FemtoLux 3

The interaction of surface acoustic waves (SAWs) with liquids enables the production of aerosols with adjustable droplet sizes in the micrometer range expelled from a very compact source. Understanding the nonlinear acousto-hydrodynamics of SAWs with a regulated micro-scale liquid film is essential for acousto-microfluidics platforms, particularly aerosol generators. In this study, we demonstrate the presence of micro-cavitation in an MHz-frequency SAW aerosol generation platform, which is touted as a leap in aerosol technology with versatile application fields including biomolecule inhalation therapy, micro-chromatography and spectroscopy, olfactory displays, and material deposition. Using analysis methods with high temporal and spatial resolution, we demonstrate that SAWs stabilize spatially arranged liquid micro-domes atop the generator’s surface. Our experiments show that these liquid domes become acoustic resonators with highly fluctuating pressure amplitudes that can even nucleate cavitation bubbles, as supported by analytical modeling. The observed fragmentation of liquid domes indicates the participation of three droplet generation mechanisms, including cavitation and capillary-wave instabilities. During aerosol generation, the cavitation bubbles contribute to the ejection of droplets from the liquid domes and also explain observed microstructural damage patterns on the chip surface eventually caused by cavitation-based erosion.

Alterations in collagen ultrastructure between human gastric adenocarcinoma and normal gastric tissue were investigated using polarization-resolved second harmonic generation (PSHG) microscopy. Cylindrical and trigonal symmetries were assumed to extract quantitative PSHG parameters, ρ, κ and S, from each image pixel. Statistically significant variations in these values were observed for gastric adenocarcinoma, indicating a higher disorder of collagen. Numerical focal volume simulations of crossing fibrils indicate increased S parameter is due to more intersecting collagen fibrils of varying diameters. These parameters were also able to distinguish between different grades of gastric adenocarcinoma indicating that PSHG may be useful for automated cancer diagnosis.

We have demonstrated the production of laser bulk nanobubbles (BNB) with ambient radii typically below 500 nm. The gaseous nature of the nanometric objects was confirmed by a focused acoustic pulse that expands the gas cavities to a size that can be visualized with optical microscopy. The BNBs were produced on demand by a collimated high-energy laser pulse in a “clean” way, meaning that no solid particles or drops were introduced in the sample by the generation method. This is a clear advantage relative to the other standard BNB production techniques. Accordingly, the role of nanometric particles in laser bubble production is discussed. The characteristics of the nanobubbles were evaluated with two alternative methods. The first one measures the response of the BNBs to acoustic pulses of increasing amplitude to estimate their rest radius through the calculation of the dynamics Blake threshold. The second one is based on the bubble dissolution dynamics and the correlation of the bubble’s lifetime with its initial size. The high reproducibility of the present system in combination with automated data acquisition and analysis constitutes a sound tool for studying the effects of the liquid and gas properties on the stability of the BNBs solution.

Second harmonic generation (SHG) microscopy is a commonly used technique to study the organization of collagen within tissues. However, individual collagen fibrils, which have diameters much smaller than the resolution of most optical systems, have not been extensively investigated. Here we probe the structure of individual collagen fibrils using polarization-resolved SHG (PSHG) microscopy and atomic force microscopy. We find that longitudinally polarized light occurring at the edge of a focal volume of a high numerical aperture microscope objective illuminated with linearly polarized light creates a measurable variation in PSHG signal along the axis orthogonal to an individual collagen fibril. By comparing numerical simulations to experimental data, we are able to estimate parameters related to the structure and chirality of the collagen fibril without tilting the sample out of the image plane, or cutting tissue at different angles, enabling chirality measurements on individual nanostructures to be performed in standard PSHG microscopes. The results presented here are expected to lead to a better understanding of PSHG results from both collagen fibrils and collagenous tissues. Further, the technique presented can be applied to other chiral nanoscale structures such as microtubules, nanowires, and nanoribbons.

Cell-sized giant unilamellar vesicles (GUVs) are an ideal tool for understanding lipid membrane structure and properties. Label-free spatiotemporal images of their membrane potential and structure would greatly aid the quantitative understanding of membrane properties. In principle, second harmonic imaging is a great tool to do so, but the low degree of spatial anisotropy that arises from a single membrane limits its application. Here, we advance the use of wide-field high throughput SH imaging by SH imaging with the use of ultrashort laser pulses. We achieve a throughput improvement of 78% of the maximum theoretical value and demonstrate subsecond image acquisition times. We show how the interfacial water intensity can be converted into a quantitative membrane potential map. Finally, for GUV imaging, we compare this type of nonresonant SH imaging to resonant SH imaging and two photon imaging using fluorophores.

