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Results for “nonlinear optical microscopy”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Analysis of laser-induced modification of collagen structure using nonlinear optical microscopy

Nonlinear optical microscopy is used to monitor changes in the collagen structure of patellar ligament after IR laser heating up to a temperature of 60 °C. Pre-denaturation modification of the tissue matrix exhibits specific properties and consists in splitting of initially parallel fibre bundles into array of divergent fibres. Image processing employing Fast Fourier transform analysis is used for characterising images of the fibre structure and determining the collagen orientation index. An increase in manifestation of laser-induced disordering with an increase in IR laser radiation power from 0.3 to 2 W is accompanied by a decrease in the collagen orientation index. The specific disorganisation of the collagen tissue structure during laser heating is supposed to be due to fast speed and local action of the laser heating, which leads to mechanical distortions of the structural elements of tissue matrix. (paper)

36 MATERIALS SCIENCE↗
DOE OSTI2021

Nonlinear Optical Microscopy with Ultralow Quantum Light

Nonlinear optical (NLO) microscopy relies on multiple light–matter interactions to provide unique contrast mechanisms and imaging capabilities that are inaccessible to traditional linear optical imaging approaches, making them versatile tools to understand a wide range of complex systems. However, the strong excitation fields that are necessary to drive higher-order optical processes efficiently are often responsible for photobleaching, photodegradation, and interruption in many systems of interest. This is especially true for imaging living biological samples over prolonged periods of time or in accessing intrinsic dynamics of electronic excited-state processes in spatially heterogeneous materials. This perspective outlines some of the key limitations of two NLO imaging modalities implemented in our lab and highlights the unique potential afforded by the quantum properties of light, especially entangled two-photon absorption based NLO spectroscopy and microscopy. Here, we further review some of the recent exciting advances in this emerging filed and highlight some major challenges facing the realization of quantum-light-enabled NLO imaging modalities.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Correlated Materials Characterization via Multimodal Chemical and Functional Imaging

Multimodal chemical imaging simultaneously offers high-resolution chemical and physical information with nanoscale and, in select cases, atomic resolution. By coupling modalities that collect physical and chemical information, we can address scientific problems in biological systems, battery and fuel cell research, catalysis, pharmaceuticals, photovoltaics, medicine, and many others. The combined systems enable the local correlation of material properties with chemical makeup, making fundamental questions of how chemistry and structure drive functionality approachable. In this Review, we present recent progress and offer a perspective for chemical imaging used to characterize a variety of samples by a number of platforms. Specifically, we present cases of infrared and Raman spectroscopies combined with scanning probe microscopy; optical microscopy and mass spectrometry; nonlinear optical microscopy; and, finally, ion, electron, and probe microscopies with mass spectrometry. As a result, we also discuss the challenges associated with the use of data originated by the combinatorial hardware, analysis, and machine learning as well as processing tools necessary for the interpretation of multidimensional data acquired from multimodal studies.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Optical second harmonic generation in anisotropic multilayers with complete multireflection of linear and nonlinear waves using ♯SHAARP.ml package

Abstract Optical second harmonic generation (SHG) is a nonlinear optical effect widely used for nonlinear optical microscopy and laser frequency conversion. Closed-form analytical solution of the nonlinear optical responses is essential for evaluating materials whose optical properties are unknown a priori. A recent open-source code, ♯SHAARP. si , can provide such closed form solutions for crystals with arbitrary symmetries, orientations, and anisotropic properties at a single interface. However, optical components are often in the form of slabs, thin films on substrates, and multilayer heterostructures with multiple reflections of both the fundamental and up to ten different SHG waves at each interface, adding significant complexity. Many approximations have therefore been employed in the existing analytical approaches, such as slowly varying approximation, weak reflection of the nonlinear polarization, transparent medium, high crystallographic symmetry, Kleinman symmetry, easy crystal orientation along a high-symmetry direction, phase matching conditions and negligible interference among nonlinear waves, which may lead to large errors in the reported material properties. To avoid these approximations, we have developed an open-source package named Second Harmonic Analysis of Anisotropic Rotational Polarimetry in Multilayers (♯SHAARP. ml ). The reliability and accuracy are established by experimentally benchmarking with both the SHG polarimetry and Maker fringes using standard and commonly used nonlinear optical materials as well as twisted 2-dimensional heterostructures.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Generalized analytical and numerical modeling of optical second harmonic generation in anisotropic crystals and complex heterostructures using #SHAARP package

