Second Harmonic Generation Signal Research Articles

#3197 A NOVEL INVESTIGATION OF AVF WITH A SECOND HARMONIC GENERATION MICROSCOPY IN PATIENTS WITH END STAGE RENAL DISEASE

Abstract Background and Aims The population of patients with end-stage renal disease is rapidly growing and hemodialysis (HD) remains the most common treatment option. In clinical practice, the formation of arteriovenous fistulas (AVFs) is considered a priority in order to ensure optimal vascular access for HD patients. One of the complications in the formation of AVF is the hyperplasia of the neointimal layer of the vein, which leads to the failure of the fistula. The impact of the arrangement of collagen fibers in the veins of AVFs is little studied and opens wide opportunities for investigations. The structural tissue can be imaged with polarimetric nonlinear microscopy. Collagen fibers have a non-centrosymmetric structure, so they can be effectively imaged by second harmonic generation (SHG) microscopy [1]. The polarimetric nonlinear microscopy, exploiting the multidimentional tensor nature of light-matter interactions, is emerging as a valuable research tool in biomedical investigations and applications to digital pathology, and is only now becoming technically feasible for potential clinical translation [2,3]. This proposal represents a novel application of multimodal polarimetric nonlinear microscopy in histopathology, and biomedical imaging. The aim of this study is to determine the influence of the arrangement of collagen fibers in veins on the formation efficiency of AVFs by using the innovative method of nonlinear SHG microscopy. Method In this prospective study, we first used a novel SHG microscopy method to investigate AVFs venous intima hyperplasia. V. Cephalica segment is being obtained during arteriovenous fistula formation surgery from patients with end stage renal disease and after the removal of aneurysmatic or fibrotic AVF. Cross-sections of venous specimens are being fixed in 10% buffered formalin and stained with hematoxylin and eosin (H&E). Further, sample investigation is being performed in Laser Research Centre, Vilnius University using a home-built multiphoton laser-scanning microscope. The investigation is being performed with the permission of Lithuanian Biomedical Research Ethics Committee. Results We determined the arrangement of collagen fibers in veins before AVF formation and after the removal of aneurysmatic AVFs. It was observed that tunica intima of V. Cephalica is dominated both by endothelial cells and connective tissue made up of high-density collagen fibers. Whereas tunica adventitia consists mainly of collagen fibers. Collagen in tunica intima and adventitia are found to be highly noncentrosymmetric. Thus a strong SHG signal, resulting in high-contrast structural visualization of the V. Cephalica segment is generated. Conclusion Our initial investigations of AVF show clearly visible collagen fibers. The future work will focus on the structural changes of collagen fibers in the vein intimal hyperplasia. Further investigations need to be done to create artificial intelligence-based identification of new predictive collagen markers.

Interference tunable second harmonic generation for two-dimensional materials in layered structures.

We experimentally study the tunability of second harmonic generation (SHG) from a two-dimensional (2D) material in a 2D material/dielectric film/substrate layered structure. Such tunability arises from two interferences: one is between the incident fundamental light and its reflected light, and the other is between the upward second harmonic (SH) light and the reflected downward SH light. When both interferences are constructive, the SHG is maximally enhanced; it becomes attenuated if either of them is destructive. The maximal signal can be obtained when both interferences are perfectly constructive, which can be realized by choosing a highly reflective substrate and an appropriate thickness for a dielectric film that has a large difference in its refractive indices at the fundamental and the SH wavelengths. Our experiments demonstrate variations of three orders of magnitude in the SHG signals from a monolayer MoS2/TiO2/Ag layered structure.

Differentiating Morphea from Lichen Sclerosus by Using Multiphoton Microscopy Combined with U-Net Model for Elastic Fiber Segmentation.

