Anisotropic Second-harmonic Generation Research Articles

Strong nonlinear optical processes with extraordinary polarization anisotropy in inversion-symmetry broken two-dimensional PdPSe

Nonlinear optical activities, especially second harmonic generation (SHG), are key phenomena in inversion-symmetry-broken two-dimensional (2D) transition metal dichalcogenides (TMDCs). On the other hand, anisotropic nonlinear optical processes are important for unique applications in nano-nonlinear photonic devices with polarization functions, having become one of focused research topics in the field of nonlinear photonics. However, the strong nonlinearity and strong optical anisotropy do not exist simultaneously in common 2D materials. Here, we demonstrate strong second-order and third-order susceptibilities of 64 pm/V and 6.2×10−19 m2/V2, respectively, in the even-layer PdPSe, which has not been discovered in other common TMDCs (e.g., MoS2). Strikingly, it also simultaneously exhibited strong SHG anisotropy with an anisotropic ratio of ~45, which is the largest reported among all 2D materials to date, to the best of our knowledge. In addition, the SHG anisotropy ratio can be harnessed from 0.12 to 45 (375 times) by varying the excitation wavelength due to the dispersion of χ(2)\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${\\chi }^{(2)}$$\\end{document} values. As an illustrative example, we further demonstrate polarized SHG imaging for potential applications in crystal orientation identification and polarization-dependent spatial encoding. These findings in 2D PdPSe are promising for nonlinear nanophotonic and optoelectronic applications.

Controlling the Orientation‐Dependent Second Harmonic Generation in Hybrid Germanium Perovskite Crystals

Manipulating the crystal orientation plays a crucial role in the conversion efficiency during second harmonic generation (SHG). Here, we provide a new strategy in controlling the surface‐dependent anisotropic SHG with the precise design of (101) and (20) MAGeI3 facets. Based on the SHG measurement, the (101) MAGeI3 single crystal exhibits larger SHG (1.3 × (20) MAGeI3). Kelvin probe force microscopy imaging shows a smaller work function for the (101) MAGeI3 compared with the (20), which indirectly demonstrates the stronger intrinsic polarization on the (101) surface. X‐ray photoelectron spectroscopy confirms the band bending within the (101) facet. Temperature‐dependent steady‐state and time‐resolved photoluminescence spectroscopy show shorter lifetime and wider emission band in the (101) MAGeI3 single crystal, revealing the higher defect states. Additionally, powder X‐ray diffraction patterns show the (101) MAGeI3 possesses larger in‐plane polar units [GeI3]‐ density, which could directly enhance the spontaneous polarization in the (101) facet. Density functional theory (DFT) calculation further demonstrates the higher intrinsic polarization in the (101) facet compared with the (20) facet, and the larger built‐in electric field in the (101) facet facilitates surface vacancy defect accumulation. Our work provides a new angle in tuning and optimizing hybrid perovskite‐based nonlinear optical materials.

Controlling the Orientation-Dependent Second Harmonic Generation in Hybrid Germanium Perovskite Crystals.

Manipulating the crystal orientation plays a crucial role in the conversion efficiency during second harmonic generation (SHG). Here, we provide a new strategy in controlling the surface-dependent anisotropic SHG with the precise design of (101) and (20) MAGeI3 facets. Based on the SHG measurement, the (101) MAGeI3 single crystal exhibits larger SHG (1.3 × (20) MAGeI3). Kelvin probe force microscopy imaging shows a smaller work function for the (101) MAGeI3 compared with the (20), which indirectly demonstrates the stronger intrinsic polarization on the (101) surface. X-ray photoelectron spectroscopy confirms the band bending within the (101) facet. Temperature-dependent steady-state and time-resolved photoluminescence spectroscopy show shorter lifetime and wider emission band in the (101) MAGeI3 single crystal, revealing the higher defect states. Additionally, powder X-ray diffraction patterns show the (101) MAGeI3 possesses larger in-plane polar units [GeI3]- density, which could directly enhance the spontaneous polarization in the (101) facet. Density functional theory (DFT) calculation further demonstrates the higher intrinsic polarization in the (101) facet compared with the (20) facet, and the larger built-in electric field in the (101) facet facilitates surface vacancy defect accumulation. Our work provides a new angle in tuning and optimizing hybrid perovskite-based nonlinear optical materials.