Optical second harmonic generation (SHG) is a nonlinear optical effect widely used for nonlinear optical microscopy and laser frequency conversion. The closed-form analytical solution of the nonlinear optical responses is essential for evaluating the optical responses of new materials whose optical properties are unknown a priori. Many approximations have therefore been employed in the existing analytical approaches, such as slowly varying approximation, weak reflection of the nonlinear polarization, transparent medium, high crystallographic symmetry, Kleinman symmetry, easy crystal orientation along a high-symmetry direction, phase matching conditions and negligible interference among nonlinear waves, which may lead to large errors in the reported material properties. To avoid these approximations, here we have developed an open-source package named Second Harmonic Analysis of Anisotropic Rotational Polarimetry (#SHAARP) for single interface (si) and in multilayers (ml) for homogeneous crystals. The reliability and accuracy are established by experimentally benchmarking with both the SHG polarimetry and Maker fringes predicted from the package using standard materials. SHAARP.si and SHAARP.ml are available through GitHub https://github.com/Rui-Zu/SHAARP and https://github.com/bzw133/SHAARP.ml, respectively.

complex systems↗
DOE OSTI2020

Adaptive noise canceling for transient absorption microscopy

Significance: Ultrafast fiber lasers are an attractive alternative to bulk lasers for nonlinear optical microscopy for their compactness and low cost. The high relative intensity noise (RIN) of these lasers poses a challenge for pump-probe measurements such as transient absorption and stimulated Raman scattering, along with modalities that provide label-free contrast from the vibrational and electronic structure of molecules. Aim: Digital adaptive filtering was applied to determine the applicability for canceling laser RIN in a transient absorption microscope with an ultrafast fiber laser source. Approach: Digitized signals from the transmitted probe and reference photodetectors were fed to an adaptive filter in MATLAB, running in a noise canceling configuration. This result was then fed to a software lock-in algorithm to demodulate the pump-probe signal. Images were built up one line scan at a time with a 3.5-kHz resonant scanner, with 100× averaging. The imaging target was Bi4Ge3O12, which exhibits nondegenerate two-photon absorption at the pump/probe wavelengths used (530-nm pump and 490-nm probe). Results: Without adaptive noise cancellation, the lock-in output primarily passes the laser RIN within its detection bandwidth, resulting in images that closely follow the linear transmissivity and lack sensitivity to pump-probe time delay. With adaptive noise cancellation in front of the lock-in, the RIN rejection is enough to restore the z-sectioning and sensitivity to pump-probe delay, as expected for transient absorption. Results were limited primarily by noise from the photodetector and analog-to-digital converter. Conclusions: Digital adaptive noise cancellation, even when limited by electronics noise, can recover pump-probe signals by removal of laser RIN, under conditions where averaging alone fails.

42 ENGINEERING↗
DOE OSTI2025

Quantitative Nonlinear Optical Polarimetry with High Spatial Resolution

Nonlinear optical microscopy such as in the optical second-harmonic generation (SHG) modality has become a popular tool today for probing materials in the physical and biological sciences. While imaging and spectroscopy are widely used in the microscopy mode, nonlinear polarimetry, which can shed light on materials’ symmetry and microstructure, is relatively underdeveloped. This is partly because quantitative analytical modeling of the optical SHG response for anisotropic crystals and films largely assumes low-numerical aperture (NA) focusing of light, where the plane-wave approximation is sufficient. Tight focusing provides unique benefits in revealing out-of-plane polarization responses, which cannot be detected by near-plane-wave illumination at normal incidence. Here, we outline a method for quantitatively analyzing SHG polarimetry measurements obtained under high-NA focusing within a microscope geometry. Experiments and simulations of a variety of standard samples, from single crystals to thin films, are in good agreement, including measured and simulated spatial SHG maps of ferroelectric domains. A solution to the inverse problem is demonstrated, where the spatial distribution of an SHG tensor with unknown tensor coefficient magnitudes is determined by experimentally measured polarimetry. The ability to extract the out-of-plane component of the nonlinear polarization in normal incidence is demonstrated, which can be valuable for high-resolution polarimetry of 2D materials, thin films, heterostructures, and uniaxial crystals with a strong out-of-plane response.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Spatially co-registered wide-field nonlinear optical imaging of living and complex biosystems in a total internal reflection geometry

