDs). The degree of lipid ordering is considered to play a major role in the mobility and enzymatic processing of lipids in LDs. Here, we provide evidence that polarized third-harmonic generation (THG) microscopy distinguishes between native TAG- and CE-enriched LDs in cells due to the different ordering of the two lipid species.

Three-dimensional winged nanocone optical antennas.

We introduce 3D optical antennas based on winged nanocones. The antennas support particle plasmon oscillations with current distributions that facilitate transformation of transverse far-field radiation to strong longitudinal local fields near the cone apices. We characterize the optical responses of the antennas by their extinction spectra and by second-harmonic generation microscopy with cylindrical vector beams.

Third- and second-harmonic generation microscopy of individual metal nanocones using cylindrical vector beams.

We demonstrate third- (THG) and second-harmonic generation (SHG) microscopy of individual silver nanocones using tightly focused cylindrical vector beams (CVBs). Although THG is expected to be a weaker process than SHG, the yield for THG with radial polarization was higher than for SHG. We also found an excellent correlation between the imaging properties of THG and SHG, suggesting that both are governed by the same overall features of the individual nanocone.

Strength retention behavior of oriented PLLA, 96L/4D PLA, and 80L/20D,L PLA.

The strength retention characteristics of oriented semicrystalline polylactides were monitored during hydrolytic degradation in vitro. The effects of the polymer type, the material's initial inherent viscosity (iv), the sample diameter and the residual monomer content on strength retention were analyzed. The analyzed polylactides had similar, but not identical, strength retention characteristics.

Analysis of the factors affecting the inherent viscosity of oriented polylactides during hydrolytic degradation.

This study focuses on analyzing the effects of several factors on the rate of decay of inherent viscosity (iv) during hydrolytic degradation. The analysis was made for oriented PLLA, 96L/4D PLA and 80L/20D,L PLA. The analyzed polymers were found to have identical rate of iv loss (P < 0.

Second-harmonic generation imaging of metal nano-objects with cylindrical vector beams.

We introduce an imaging technique based on second-harmonic generation with cylindrical vector beams that is extremely sensitive to three-dimensional orientation and nanoscale morphology of metal nano-objects. Our experiments and second-harmonic field calculations based on frequency-domain boundary element method are in very good agreement. The technique provides contrast for structural features that cannot be resolved by linear techniques or conventional states of polarization and shows great potential for simple and cost-effective far-field optical imaging in plasmonics.

A simple and high production rate manufacturing method for submicron polymer fibres.

The manufacturing technique for cotton-candy floss, heat-aided rotary jet-spinning, was used to produce submicron-scale fibrous meshes by using bioabsorbable thermoplastic polymers. The method was feasible for 100 wt% polymer concentrations functioning completely without solvents. It was possible to produce submicron diameter fibres using a simple device, which indicates that this manufacturing method is a very promising technique for obtaining high-throughput rates for submicron, and possibly nano-scale, fibrous meshes.

Tip-enhanced Raman scattering from bridged nanocones.

We present two silver nanocones separated by 450 nm, well beyond the typical gap spacing of coupled nanoantennas, and connected by a metal bridge to facilitate plasmonic coupling between them. The tip-enhanced Raman scattering from crystal violet molecules is found to be almost an order of magnitude higher from the bridged cones than from individual cones. This result is supported by local-field calculations of the two types of structures.

Nanoimprint fabrication of gold nanocones with approximately 10 nm tips for enhanced optical interactions.

We show that nanoimprint lithography combined with electron-beam evaporation provides a cost-efficient, rapid, and reproducible method to fabricate conical nanostructures with very sharp tips on flat surfaces in high volumes. We demonstrate the method by preparing a wafer-scale array of gold nanocones with an average tip radius of 5 nm. Strong local fields at the tips enhance the second-harmonic generation by over 2 orders of magnitude compared with a nonsharp reference.