Abstract PO3-07-01: Multiscale Computational Analysis of Patient-Matched Multi-Modal Imaging of Breast Tissue Microenvironment

Abstract Introduction: Mammographic breast density is a strong quantitative cancer risk factor, but its link to underlying tissue and cellular level changes are weakly understood. Understanding the complex restructuring changes in the breast tumor microenvironment and its impact on breast density is integral to improving risk assessment and treatment strategies. A novel approach was developed to stratify mammographic dense breast tissue into areas of active dense tissue and passive dense tissue. Active dense tissue is structurally reorganizing and links to cancer dynamics, whereas passive dense mammographic tissue remains organized.1,2 A complementary wavelet-based analysis technique to measure the multiscale anisotropy of collagen fibers from Second-Harmonic Generation (SHG) imaging demonstrated clinical cancer diagnostic potential in mouse carcinoma and human pancreatic cancer.3,4 This tool is now leveraged for a multi-modal study in which patient-matched H&E tissue biopsies are imaged using both bright-field microscopy and SHG imaging to compare with the patient’s corresponding mammograms. Stratifying the mammographic density into active and passive dense areas, a correlation between biopsy tissue anisotropy and mammographic density subtypes can be calculated to help understand how tumor microenvironment changes affect a patient’s mammographic breast tissue composition. Methods: SHG and brightfield-imaged biopsy slides from 10 patients (five malignant, five benign) collected from Maine Medical Center (Maine, US) were analyzed using the 2D Wavelet Transform Modulus Maxima (WTMM) Anisotropy Method generating a large-scale and a small-scale anisotropy factor as well as a scale-combined anisotropy calculated from their large- and small-scale anisotropy separation. A multi-modal anisotropy score was calculated by adding the imaged area’s H&E combined anisotropy score with its respective SHG combined anisotropy score. This analysis was done on eight randomly selected ductal areas for each imaging modality on a slide and correlated with the measured areas of density subtypes from the whole mammographic view. Linear regression was used for determining correlation between H&E and SHG anisotropy factors as well as with active and passive mammographic density subtype measurements. Results: The malignant patients’ small-scale H&E anisotropy factor positively correlated with their small scale SHG anisotropy factor (R2=0.571). No correlation was found for the benign patients (R2=0.011). The strongest correlations were found between benign patients’ mammographic passive (positive correlation) and active (negative correlation) dense tissues vs the H&E anisotropy scale-combined factor (R2=0.858 and R2=0.961, respectively). The largest malignant patient correlation was a negative relationship between SHG anisotropy scale-combined factor and overall mammographic density (inclusive of both active and passive dense tissue) (R2=0.891). The multi-modal anisotropy score correlated with overall mammographic density for both benign (positive correlation, R2=0.698) and malignant patients (negative correlation, R2=0.773). Combining the multi-modal anisotropy factor from SHG and H&E with the active dense tissue measurement using K-Means clustering, 5/5 malignant and 4/5 benign patients were correctly classified. Conclusion: Density in mammograms correlates with underlying quantitative changes in a patient’s tissue and collagen anisotropy. Combining both H&E and SHG analysis on tissue biopsy with active and passive density metrics from computational mammography leads to the best predictive potential than any one method on their own.

Observation of Anisotropic Second Harmonic Generation in Two-Dimensional Niobium Diselenide.

The intrinsic anisotropy of NbSe2 provides a favorable prerequisite of second harmonic generation (SHG) and rich possibilities for tailoring its nonlinear optical (NLO) properties. Here we report the highly efficient SHG of mechanically exfoliated NbSe2 flakes. The nonlinear optical response changes with excitation wavelengths, layer thicknesses, and polarizations of the excitation laser. The anisotropic SHG response further exhibits the intrinsic non-centrosymmetric crystal structure and could effectively assign the crystalline orientation of NbSe2 flakes. Interestingly, although NbSe2 flakes with tens of nanometers thickness experience attenuations in SHG performance, more efficient SHG anisotropy ratios were obtained, which are around 4 times higher than that of the 5-layer counterpart. The determined second-order nonlinearities of NbSe2 flakes (monolayer: ∼1.0 × 103 pm/V; 3-layer: ∼73 pm/V) are comparable to those of the commonly reported two-dimensional materials (e.g., MoS2, WSe2, graphene) with the same number of layers and much higher than those of commercial nonlinear optical crystals.