This paper describes a methodology to differentiate morphea from lichen sclerosus based on examination with multiphoton microscopy (MPM) composed of two-photon excited fluorescence (TPEF) and second harmonic generation (SHG). Subcellular-resolution images were acquired by MPM from unstained lesion tissues then process spectral analysis to quantify the TPEF and SHG signals. Moreover, U-Net was employed to segment elastic fiber in TPEF images to combine with collagen fiber in SHG images for precise fiber quantification. Predictions of segmentation showed excellent performance on several evaluation indicators. The mIoU, mPA, and F1 score reach 0.8516, 0.9281, and 0.941. The quantitative analysis demonstrated the increase of collagen fibers in morphea compared to that in lichen sclerosus cases. Meanwhile, the great diminution of elastic fiber in the dermis of lichen sclerosus was depicted based on MPM imaging. Thus, MPM was comparable to the histopathological examination and our experimental results accurately distinguish between morphea and lichen sclerosus. This article is protected by copyright. All rights reserved.

Enhanced nonlinearities in hybrid structure based on nanoporous membrane and a metallohelicate with promising application in nanophotonics and NLO.

The main purposes of this work are designing new hybrid structures based on alumina nanoporous membranes with specific metallosupramolecular structure as well as studies of their usefulness in nonlinear optics (NLO). The NLO studies of the hybrid material is performed on the basis of two methods: the first by the Maker fringe technique, where the second harmonic generation (SHG) signal is recorded by rotating the sample; and the second by SHG imaging microscopy, where the SHG signal is collected point by point on the sample surface. The enhanced SHG signals were obtained without the use of the corona poling method needed during the experiment on thin films in our previous works and clearly shows the efficiency of hybrid materials based on nanoporous membranes as promising materials in devices developed based on NLO.

Strong second-harmonic generation by sublattice polarization in non-uniformly strained monolayer graphene

Despite the potential of graphene for building a variety of quantum photonic devices, its centrosymmetric nature forbids the observation of second harmonic generation (SHG) for developing second-order nonlinear devices. To activate SHG in graphene, extensive research efforts have been directed towards disrupting graphene’s inversion symmetry using external stimuli like electric fields. However, these methods fail to engineer graphene’s lattice symmetry, which is the root cause of the forbidden SHG. Here, we harness strain engineering to directly manipulate graphene’s lattice arrangement and induce sublattice polarization to activate SHG. Surprisingly, the SHG signal is boosted 50-fold at low temperatures, which can be explained by resonant transitions between strain-induced pseudo-Landau levels. The second-order susceptibility of strained graphene is found to be larger than that of hexagonal boron nitride with intrinsic broken inversion symmetry. Our demonstration of strong SHG in strained graphene offers promising possibilities for developing high-efficiency nonlinear devices for integrated quantum circuits.

Observing soft x-ray magnetization-induced second harmonic generation at a heterojunction interface

Second harmonic generation (SHG) spectroscopy in the visible and infrared regions has been a useful tool to selectively probe electronic properties at surfaces and interfaces. By examining variation of SHG under a magnetic field, one can also evaluate magnetic properties at the surfaces/interfaces. When multiple elements are involved in SHG, however, it is difficult to separate their contributions. In order to meet the demand of studying increasingly complex magnetic multilayer materials, element selectivity is desired. Here, using an Fe-based multilayer sample with broken inversion symmetry, we present observation of magnetization-induced SHG in the soft x-ray regime around the Fe M-shell absorption edge. Significant variation of SHG signal was captured depending on the direction of the magnetic moment, assuring sensitivity of the measurement likely enhanced by the Fe M-edge inner-shell resonance. The present methodology paves the way for element specific studies of magnetic properties at buried interfaces.

Large Spontaneous Polarization Ferroelectric Property, Switchable Second-Harmonic Generation Responses, and Magnetism in an Fe-Based Compound.

