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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.

The laser synthesis and processing of colloids represents a group of scalable and “green” synthesis methods of crystalline metal oxides, that have recently made encouraging progresses in preparing amorphous as well as defect-rich nanoparticles. The relevant conditions and mechanisms that allow the design of amorphous metal oxides (AMOs) remain unknown. Consequently, in this work the synthesis of Fe-based partially amorphous oxide nanoparticles (NPs) by pulsed laser ablation in water was studied. Furthermore, both laser pulse duration and the number of laser pulse in pulsed laser fragmentation in liquid (LFL) allow a precise control of amorphization of AMOs in water. Hereby, a high-fluence nanosecond-LFL provides a significantly higher amorphization rate, whereas picosecond-LFL always presents minor fractions of crystalline α-Fe even with a higher specific energy input and laser intensity. Consequently, the laser fluence required for the repeated melting and quenching of NP appears to be the decisive parameter to control amorphization. During laser synthesis and processing of colloids, the amorphization of AMOs appears to be linked to the apparent size reduction effect, while a complete full amorphization of AMOs may be attributed to the stronger oxidation effects. This work will stimulate future studies using laser-generated AMO NPs for further functional purposes.

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.

A new versatile patent-pending technology enabling new operation regimes and a unique set of features in the industrialgrade 30 W-level average power femtosecond hybrid laser is introduced in this work. The developed technology, based on the use of an all-in-fiber active fiber loop (AFL), enabled to form GHz bursts of ultrashort laser pulses with any desired pulse repetition rate and any number of pulses in a burst with identical intra-burst pulse separation. Furthermore, the AFL allowed to tune pulse duration from a few hundred femtoseconds to picoseconds and even up to the nanosecond range.

Laser sources which produce GHz bursts of ultrashort pulses attract a lot of attention by demonstrating superior performance in material processing. Flexibility of the laser source in a selection of parameters for custom application is highly preferable. In this work, we demonstrate a very versatile method for burst formation using the active fiber loop (AFL). It allows forming GHz bursts containing from 2 up to approximately 2200 pulses in a burst (1000 ns burst width) with identical pulse separation and any predefined intra-burst pulse repetition rate (PRR). The burst pre-shaping by the amplification conditions in the AFL and by the modulation of transmission of the acousto-optic modulator was demonstrated. Industrial-grade ultrafast laser system was able to operate in the single-pulse and GHz-burst regimes. The laser system delivered high-quality 368 fs duration (FWHM) pulses of 15.3 µJ pulse energy and 30.6 W average output power at 2 MHz PRR in the single-pulse regime. In the GHz-burst operation regime, bursts of 2.2 GHz intra-burst repetition rate were formed and amplified to more than 30 W average output power with a burst energy up to 135 µJ at a burst repetition rate of 200 kHz. The sub-picosecond duration of pulses was obtained in the GHz-burst regime at different burst widths.

Subwavelength dielectric resonators assembled into metasurfaces have become a versatile tool for miniaturizing optical components approaching the nanoscale. An important class of metasurface functionalities is associated with asymmetry in both the generation and transmission of light with respect to reversals of the positions of emitters and receivers. The nonlinear light–matter interaction in metasurfaces offers a promising pathway towards miniaturization of the asymmetric control of light. Here we demonstrate asymmetric parametric generation of light in nonlinear metasurfaces. We assemble dissimilar nonlinear dielectric resonators into translucent metasurfaces that produce images in the visible spectral range on being illuminated by infrared radiation. By design, the metasurfaces produce different and completely independent images for the reversed direction of illumination, that is, when the positions of the infrared emitter and the visible light receiver are exchanged. Nonlinearity-enabled asymmetric control of light by subwavelength resonators paves the way towards novel nanophotonic components via dense integration of large quantities of nonlinear resonators into compact metasurface designs.

The collapse of a laser-induced vapor bubble near a solid boundary usually ends in a liquid jet. When the boundary is from a soft material the jetting may pierce the liquid-solid interface and result in the injection of liquid into it. A particular impulsive jet flow can be generated when a laser pulse is focused just below the free surface of a thin liquid layer covering a gelatin sample used as a surrogate of biological tissue. Here, a downwards jet forms from a liquid splash at the free surface and then penetrates through the liquid layer into the soft boundary. In the present manuscript we report on the use of this novel jet, termed “bullet” jet, to pierce soft materials and we explore its potential to become an optical needle-free injection platform. The dynamics and depth of the injection is studied as a function of the elasticity of the solid and the liquid properties. Injections of up to 4 mm deep into 4 %w/w gelatin within 0.5 ms are observed. The advantages of the bullet jet over other kinds of impulsively generated jets with lasers are discussed.