Extraordinary second harmonic generation modulated by divergent strain field in pressurized monolayer domes

The most prominent form of nonlinear optical (NLO) frequency conversion is second harmonic generation (SHG), where incident light interacts with a nonlinear medium producing photons at double the input frequency, which has vast applications in material and biomedical science. Emerging two-dimensional nonlinear optical materials led by transition metal dichalcogenides (TMDs) have fascinating optical and mechanical properties and are highly anticipated to overcome the technical limitations imposed by traditional bulky NLO materials. However, the atomic scale interaction length and low conversion efficiency in TMD materials prevent their further implementation in NLO applications. While some uniaxial strain-engineering studies intensively investigated the anisotropic SHG response in TMDs, they did not realize giant SHG enhancement by exploiting the opto-mechanical characteristics. Herein, we employ proton (H+) irradiation to successfully fabricate large pressurized monolayer TMD domes (d ≥ 10 μm) and conduct a comprehensive investigation and characterization of their SHG performance enhancement. We show that the intensity of SHG is effectively enhanced by around two orders of magnitude at room temperature. Such giant enhancement arises from the distinct separation distance induced by capped pressurized gas and the hemi-spherical morphology, enabling constructive optical interference. Moreover, the unique divergent strain field in TMD domes promotes the first experimental study on the anisotropic nonlinear optical behavior based on biaxial strain conditions in terms of varying strain orientation and relative weights. Our work demonstrates a promising system with enhanced NLO performance and well-preserved biocompatibility, paving a way toward the future nano-scaled quantum optics design and biomedical applications.

Estimation of crossbridge-state during cardiomyocyte beating using second harmonic generation.

Estimation of dynamic change of crossbridge formation in living cardiomyocytes is expected to provide crucial information for elucidating cardiomyopathy mechanisms, efficacy of an intervention, and others. Here, we established an assay system to dynamically measure second harmonic generation (SHG) anisotropy derived from myosin filaments depended on their crossbridge status in pulsating cardiomyocytes. Experiments utilizing an inheritable mutation that induces excessive myosin-actin interactions revealed that the correlation between sarcomere length and SHG anisotropy represents crossbridge formation ratio during pulsation. Furthermore, the present method found that ultraviolet irradiation induced an increased population of attached crossbridges that lost the force-generating ability upon myocardial differentiation. Taking an advantage of infrared two-photon excitation in SHG microscopy, myocardial dysfunction could be intravitally evaluated in a Drosophila disease model. Thus, we successfully demonstrated the applicability and effectiveness of the present method to evaluate the actomyosin activity of a drug or genetic defect on cardiomyocytes. Because genomic inspection alone may not catch the risk of cardiomyopathy in some cases, our study demonstrated herein would be of help in the risk assessment of future heart failure.

Surface symmetry determination by a deep learning application of optical second-harmonic generation results

Optical second-harmonic generation (SHG) technique is widely used to characterize the structural symmetry of condensed matters not only for the bulk but also for the surface states. Since experimental results of the SHG anisotropy patterns often contain multiple contributions from bulk and surface states, a conventional regression process may not provide a unique solution about the symmetry of each part. With a given symmetry for the bulk state, we here develop a discriminator for the surface symmetry by exploiting neural architectures based on 1D convolution layers where simulation results of SHG anisotropy patterns are taken as learning sequence data. Since SHG experimental results have limited information for determining a unique symmetry out of several symmetry candidates, our discriminator consists of tens of neural architectures optimized with different hyperparameters. As a final output, the surface symmetry discriminator gives a weighted sum of results suggested from all the individual neural architectures. We demonstrate that the discrimination results of the deep learning approach agree well with those of the conventional regression method for GaAs and Bi2Se3.

Strong In‐Plane Anisotropy and Giant Second Harmonic Generation Response of Organic Single‐Crystalline Microwire Arrays

AbstractOrganic nonlinear optical (NLO) crystals play an indispensable role in high‐performance photonic devices due to their large nonlinear coefficient, fast response time, and low dielectric constant. However, in contrast to the strides of bulk crystals, researches on the next generation of nanophotonic devices are ignored to some extent. One of the bottlenecks is the controllable manufacturing and patterning of high‐quality organic NLO crystals with the nanometer‐scale thickness. Herein, a confined assembly method for fabricating the microwire arrays of organic NLO crystal OH1 and DAT2 with precise position, flat morphology, high crystallinity, and consistent crystallographic orientation is reported. Two strong NLO effects observed in the experiments are comprehensively studied, including second harmonic generation (SHG) and two‐photon excited fluorescence. Furthermore, it is demonstrated that the anisotropic SHG effect depends on both the polarization of incident light and the crystallographic orientation of microwire arrays. Microwire arrays can exhibit large in‐plane anisotropy with the polarization ratio up to 0.95 and second‐order nonlinear coefficient up to 55.1 pm V−1. This work provides new insights into the potential applications of organic NLO crystals in integrated optical devices.