Higher-order optical harmonics entered the realm of nanostructured solids being observed recently in optical gratings and metasurfaces with a subwavelength thickness. Structuring materials at the subwavelength scale allows us toresonantly enhance the efficiency of nonlinear processes and reduce the size of high-harmonic sources. We report the observation of up to a seventh harmonic generated from a single subwavelength resonator made of AlGaAs material. This process is enabled by careful engineering of the resonator geometry for supporting an optical mode associated with a quasi-bound state in the continuum in the mid-infrared spectral range at around λ = 3.7 μm pump wavelength. The resonator volume measures ~0.1 λ³. The resonant modes are excited with an azimuthally polarized tightly focused beam. We evaluate the contributions of perturbative and nonperturbative nonlinearities to the harmonic generation process. Our work proves the possibility to miniaturize solid-state sources of high harmonics to the subwavelength volumes.

Crystalline maltodextrin particles (CMPs) were investigated using polarization-sensitive second harmonic generation (PSHG) microscopy to determine changes in their crystalline organization due to crystal type (A- and B-type) and hydration for application as starch model systems. Optimization of their synthesis resulted in intense SHG emission, exceeding maize starch granules. PSHG data showed that CMPs have a radial macrostructure with respect to their nucleation regions, fitted ρ values of 2-6, and some similar hydration variations, mimicking starch granules and validating that CMPs may be used as a model system for improved understanding of the SHG properties and applications of starch granules.

Lead halide perovskites are widely employed in photonic and light-emitting devices because of their rich optoelectronic properties and simplicity of fabrication based on low-cost flexible technologies. Perovskite bulk crystals and films demonstrate outstanding nonlinear characteristics with large optical nonlinearities exceeding the nonlinear susceptibilities of conventional semiconductor materials by several orders of magnitude. One of the promising approaches for further enhancement of the nonlinear response of perovskites as dielectric photonic materials is to employ optical resonances of structured surfaces, or metasurfaces. Nonlocal metasurfaces supporting lattice modes over many unit cells provide a new approach to both spatial and spectral control of light fields, and they may deliver improved characteristics of nonlinear effects for a wide range of applications associated with broadband excitation of multiple high-quality resonances. Here we report on the first observation of enhanced fifth harmonic generation in MAPbBr3 halide perovskite nonlocal metasurfaces driven by high-quality resonances at the generated harmonic wavelength in the visible frequency range. The demonstrated enhancement is about 2 orders of magnitude compared to an unpatterned MAPbBr3 film of the same thickness, and is broadband by virtue of the excitation of multiple resonant modes in the highly nonlocal regime. Our work suggests a novel approach for achieving parametric processes in resonant dielectric structures with high efficiency.

In biology, release of Ca²⁺ ions in the cytosol is essential to trigger or control many cell functions. Calcium signaling acutely depends on lipid membrane permeability to Ca²⁺. For proper understanding of membrane permeability to Ca²⁺, both membrane hydration and the structure of the hydrophobic core must be taken into account. Here, we vary the hydrophobic core of bilayer membranes and observe different types of behavior in high-throughput wide-field second harmonic imaging. Ca²⁺ translocation is observed through mono-unsaturated (DOPC:DOPA) membranes, reduced upon the addition of cholesterol, and completely inhibited for branched (DPhPC:DPhPA) and poly-unsaturated (SLPC:SLPA) lipid membranes. We propose, using molecular dynamics simulations, that ion transport occurs through ion-induced transient pores, which requires nonequilibrium membrane restructuring. This results in different rates at different locations and suggests that the hydrophobic structure of lipids plays a much more sophisticated regulating role than previously thought.

High-index dielectric subwavelength structures and metasurfaces are capable of enhancing light-matter interaction by orders of magnitude via geometry-dependent optical resonances. This enhancement, however, comes with a fundamental limitation of a narrow spectral range of operation in the vicinity of one or few resonant frequencies. Here we tackle this limitation and introduce an innovative and practical approach to achieve spectrally tunable enhancement of light-matter interaction with resonant metasurfaces. We design and fabricate {\it resonance-gradient metasurfaces} with varying geometrical parameters that translate into resonant frequencies dependence on one of the coordinates of the metasurface. The metasurfaces are composed of bone-like nanoresonators which are made of germanium, and they support high-Q optical resonances in the mid-IR spectral range. We apply this general concept to observe the resonant enhancement of the 3rd and 5th harmonics generated from the gradient metasurfaces being used in conjunction with a tunable excitation laser to provide a wide spectral coverage of resonantly-enhanced tunable generation of multiple optical harmonics.