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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.

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.

In this work, full-field detection of laser-induced ultrasound waves was performed with an off-axis LED-based Schlieren system. Sensing strobe light, pulsed laser dual light-sheet excitation, and CMOS sensor device were all synchronized to capture the pressure wave as it propagated through an elastic liquid surrounding the test sample. In addition, a reconstruction algorithm based on the Radon transform was applied to the digitally recorded field in order to obtain an image of the photoacoustic source. The proposed system is capable of retrieving the profile of cylindrical and hexagonal targets.

Abstract Although efficient light delivery is required for various biomedical applications, the high stiffness of traditional silica-based optical fibers limits their in vivo usage. In this study, highly deformable and stretchable soft optical fibers are prepared based on the mechanically tough hydrogels of a double network (DN) structure comprising covalently crosslinked acrylamide and ionically crosslinked alginate using a microfluidic device. Owing to the optimized chemical composition, the core/cladding structure, and the mechanical robustness of the prepared hydrogel optical fibers, highly efficient optical delivery is achieved even at highly deformed and elongated states. Furthermore, the microfluidic device further allowed the formation of dual-core, novel architectures for hydrogel optical fibers. With the aid of the dopamine moiety included in the cladding, the hydrogel optical fibers attached strongly to all surfaces tested. Light delivery is further confirmed by implantation in the biological tissues. The high light-guiding performance of the developed hydrogel optical fibers enables them to replace the conventional silica optical fibers used in UV/Vis, fluorescence, and photoacoustic spectroscopies. To demonstrate their in vivo fiber-optic application potential, they are placed inside mice, and the excitation and emission of the generated fluorescence signals are detected.

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.

A computational and experimental study is conducted to examine how directivity associated with a finite aperture sensor affects photoacoustic tomography (PAT) image reconstruction. Acoustic signals for the simulation work were computed using a discrete particle approach from three numerical phantoms including a vasculature. The theoretical framework and a Monte Carlo approach for construction of a tissue configuration are discussed in detail. While simulating forward data, the directivity of the sensor was taken into account. The image reconstruction was accomplished using system matrix based methods like l₂ norm Tikhonov regularization, l₁ norm regularization and total variation (TV) minimization. Accordingly, two different system matrices were constructed- (i) assuming transducer as a point detector (PD) and (ii) retaining properties of a finite detector with directivity (FDWD). Image reconstruction was also performed utilizing experimentally measured PA signals. Both the computational and experimental results demonstrate that blur-free PAT imaging can be achieved with the FDWD method. Additionally, TV minimization provides marginally better image reconstruction compared to the other schemes.

Near-infrared photoacoustic imaging (NIR-PAI) combines the advantages of optical and ultrasound imaging to provide anatomical and functional information of tissues with high resolution. Although NIR-PAI is promising, its widespread use is hindered by the limited availability of NIR contrast agents. J-aggregates (JA) made of indocyanine green dye (ICG) represents an attractive class of biocompatible contrast agents for PAI. Here, we present a facile synthesis method that combines ICG and ICG-azide dyes for producing contrast agents with tunable size down to 230 nm and direct functionalization with targeting moieties. The ICG-JA platform has a detectable PA signal in vitro that is two times stronger than whole blood and high photostability. The targeting ability of ICG-JA was measured in vitro using HeLa cells. The ICG-JA platform was then injected into mice and in vivo NIR-PAI showed enhanced visualization of liver and spleen for 90 min post-injection with a contrast-to-noise ratio of 2.42.