Since the switchable spontaneous polarization of ferroelectric materials endows it with many useful properties such as a large pyroelectric coefficient, switchable spontaneous polarization, and semiconductor, it has a wide range of application prospects, and the research of high-performance molecular ferroelectric materials has become a hot spot. We obtained a 0D organic-inorganic hybrid ferroelectric [(CH3)3NCH2CH2CH3]2FeCl4 (1) with well-defined ferroelectric domains and excellent domain inversion and exhibited a relatively large spontaneous polarization (Ps = 9 μC/m-2) and a Curie temperature (Tc) of 394 K. Furthermore, compound 1 belongs to the non-centrosymmetrical space group Cmc21 and has a strong second-harmonic generation signal. Interestingly, we also performed magnetic tests on 1, which confirmed that it is a magnetic material. This work provides clues for exploring the application of high-performance molecular ferroelectric materials in future multifunctional smart devices.

Polarizable Anionic Sublattices Can Screen Molecular Dipoles in Noncentrosymmetric Inorganic-Organic Hybrids.

We report the growth and photophysical characterization of two polar hybrid lead halide phases, methylenedianiline lead iodide and bromide, (MDA)Pb2I6 and (MDA)Pb2Br6, respectively. The phases crystallize in noncentrosymmetric space group Fdd2, which produces a highly oriented molecular dipole moment that gives rise to second harmonic generation (SHG) upon excitation at 1064 nm. While both compositions are isostructural, the size dependence of the SHG signal suggests that the bromide exhibits a stronger phase-matching response whereas the iodide exhibits a significantly weaker non-phase-matching signal. Similarly, fluorescence from (MDA)Pb2Br6 is observed around 630 nm below 75 K whereas only very weak luminescence from (MDA)Pb2I6 can be seen. We attribute the contrasting optical properties to differences in the character of the halide sublattice and postulate that the increased polarizability of the iodide ions acts to screen the local dipole moment, effectively reducing the local electric field in the crystals.

Terahertz-Driven Local Dipolar Correlation in a Quantum Paraelectric

Light-induced ferroelectricity in quantum paraelectrics is a new avenue of achieving dynamic stabilization of hidden orders in quantum materials. In this Letter, we explore the possibility of driving a transient ferroelectric phase in the quantum paraelectric KTaO_{3} via intense terahertz excitation of the soft mode. We observe a long-lived relaxation in the terahertz-driven second harmonic generation (SHG) signal that lasts up to 20ps at 10K, which may be attributed to light-induced ferroelectricity. Through analyzing the terahertz-induced coherent soft-mode oscillation and finding its hardening with fluence well described by a single-well potential, we demonstrate that intense terahertz pulses up to 500 kV/cm cannot drive a global ferroelectric phase in KTaO_{3}. Instead, we find the unusual long-lived relaxation of the SHG signal comes from a terahertz-driven moderate dipolar correlation between the defect-induced local polar structures. We discuss the impact of our findings on current investigations of the terahertz-induced ferroelectric phase in quantum paraelectrics.

Polarization-Independent Second Harmonic Generation in 2D Van Der Waals Kagome Nb3 SeI7 Crystals.

Second harmonic generation (SHG) of 2D crystals has been of great interest due to its advantages of phase-matching and easy integration into nanophotonic devices. However, the polarization-dependence character of the SHG signal makes it highly troublesome but necessary to match the laser polarization orientation relative to the crystal, thus achieving the maximum polarized SHG intensity. Here, it is demonstrated a polarization-independent SHG, for the first time, in the van der Waals Nb3 SeI7 crystals with a breathing Kagome lattice. The Nb3 triangular clusters and Janus-structure of each Nb3 SeI7 layer are confirmed by the STEM. Nb3 SeI7 flake shows a strong SHG response due to its noncentrosymmetric crystal structure. More interestingly, the SHG signals of Nb3 SeI7 are independent of the polarization of the excitation light owing to the in-plane isotropic arrangement of nonlinear active units. This work provides the first layered nonlinear optical crystal with the polarization-independent SHG effect, providing new possibilities for nonlinear optics.

