Quasicrystal Photonic Metasurfaces for Radiation Controlling of Second Harmonic Generation

Photonic metasurfaces, a kind of 2D structured medium, represent a novel platform to manipulate the propagation of light at subwavelength scale. In linear optical regime, many interesting topics such as planar meta‐lenses, metasurface optical holography, and so on have been widely investigated. Recently, metasurfaces have gone into the nonlinear optical regime. While it is recognized that the local symmetry of the meta‐atoms plays a vital role in determining the polarization, phase, and intensity of the nonlinear waves, much less attention has been paid to the global symmetry of the nonlinear metasurfaces. According to the Penrose tiling and the newly proposed hexagonal quasicrystalline tiling, nonlinear optical quasicrystal metasurfaces are designed and fabricated based on the geometric‐phase‐controlled plasmonic meta‐atoms with local rotational symmetry. It is found that the far‐field radiation behavior of second harmonic generation waves are determined by both the tiling schemes of quasicrystal metasurfaces and the local symmetry of meta‐atoms they consist of. The proposed concept may open new avenues for designing nonlinear optical sources with metasurface crystals.     

二次谐波在二维材料结构表征中的应用

二次谐波作为非线性光学的重要分支,逐渐成为表征晶体结构的重要手段之一。在众多表征方法中,二次谐波因其无损检测、高稳定性、可调谐性、超快响应、偏振敏感性、通用性、操作简单等特点被广泛应用于二维材料结构表征,为二维材料的物性研究和功能应用提供了重要信息,大大推动了二维材料基础研究的快速发展。本文综述了近几年二次谐波在二维材料结构表征中的研究,简述了二次谐波产生原理,介绍了飞秒激光器接入共聚焦拉曼光谱仪产生二次谐波测试装置,分别讨论了二次谐波在二维材料的层间堆垛层数、层间堆垛角度、单层二维材料晶界及晶体取向表征方面的应用。同时,本文还介绍了采用二次谐波强度直接、灵敏地检测晶体中应变幅度以及通过二次谐波信号变化跟踪材料中的缺陷变化,接着讨论了二次谐波与拉曼光谱、光致发光的多维度关联分析在材料全面深度表征方面的重要性。最后展望了二次谐波未来在材料结构表征中的潜在研究方向。     

Effective Labeling of Primary Somatic Stem Cells with BaTiO3 Nanocrystals for Second Harmonic Generation Imaging

While nanoparticles are an increasingly popular choice for labeling and tracking stem cells in biomedical applications such as cell therapy, their intracellular fate and subsequent effect on stem cell differentiation remain elusive. To establish an effective stem cell labeling strategy, the intracellular nanocrystal concentration should be minimized to avoid adverse effects, without compromising the intensity and persistence of the signal necessary for long‐term tracking. Here, the use of second‐harmonic generating barium titanate nanocrystals is reported, whose achievable brightness allows for high contrast stem cell labeling with at least one order of magnitude lower intracellular nanocrystals than previously reported. Their long‐term photostability enables to investigate quantitatively at the single cell level their cellular fate in hematopoietic stem cells (HSCs) using both multiphoton and electron microscopy. It is found that the concentration of nanocrystals in proliferative multipotent progenitors is over 2.5‐fold greater compared to quiescent stem cells; this difference vanishes when HSCs enter a nonquiescent, proliferative state, while their potency remains unaffected. Understanding the nanoparticle stem cell interaction allows to establish an effective and safe nanoparticle labeling strategy into somatic stem cells that can critically contribute to an understanding of their in vivo therapeutic potential.     

Broadband High‐Efficiency Chiral Splitters and Holograms from Dielectric Nanoarc Metasurfaces

Simultaneous broadband and high efficiency merits of designer metasurfaces are currently attracting widespread attention in the field of nanophotonics. However, contemporary metasurfaces rarely achieve both advantages simultaneously. For the category of transmissive metadevices, plasmonic or conventional dielectric metasurfaces are viable for either broadband operation with relatively low efficiency or high efficiency at only a selection of wavelengths. To overcome this limitation, dielectric nanoarcs are proposed as a means to accomplish two advantages. Continuous nanoarcs support different electromagnetic resonant modes at localized areas for generating phase retardation. Meanwhile, the geometric nature of nanoarc curvature endows the nanoarcs with full phase coverage of 0–2π due to the Pancharatnam–Berry phase principle. Experimentally incorporated with the chiral‐detour phase principle, a few compelling functionalities are demonstrated, such as chiral beamsplitting, broadband holography, and helicity‐selective holography. The continuous nanoarc metasurfaces prevail over plasmonic or dielectric discretized building block strategies and the findings lead to novel designs of spin‐controllable metadevices.     