Terahertz-field-induced second optical harmonic generation from Si(111) surface

We study, both experimentally and theoretically, the second-harmonic (SH) generation (SHG) of optical radiation assisted by intense terahertz electromagnetic pulses from the surface of high-resistivity Si(111). The study was performed within the framework of the analysis of the superposition of different SH sources, including the surface-dipole, bulk-quadruple, and electric-field-induced (EFI) bulk-dipole (arising from internal built-in and external terahertz fields) contributions. Azimuthal rotation anisotropy of SHG for an arbitrary mutual polarization of the terahertz, fundamental, and SH optical fields was calculated and experimentally verified. The strongest impact of the terahertz field on SHG was observed in the case where the polarizations of the terahertz and SH fields coincide. In these polarization configurations, the terahertz field added mainly an isotropic term to the SH azimuthal dependences. It has been demonstrated that the application of the terahertz field can be helpful for distinguishing the SHG mechanism. For the sample under study, the contribution to the SH energy from the built-in field-induced source was found to be >4 times greater than the contribution from the surface and quadrupole nonlinear sources. The dominance of the EFISHG allowed us to find the ratio between the components of a silicon third-order nonlinear tensor ${\ensuremath{\chi}}_{}^{(3)}(2\ensuremath{\omega};\ensuremath{\omega},\ensuremath{\omega},0)$: ${\ensuremath{\chi}}_{1122}={\ensuremath{\chi}}_{1212}\ensuremath{\approx}0.51{\ensuremath{\chi}}_{1111}$ and ${\ensuremath{\chi}}_{1212}\ensuremath{\approx}{\ensuremath{\chi}}_{1221}$ for the fundamental optical wavelength 790 nm.

Regulating Optical Activity and Anisotropic Second-Harmonic Generation in Zero-Dimensional Hybrid Copper Halides.

Structural engineering permits the introduction of chirality into organic-inorganic hybrid metal halides (HMHs), which creates a promising and exclusive material for applications in various optoelectronics. However, the optical activity regulation of chiral HMHs remains largely unexplored. In this work, we have synthesized two pairs of lead-free chiral HMHs with a zero-dimensional tetrahedral arrangement, i.e., (R- and S-1-(1-naphthyl)ethylammonium)2CuCl4 and (R- and S-1-(2-naphthyl)ethylammonium)2CuCl4. The magnitude of optical activity in these HMHs can be efficiently modulated as a result of the different magnetic transition dipole moments. Furthermore, these HMHs exhibited effective second-harmonic generation (SHG) and distinct SHG-circular dichroism (CD), with (R-1-(1-naphthyl)ethylammonium)2CuCl4 having an anisotropy factor (gSHG-CD) of up to 0.41. This work not only provides insights into regulating the optical activity and anisotropic SHG effect of lead-free chiral HMHs but also confirms the feasibility of SHG-CD spectroscopy as a promising tool for characterizing the intrinsic optical activity of chiral materials.

Anisotropic Second-Harmonic Generation Induced by Reduction of In-Plane Symmetry in 2D Materials with Strain Engineering.

Strain engineering is an attractive method to induce and control anisotropy for polarized optoelectronic applications with two-dimensional (2D) materials. Herein, we have investigated the nonlinear optical coefficient dispersion relationship and the second-harmonic generation (SHG) pattern evolution under the uniaxial strains for graphene, WS2, GaSe, and In2Se3 monolayers. The uniaxial strain can break the in-plane symmetry of 2D materials, leading to both trade-off breaking of the nonlinear coefficient and new emergent nonlinear coefficients. In such a case, a classical sixfold ϕ-dependent SHG pattern is transformed into a distorted sixfold SHG pattern under the strain. Due to the lattice symmetry breaking and the uneven charge density distribution in strained 2D materials, the SHG patterns also depend on the excitation photon energy. The results could give a guide for the SHG pattern analysis in experiments, suggesting strain engineering on 2D materials for the tunable anisotropy in polarized and flexible nonlinear optical devices.