Intercalating-induced second-harmonic generation in centrosymmetric multilayer graphene

Second-harmonic generation (SHG) is a nonlinear optical process, where two incident photons coherently combine into one photon with double the energy, which is important for laser frequency conversion. Graphene has huge potential in various on-chip optical applications including laser sources, waveguide structures, and detection-sensitive units. However, efficient SHG is commonly present in systems with broken inversion symmetry but absent from centrosymmetric structures such as graphene. The study of graphene SHG signal has gradually become a hot research topic. In our work, H2SO4-intercalation tunable method was developed to tune the lattice distortion of multilayer graphene and lead to charge transfer from graphene layers to H2SO4 molecules. Thus, noncentrosymmetric electric dipoles can be acquired and enhance SHG response. Furthermore, the change of SHG is reversible after deintercalation, because the lattice distortion can be restored. Our research on the intercalating-induced SHG effect may lead to a better design of graphene-based nonlinear optical devices in the future.

Field-induced second-harmonic generation induced by distorted soft chiral crystal

The nonlinear optical response of soft chiral crystal system-blue-phase (BP) liquid crystals was studied experimentally using a second-harmonic-generation (SHG) microscope. With the aid of the SHG microscope (SHM), the internal coupling between the polarization and structural deformation was visualized in a short time. In this study, a fringing field, formed at the electrode edges, causes lattice deformation of the cubic BPs, which contributes to the flexoelectric-optic response and field-induced SHG at low frequencies. Using the SHM, we can observe the spatial distribution of the induced polarization in the BPs, and the mean SHG intensity of the cubic BP depends quadratically on the strength of the electric field at a lower value. As the applied electric field increases, the structure of the BPs transfers to the chiral nematic phase (N*), and then the SHG intensity remains constant. Compared to the mean intensities of the SHG signal in N* and the different BPs in the low electric field, the SHG signal caused by the lattice deformation in BPs is weaker in N* and depends on the cubic structure of the BPs. The experimental results demonstrate that through the SHM, the influence of the inhomogeneous electric field on the BPs can be exhibited clearly because the response of the SHG signal in BPs is sensitive to field-induced lattice deformation and phase transitions between the BPs and chiral nematic. This will help us elucidate the mechanism of the secondary electro-optical response in BPs and for further improvement and development of high-performance photonic devices using BPs.

Second harmonic generation in air-exposed few-layer black phosphorus

Black phosphorus (BP) shows significant saturable absorption and other unique properties in nonlinear optical effects, and it can be used for nonlinear optical elements and other photonic devices. However, the second harmonic generation (SHG) emission is prohibited due to its inversion symmetry. Here we report emerging SHG emission in BP by exposing BP to oxygen so as to break the inversion symmetry. The intensity of SHG signal shows a dependence on thickness and exposure time. It is interesting to find that the thinner BP flakes have faster SHG intensity change rate. Our results demonstrate that the intensity of SHG signal is attributed to oxidation degree. Air exposure also causes a blue shift of photoluminescence (PL) peaks, which is consistent with our calculation results. Our study demonstrates a feasible approach to modulate the SHG emission of BP, which may provide insights to other inversion symmetric crystals like BP. • We report emerging SHG emission in BP by exposing BP to oxygen so as to break the inversion symmetry. • It is founded that the intensity of SHG signal shows a dependence on thickness and exposure time. • It is founded that air exposure causes a blue shift of PL peaks, which is consistent with our calculation results. The results demonstrate that the intensity of SHG signal is attributed to oxidation degree. • To the best of our knowledge, there is no report on the SHG in BP before. This work demonstrates a feasible approach to modulate the SHG emission of BP, which may provide insights to other inversion symmetric crystals like BP.

Non-invasive monitoring of microbial triterpenoid production using nonlinear microscopy techniques.