Nonlinear optical microscopy that leverages an objective based total internal reflection (TIR) excitation scheme is an attractive means for rapid, wide-field imaging with enhanced surface sensitivity. Through select combinations of distinct modalities, one can, in principle, access complementary chemical and structural information for various chemical species near interfaces. Here, we report a successful implementation of such a wide-field nonlinear optical microscope system, which combines coherent anti-Stokes Raman scattering (CARS), two-photon fluorescence (TPF), second harmonic generation (SHG), and sum frequency generation (SFG) modalities on the same platform. The intense optical fields needed to drive these high order nonlinear optical processes are achieved through the use of femtosecond pulsed light in combination with the intrinsic field confinement induced by TIR over a large field of view. The performance of our multimodal microscope was first assessed through the experimental determination of its chemical fidelity, intensity and polarization dependences, and spatial resolution using a set of well-defined model systems. Subsequently, its unique capabilities were validated through imaging complex biological systems, including Hydrangea quercifolia pollen grains and Pantoea sp. YR343 bacterial cells. Specifically, the spatial distribution of different molecular groups in the former was visualized via vibrational contrast mechanisms of CARS, whereas co-registered TPF imaging allowed the identification of spatially localized intrinsic fluorophores. We further demonstrate the feasibility of our microscope for wide-field CARS imaging on live cells through independent characterization of cell viability using spatially co-registered TPF imaging. Overall, this approach to TIR enabled wide-field imaging is expected to provide new insights into bacterial strains and their interactions with other species in the rhizosphere in a time-resolved and chemically selective manner.

47 OTHER INSTRUMENTATION↗
DOE OSTI2017

Three-Dimensional Geometry of Collagenous Tissues by Second Harmonic Polarimetry

Collagen is a biological macromolecule capable of second harmonic generation, allowing label-free detection in tissues; in addition, molecular orientation can be determined from the polarization dependence of the second harmonic signal. Previously we reported that in-plane orientation of collagen fibrils could be determined by modulating the polarization angle of the laser during scanning. We have now extended this method so that out-of-plane orientation angles can be determined at the same time, allowing visualization of the 3-dimensional structure of collagenous tissues. This approach offers advantages compared with other methods for determining out-of-plane orientation. First, the orientation angles are directly calculated from the polarimetry data obtained in a single scan, while other reported methods require data from multiple scans, use of iterative optimization methods, application of fitting algorithms, or extensive post-optical processing. Second, our method does not require highly specialized instrumentation, and thus can be adapted for use in almost any nonlinear optical microscopy setup. It is suitable for both basic and clinical applications. We present three-dimensional images of structurally complex collagenous tissues that illustrate the power of such 3-dimensional analyses to reveal the architecture of biological structures.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2018

Linear and nonlinear optical probe of the ferroelectric-like phase transition in a polar metal, LiOsO 3

LiOsO 3 is one of the first materials identified in the current literature as a “polar metal,” a class of materials that are simultaneously noncentrosymmetric and metallic. In this work, the linear and nonlinear optical susceptibility of LiOsO 3 is studied by means of ellipsometry and optical second harmonic generation (SHG). Robust optical birefringence is observed using spectroscopic ellipsometry. The nonlinear optical susceptibility extracted from SHG polarimetry reveals that the tensor components are of the same magnitude as in the isostructural insulator LiNbO 3 , except the component along the polar axis d 33 is suppressed by an order of magnitude. Temperature-dependent SHG measurements in combination with Raman spectroscopy indicate a continuous order-disorder type polar phase transition at 140 K. Linear and nonlinear optical microscopy measurements reveal 109°/71° ferroelastic domain walls, like in other trigonal ferroelectrics. No 180° polar domain walls are observed to emerge across the phase transition.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Flexosensitive polarization vortices in thin ferroelectric films