The First Improper Ferroelectric of 2D Multilayered Hybrid Perovskite Enabling Strong Tunable Polarization‐Directed Second Harmonic Generation Effect

Abstract2D organometallic halide perovskites are recently emerging as a robust family of ferroelectrics, of which their inherent spontaneous polarization (Ps) endows fascinating quadratic nonlinear optical properties. However, up to date, few studies are reported to tune and control the second harmonic generation (SHG) effect in this ferroelectric branch. Herein, the first improper ferroelectric of 2D multilayered hybrid perovskites, (IA)2(EA)2Pb3Br10 (1, where IA is isoamylammonium and EA is ethylammonium), which exhibits a high Curie temperature (≈371 K) and biaxial ferroelectricity with Ps of 2.2 µC cm−2 is reported. Strikingly, its unique in‐plane ferroelectricity allows strong tunable SHG properties under the polarized‐light. That is, the maximum SHG signals are observed with polarized‐light parallel to Ps, while the minimum SHG appears along the vertical direction. This SHG anisotropy creates an extremely large dichroism ratio of ≈12, as visualized by 2D color mapping, which is the record‐high merit for this type of SHG systems. To the best knowledge, this is the first time to achieve tunable SHG effects through ferroelectric polarization. As a pioneering study, the coupling between the SHG effect and ferroelectricity paves a new direction of 2D hybrid perovskite ferroelectrics toward smart optical device applications.

Probing the Chiral Domains and Excitonic States in Individual WS2 Tubes by Second-Harmonic Generation.

Distinct from carbon nanotubes, transition-metal dichalcogenide (TMD) nanotubes are noncentrosymmetric and polar and can exhibit some intriguing phenomena such as nonreciprocal superconductivity, chiral shift current, bulk photovoltaic effect, and exciton-polaritons. However, basic characterizations of individual TMD nanotubes are still quite limited, and much remains unclear about their structural chirality and electronic properties. Here we report an optical second-harmonic generation (SHG) study on multiwalled WS2 nanotubes on a single-tube level. As it is highly sensitive to the crystallographic symmetry, SHG microscopy unveiled multiple structural domains within a single WS2 nanotube, which are otherwise hidden under conventional white-light optical microscopy. Moreover, the polarization-resolved SHG anisotropy patterns revealed that different domains on the same tube can be of different chirality. In addition, we observed the excitonic states of individual WS2 nanotubes via SHG excitation spectroscopy, which were otherwise difficult to acquire due to the indirect band gap of the material.

Optical second-harmonic generation microscopy as a tool for ferroelastic domain wall exploration

Domain walls (DWs) of four typical ferroelastics, CaTiO3 (CTO), LaAlO3 (LAO), Pb3(PO4)2 (PPO), and BiVO4 (BVO), were observed by the second harmonic generation (SHG) microscopy, and the results were compared. The DWs of the examined ferroelastics are all polar. This fact does not depend on whether the crystal is an insulator (CTO, LAO, and PPO) or a semiconductor (BVO), on whether it has ferroelectric instability (CTO) or not (LAO, PPO, and BVO), or on the DW state, namely, whether the DW is crystallographically prominent or non-prominent. The symmetry of these DWs was determined from the SHG anisotropy, and it was clarified that they are a subgroup of the high temperature phase. In the cases of CTO and PPO, stress was applied to move the DW, and its polarity and symmetry were examined. The main characteristics did not change even when stress was applied. In all samples, uniform SHG was observed for each DW. This indicates that the DWs of the examined ferroelastics seem to be in a ferroelectric single domain state.

Polarization-dependent second-harmonic generation for collagen-based differentiation of breast cancer samples.

Nonlinear optical imaging techniques have been widely used to reveal biological structures for accurate diagnosis at the cellular as well as the tissue level. In the present study, polarization-dependent second-harmonic generation (PSHG) was used to determine collagen orientation in breast cancer biopsy tissues (grades 0, I, II and III). The obtained data were processed using fast Fourier transform (FFT) analysis, while second-harmonic generation (SHG) anisotropy and the "ratio parameter" values were also calculated. Such measurements were shown to be able to distinguish collagen structure modifications in different cancer grades tested. The analysis presented herein suggests that PSHG imaging could provide a quantitative evaluation of the tumor state and the distinction of malignant from benign breast tissues. The obtained results also allowed the development of a biophysical model, which can explain the aforementioned differentiations and is in agreement with the simulations relating the SHG anisotropy values with the mechanical tension applied to the collagen during cancer progression. The current approach could be a step forward for the development of new, nondestructive, label free optical diagnostic tools for cancer reducing the need of recalls and unnecessary biopsies, while potentially improving cancer detection rates.