Introduction: Bioproduction of plant-derived triterpenoids in recombinant microbes is receiving great attention to make these biologically active compounds industrially accessible as nutraceuticals, pharmaceutics, and cosmetic ingredients. So far, there is no direct method for detecting triterpenoids under physiological conditions on a cellular level, information yet highly relevant to rationalizing microbial engineering. Methods: Here, we show in a proof-of-concept study, that triterpenoids can be detected and monitored in living yeast cells by combining coherent anti-Stokes Raman scattering (CARS) and second-harmonic-generation (SHG) microscopy techniques. We applied CARS and SHG microscopy measurements, and for comparison classical Nile Red staining, on immobilized and growing triterpenoid-producing, and non-producing reference Saccharomyces cerevisiae strains. Results and Discussion: We found that the SHG signal in triterpenoid-producing strains is significantly higher than in a non-producing reference strain, correlating with lipophile content as determined by Nile red staining. In growing cultures, both CARS and SHG signals showed changes over time, enabling new insights into the dynamics of triterpenoid production and storage inside cells.

Magnetic Fano resonance enhanced second-harmonic generation in chiral hybrid bismuth halides

Magnetic Fano resonance provides a potential opportunity to control both linearity and nonlinearity of light for their low radiation loss and near-field enhancement. Previous investigations have demonstrated its significant enhancement of nonlinearity in a plasmonic structure and the 2D materials coupled to it. In this work, the enhancement of second harmonic generation (SHG) of hybrid bismuth halides at the important communication wavelength of 1550 nm with a magnetic Fano dip is theoretically studied. To this end, a hybrid system composed of two asymmetric silver square split rings (SSRs) and this chiral perovskite film is designed. The simulation results show that magnetic Fano-like resonance is induced at the destructive interface of two magnetic modes in the SSR dimer, which can be inherited to hybrid bismuth halides, thereby leading to the increase of four orders of magnitude in its SH near-field enhancement factor. With a peak intensity of 0.16 GW cm−2, the composite structure features a high SHG conversion efficiency of up to 1.6 × 10−3 at the Fano resonance position. By rotating the polarization angle of fundamental optical excitation, the emitted SHG signal is switched on–off. Our research provides a valuable thought for enhancing the nonlinear optical process of the perovskite films by coupling the magnetic modes.

Tuning of Second-Harmonic Generation in Zn-Based Metal–Organic Frameworks by Controlling the Structural Interpenetrations: A First-Principles Investigation

To explain the huge difference in the second harmonic generation (SHG) response of two novel interpenetrated metal–organic frameworks (MOFs) that consist of Zn2+ ions coordinated to the trans-2-(4-pyridyl)-4-vinylbenzoate (pvb) ligand, eightfold interpenetrated Zn(pvb)2 (M1) and sevenfold interpenetrated [Zn(pvb)2]·DMF (M2), first-principles calculations were performed to study the geometries, band structures, and various linear and second-order nonlinear optical properties of M1 and M2 and two other hypothetical Zn-MOFs. Our results indicate that the structural transformation from M2 to M1 by the loss of the DMF guest is energetically favorable, and the M1 compound with the most tightly packed structure has the largest dielectric constant. For MOFs with the same order of interpenetration, the presence of the DMF guest has a small effect on the optical anisotropy of the system. Due to the different coordination environments of two kinds of Zn atoms, eightfold interpenetrated M1 shows more significant optical anisotropy than M2, and correspondingly, the range of phase matchability of M1 (>863 nm) is wider than that of M2 (>1126 nm). This means that at an experimental wavelength of 950 nm, M1 has a favorable phase-matching feature and displays strong SHG response, while the phase-mismatched behavior of M2 with sevenfold interpenetration leads to a weak SHG signal. Therefore, the difference in the interpenetrated structure induced by the guest DMF solvent is the main reason for the giant deviation in SHG intensity between M1 and M2 compounds. The present work provides new insights into how the phase-matching ability can be tuned by switching of the degree of interpenetration to enhance SHG response of MOFs.