In this work, we present a theoretical study on the influence of the flexoelectric coupling on the spatial distribution and temperature behavior of the spontaneous polarization for several types of stable domain structure in thin ferroelectric films, such as stripe domains and vortices. Finite-element modeling (FEM) for BaTiO 3 films and analytical calculations within the Landau-Ginzburg-Devonshire approach reveals that an out-of-plane polarization component can be very sensitive to the flexoelectric coupling for periodic quasi-2D stripe domains and 3D vortex-antivortex structures. However, the influence is rather different for these structures. The flexoelectric coupling increases significantly the amplitude of a small out-of-plane polarization component in the stripe domains, and the “up” or “down” direction of the component is defined by the sign of the flexoelectric coefficients. Concerning the vortex-antivortex pairs, their antivortices with in-plane antiсirculation have smooth wide dipolar cores through the entire film, whose shape and other features are almost insensitive to the coupling. The vortices with in-plane vorticity have spikelike cores with an out-of-plane quadrupolar moment induced by the flexoelectric coupling. The cores are located near the film–dead-layer interfaces. FEM results corroborated by analytical calculations prove that a change of the flexoelectric coefficient sign leads to a reorientation of the core axial polarization, making the flexosensitive 3D vortices similar to the recently introduced “flexons” in cylindrical nanoparticles. The relatively wide temperature range (from 200 to 400 K) of the flexosensitive vortices' existence gives us confidence that they can be observed experimentally in thin ferroelectric films by scanning-probe and nonlinear optical microscopy methods.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Imaging Interfacial Electric Fields on Ultrafast Timescales (Final Report)

The goal of this project is to dynamically probe interfacial electric fields on ultrafast timescales and sub-micron length scales. The proposed method could be applied to a variety of heterointerfaces, with particular emphasis on interfaces involving colloidal quantum dots. The primary objective is development of an ultrafast nonlinear optical imaging technique with this capability. A secondary objective is obtaining new insights into excited state charge carrier dynamics in colloidal quantum dot solids and at quantum dot interfaces. Research activities involve validation of the technical approach, construction of the microscope, and synthesis and characterization of materials to be studied using the instrument.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Ferroelectricity in a semiconducting all-inorganic halide perovskite

Ferroelectric semiconductors are rare materials with both spontaneous polarizations and visible light absorptions that are promising for designing functional photoferroelectrics, such as optical switches and ferroelectric photovoltaics. The emerging halide perovskites with remarkable semiconducting properties also have the potential of being ferroelectric, yet the evidence of robust ferroelectricity in the typical three-dimensional hybrid halide perovskites has been elusive. Here, we report on the investigation of ferroelectricity in all-inorganic halide perovskites, CsGeX 3 , with bandgaps of 1.6 to 3.3 eV. Their ferroelectricity originates from the lone pair stereochemical activity in Ge (II) that promotes the ion displacement. This gives rise to their spontaneous polarizations of ~10 to 20 μC/cm 2 , evidenced by both ab initio calculations and key experiments including atomic-level ionic displacement vector mapping and ferroelectric hysteresis loop measurement. Furthermore, characteristic ferroelectric domain patterns on the well-defined CsGeBr 3 nanoplates are imaged with both piezo-response force microscopy and nonlinear optical microscopic method.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Tunable, Ultrafast Fiber-Laser between 1.15 μm and 1.35 μm for Harmonic Generation Microscopy in Human Skin

We demonstrate a fiber-optic ultrafast tunable source for harmonic generation microscopy (HGM) in human skin. The source is based on a 31-MHz Er-fiber laser followed by self-phase modulation enabled spectral selection (SESS). The resulting pulses are tunable between 1.15 and 1.35 μm with up to >10-nJ pulse energy and ~100-fs pulse duration. Here we employ this source to drive a scanning microscope for HGM imaging of ex vivo human skin. A systematic investigation on imaging depth versus excitation wavelength reveals that excitation wavelengths in the 1.15-1.25 μm range exhibit low optical attenuation within the tissue and allows larger imaging depth for HGM in human skin. HGM driven by fiber-based SESS sources constitutes an enabling tool for noninvasive virtual skin biopsy in clinical applications.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2017