Bond additivity model for anisotropic second-harmonic generation from two-dimensional honeycomb lattices

We provide an analytical method for extracting detailed structural information about two-dimensional (2D) honeycomb lattices from optical second-harmonic generation (SHG) anisotropy patterns. When the lattice deviates from the ideal honeycomb structure, we relate the microscopic structural properties, such as bond length and bonding angle, to the macroscopic nonlinear susceptibility tensor based on the molecular bond additivity model. Our method will help quantitative studies of 2D materials with SHG and is readily applied to more general cases.

Anisotropic Enhancement of Second-Harmonic Generation in Monolayer and Bilayer MoS2 by Integrating with TiO2 Nanowires.

The ability to design and enhance the nonlinear optical responses in two-dimensional (2D) transition-metal dichalcogenides (TMDCs) is both of fundamental interest and highly desirable for developing TMDC-based nonlinear optical applications, such as nonlinear convertors and optical modulators. Here, we report for the first time a strong anisotropic enhancement of optical second-harmonic generation (SHG) in monolayer molybdenum disulfide (MoS2) by integrating with one-dimensional (1D) titanium dioxide nanowires (NWs). The SHG signal from the MoS2/NW hybrid structures is over 2 orders of magnitude stronger than that in the bare monolayer MoS2. Polarized SHG measurements revealed a giant anisotropy in SHG response of the MoS2/NW hybrid. The pattern of the anisotropic SHG depends highly on the stacking angle between the nanowire direction and the MoS2 crystal orientation, which is attributed to the 1D NW-induced directional strain fields in the layered MoS2. A similar effect has also been observed in bilayer MoS2/NW hybrid structure, further proving the proposed scenario. This work provides an effective approach to selectively and directionally designing the nonlinear optical response of layered TMDCs, paving the way for developing high-performance, anisotropic nonlinear photonic nanodevices.

Polarization-resolved second harmonic generation imaging of human ovarian cancer.

.Remodeling of the extracellular matrix in human ovarian cancer can be manifested in increased collagen concentration, changes in alignment within fibrils/fibers and/or up-regulation of different collagen isoforms. We used pixel-based second harmonic generation (SHG) polarization microscopy analyses to probe these molecular changes in human ovarian tissues [normal stroma, benign tumors, and high-grade serous (HGS) tumors] by: (i) determination of the -helical pitch angle via the single-axis molecular model, (ii) collagen alignment within fibrils via SHG anisotropy, and (iii) chirality via SHG circular dichroism (SHG-CD). Pixel approaches are required due to the complex structure of the matrix that lacks a high degree of fiber alignment. The largest differences in the helical pitch angle were between normal stroma and benign tumors, consistent with gene expression showing the Col III isoform is up-regulated in the latter. The data were not consistent with up-regulation of Col III in HGS tumors as previous reports have suggested. The different tissues also displayed differing SHG anisotropies and SHG-CD responses, consistent with either Col III incorporation or randomization of Col I alignment within benign and malignant tumors. Additionally, the high-grade tumors displayed higher collagen concentration, where this desmoplasia is consistent with the higher fiber density in these tissues. These results collectively indicate that the fibril assemblies are distinct in all tissues, where these differences likely result from the synthesis of collagen rather than remodeling of existing collagen. Importantly, these analyses are label-free and interrogate subresolution collagen structure on intact tissues, without the need for conventional structural biology tools.

Precise characterization of self-catalyzed III–V nanowire heterostructures via optical second harmonic generation

We demonstrate the utility of optical second harmonic generation (SHG) polarimetry to perform structural characterization of self-assembled zinc-blende/wurtzite III–V nanowire heterostructures. By analyzing four anisotropic SHG polarimetric patterns, we distinguish between wurtzite (WZ), zinc-blende (ZB) and ZB/WZ mixing III–V semiconducting crystal structures in nanowire systems. By neglecting the surface contributions and treating the bulk crystal within the quasi-static approximation, we can well explain the optical SHG polarimetry from the NWs with diameter from 200–600 nm. We show that the optical in-coupling and out-coupling coefficients arising from depolarization field can determine the polarization of the SHG. We also demonstrate micro-photoluminescence of GaAs quantum dots in related ZB and ZB/WZ mixing sections of core–shell NW structure, in agreement with the SHG polarimetry results. The ability to perform in situ SHG-based crystallographic study of semiconducting single and multi-crystalline nanowire heterostructures will be useful in displaying structure-property relationships of nanodevices.