Intermolecular interactions enhanced second harmony generation of iridium complex for bio-labeling

Second harmonic generation (SHG) microscopy avoids the inherent drawbacks of traditional fluorescent probes and brings a major breakthrough in live cell imaging. However, not all ordered non-centrosymmetric matter has the ability to generate SHG signals due to the different modes of intermolecular interaction. Here, we designed a non-centrosymmetric metal iridium complex (Ir-SHG) and obtained single crystals with two different intermolecular interaction modes in red (Ir-R) and yellow (Ir-Y), in which Ir-Y was shown to acquire a significant SHG effect. Interestingly, the SHG imaging of Ir-SHG exhibits high imaging signal-to-ratio (SNR) and brightness, as well as can be used in combination with a large number of fluorophores without signal cross-talk. We believe this work brings new insights into the development of SHG materials for multimodal nonlinear optical imaging.

Fast polarization-sensitive second-harmonic generation microscopy based on off-axis interferometry.

We propose polarization-sensitive second-harmonic generation microscopy based on off-axis interferometry (OI-PSHG) by recording the complex field of a wide-field second-harmonic generation (SHG) image and performing polarization measurements. With the ability to record the SHG signals associated with different positions simultaneously, the proposed method exhibits a higher imaging frame rate than raster scanning-based SHG microscopy. The molecular orientation (in terms of their symmetric axis) of tendon collagen fibrils and myosin in muscle is resolved in three dimensions from a subset of polarization-resolved SHG holograms. With the present configuration, it takes approximately 0.01 s to acquire an image with 128 × 128 pixels, which is mainly limited by the excitation power density for wide-field illumination. For the same data throughput using pixel-by-pixel scanning, 0.16-s-long acquisition is required, with the pixel dwell time of 10 µs. Offering the ability to perform wide-field imaging and polarization measurements, the present work lays the foundation for fast SHG microscopy using complex deconvolution and harmonic tomography.

Controlled Self-assembly of Gold(I) Complexes by Multiple Kinetic Aggregation States with Nonlinear Optical and Waveguide Properties.

Introduction of multiple kinetic aggregation states (Aggs) into the self-assembly pathway could bring complexity and flexibility to the self-assemblies, which is difficult to realize due to the delicate equilibria established among different Aggs bonded by weak noncovalent interactions. Here, we describe a series of chiral and achiral d10 AuI bis(N-heterocyclic carbene, NHC) complexes, and the achiral complex could undergo self-assembly with multiple kinetic Aggs. Generation of multiple kinetic Aggs was realized by applying chiral or achiral seeds exhibiting large differences in elongation temperatures for their respective cooperative self-assembly processes. We further showed that the chiral AuI self-assemblies having non-centrosymmetric packing forms exhibit nonlinear optical response of second harmonic generation (SHG), while the SHG signal is absent in the achiral analogue. The crystalline achiral AuI self-assemblies could function as optical waveguides with strong emission polarization.

Controlled Self‐assembly of Gold(I) Complexes by Multiple Kinetic Aggregation States with Nonlinear Optical and Waveguide Properties

AbstractIntroduction of multiple kinetic aggregation states (Aggs) into the self‐assembly pathway could bring complexity and flexibility to the self‐assemblies, which is difficult to realize due to the delicate equilibria established among different Aggs bonded by weak noncovalent interactions. Here, we describe a series of chiral and achiral d10 AuI bis(N‐heterocyclic carbene, NHC) complexes, and the achiral complex could undergo self‐assembly with multiple kinetic Aggs. Generation of multiple kinetic Aggs was realized by applying chiral or achiral seeds exhibiting large differences in elongation temperatures for their respective cooperative self‐assembly processes. We further showed that the chiral AuI self‐assemblies having non‐centrosymmetric packing forms exhibit nonlinear optical response of second harmonic generation (SHG), while the SHG signal is absent in the achiral analogue. The crystalline achiral AuI self‐assemblies could function as optical waveguides with strong emission polarization.