Dynamic X-ray diffraction sampling for protein crystal positioning

A sparse supervised learning approach for dynamic sampling (SLADS) is described for dose reduction in diffraction-based protein crystal positioning. Crystal centering is typically a prerequisite for macromolecular diffraction at synchrotron facilities, with X-ray diffraction mapping growing in popularity as a mechanism for localization. In X-ray raster scanning, diffraction is used to identify the crystal positions based on the detection of Bragg-like peaks in the scattering patterns; however, this additional X-ray exposure may result in detectable damage to the crystal prior to data collection. Dynamic sampling, in which preceding measurements inform the next most information-rich location to probe for image reconstruction, significantly reduced the X-ray dose experienced by protein crystals during positioning by diffraction raster scanning. The SLADS algorithm implemented herein is designed for single-pixel measurements and can select a new location to measure. In each step of SLADS, the algorithm selects the pixel, which, when measured, maximizes the expected reduction in distortion given previous measurements. Ground-truth diffraction data were obtained for a 5 µm-diameter beam and SLADS reconstructed the image sampling 31% of the total volume and only 9% of the interior of the crystal greatly reducing the X-ray dosage on the crystal. Furthermore, by using in situ two-photon-excited fluorescence microscopy measurements as a surrogate for diffraction imaging with a 1 µm-diameter beam, the SLADS algorithm enabled image reconstruction from a 7% sampling of the total volume and 12% sampling of the interior of the crystal. When implemented into the beamline at Argonne National Laboratory, without ground-truth images, an acceptable reconstruction was obtained with 3% of the image sampled and approximately 5% of the crystal. The incorporation of SLADS into X-ray diffraction acquisitions has the potential to significantly minimize the impact of X-ray exposure on the crystal by limiting the dose and area exposed for image reconstruction and crystal positioning using data collection hardware present in most macromolecular crystallography end-stations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Integrating Plasmonic Metals and 2D Transition Metal Dichalcogenides for Enhanced Nonlinear Frequency Conversion

Surface plasmon resonant nanoantennas can confine incident energy onto two-dimensional (2D) transition metal dichalcogenides (TMD) to enhance efficiency of harmonic conversion to higher energies, which is otherwise limited by the intrinsic A-scale interaction length. Second harmonic generation (SHG) from nanoantenna-decorated 2D TMD was heuristically examined with hyper Rayleigh scattering (HRS), multi-photon microscopy, electron energy loss spectroscopy (EELS), and discrete dipole computation. HRS experimentally quantified the frequency dependence of the second-order nonlinear susceptibility, x(2), for liquid-exfoliated WS2. Measured x(2) fell within 21% of independent density functional theory (DFT) calculations, overcoming the known 100-1000x overestimation of microscopy approaches. EELS supported design of nanoantennas for integration with TMD. Overall SHG conversion efficiencies from chemical vapor-deposited (CVD) 4x105 nm2 MoS2 crystals on silicon dioxide were enhanced up to 0.025 % W-1 in the presence of by single 150 nm Au nanoshell monomers and dimers, ostensibly due to augmented local plasmonic fields.

2D materials↗
DOE OSTI2024

Quantum enhanced magneto-optical microscopy and spectroscopy

A system comprising a nonlinear medium (NLM), an optical transduction module, a dual homodyne detector and a processor is provided. The NLM receives at least a pump beam and issues the pump, probe and conjugate beams, where the beams are linearly polarized. Optics route the probe, the conjugate or both beams to the sample. The sample imparts polarization rotation to light that interacts therewith. The optical transduction module imparts to the interacted light an optical phase shift that is a 1:1 transduction of the polarization rotation, where at least one of the probe light or the conjugate light carries the imparted optical phase shift. The processor obtains the optical-phase shift based on respective detection signals from the dual homodyne detector and determines, based on the obtained optical-phase shift, at least one of a Faraday polarization rotation, a Kerr polarization rotation or a spin noise spectrum.

Lawrie, Benjamin J.↗
DOE OSTI2025

Tailoring spectral properties for entangled photon generation

The linear intensity scaling of entangled two-photon absorption (ETPA) offers a fundamental mechanism to enable nonlinear optical spectroscopy and microscopy under a substantially lower excitation power than is currently feasible. However, the long data acquisition time and low signal-to-noise ratio in reported ETPA-based spectroscopic and microscopic studies prevent its widespread application. To gain the full potential of this novel quantum light approach, it is essential to optimize entangled photon generation for significantly enhanced ETPA responses. Here, we report a new quantum light source by combining entangled photon generation with free-space femtosecond pump-pulse shaping. Here, through measurements of singles and coincidence counts by varying the patterns applied to a spatial light modulator to control the spectral widths of the pump pulses, we reveal strong dependence of the singles and coincidence count rates as well as their ratios on the spectral widths of pump pulses. An optimal spectral width for the highest ratios between the coincidence photon and the signal or idler photon count rates is also determined. Identification of such optimal spectral widths for entangled photon generation in the presence of postgeneration spectral selection makes this quantum light source a promising choice for ETPA-based spectroscopy and imaging.

Photon pairs & parametric down-conversion↗