Second Harmonic Light Manipulation with Vertical Split Ring Resonators

The second harmonic generation (SHG) of vertical and planar split‐ring resonators (SRRs) that are broken centro‐symmetry configurations at the interface of metal surface and air is investigated. Strong interactions, better electromagnetic field confinements, and less leakage into the substrate for vertical SRRs are found. Experimental results show a 2.6‐fold enhancement of SHG nonlinearity, which is in good agreement with simulations and calculations. Demonstrations of 3D metastructures and vertical SRRs with strong SHG nonlinearity majorly result from magnetic dipole and electric quadrupole clearly provides potential applications for photonics and sensing.     

Resource‐Efficient Low‐Temperature Synthesis of Microcrystalline Pb2B5O9X (X = Cl,Br) for Surfaces Studies by Optical Second Harmonic Generation

Optically nonlinear Pb₂B₅O₉X (X = Cl, Br) borate halides are an important group of materials for second harmonic generation (SHG). Additionally, they also possess excellent photocatalytic activity and stability in the process of dechlorination of chlorophenols, which are typical persistent organic pollutants. It would be of great interest to conduct in situ (photo‐) catalysis investigations during the whole photocatalytic process by SHG when considering them as photocatalytic materials. In order to get superior photocatalytic efficiency and maximum surface information, small particles are highly desired. Here, a low‐cost and fast synthesis route that allows growing microcrystalline optically nonlinear Pb₂B₅O₉X borate halides at large quantities is introduced. When applying the ionothermal growth process at temperatures between 130 and 170 °C, microcrystallites with an average size of about 1 µm precipitate with an orthorhombic hilgardite‐like borate halide structure. Thorough examinations using powder X‐ray diffraction and scanning electron microscopy, the Pb₂B₅O₉X microcrystals are indicated to be chemically pure and single‐phased. Besides, the Pb₂B₅O₉X borate halides' SHG efficiencies are confirmed using confocal SHG microscopy. The low‐temperature synthesis route thus makes these borate halides a highly desirable material for surface studies such as monitoring chemical reactions with picosecond time resolution and in situ (photo‐) catalysis investigations.     

Bismuth Ferrite Second Harmonic Nanoparticles for Pulmonary Macrophage Tracking

Recently, second harmonic generation (SHG) nanomaterials have been generated that are efficiently employed in the classical (NIR) and extended (NIR‐II) near infrared windows using a multiphoton microscope. The aim was to test bismuth ferrite harmonic nanoparticles (BFO‐HNPs) for their ability to monitor pulmonary macrophages in mice. BFO‐loaded MH‐S macrophages are given intratracheally to healthy mice or BFO‐HNPs are intranasally instilled in mice with allergic airway inflammation and lung sections of up to 100 μM are prepared. Using a two‐photon‐laser scanning microscope, it is shown that bright BFO‐HNPs signals are detected from superficially localized cells as well as from deep within the lung tissue. BFO‐HNPs are identified with an excellent signal‐to‐noise ratio and virtually no background signal. The SHG from the nanocrystals can be distinguished from the endogenous collagen–derived SHG around the blood vessels and bronchial structures. BFO‐HNPs are primarily taken up by M2 alveolar macrophages in vivo. This SHG imaging approach provides novel information about the interaction of macrophages with cells and the extracellular matrix in lung disease as it is capable of visualizing and tracking NP‐loaded cells at high resolution in thick tissues with minimal background fluorescence.     

Polarization-Independent Second Harmonic Generation in 2D Van Der Waals Kagome Nb3SeI7 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 Nb₃SeI₇ crystals with a breathing Kagome lattice. The Nb₃ triangular clusters and Janus-structure of each Nb₃SeI₇ layer are confirmed by the STEM. Nb₃SeI₇ flake shows a strong SHG response due to its noncentrosymmetric crystal structure. More interestingly, the SHG signals of Nb₃SeI₇ 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.     

Second‐Harmonic Generation from a Single Core/Shell Quantum Dot

Nanoparticles emitting two‐photon luminescence are broadly used as photostable emitters for nonlinear microscopy. Second‐harmonic generation (SHG) as another two‐photon mechanism offers complementary optical properties but the reported sizes of nanoparticles are still large, of a few tens of nanometers. Herein, coherent SHG from single core/shell CdTe/CdS nanocrystals with a diameter of 10 to 15 nm is reported. The nanocrystal excitation spectrum reveals resonances in the nonlinear efficiency with an overall maximum at about 970 nm. Polarization analysis of the second‐harmonic emission confirms the expected zinc blende symmetry, and allows extraction of the three‐dimensional nanocrystal orientation. The small size of these nonlinearly active quantum dots, together with the intrinsic coherence and orientation sensitivity of the SHG process, are well adapted for ultrafast probing of optical near‐fields with high resolution as well as for orientation tracking for bioimaging applications.     

碘化亚铜微晶掺杂硼硅酸盐玻璃的制备及其电致二阶非线性光学效应

采用可分相的Ｎａ２－Ａｌ２Ｏ３－Ｂ２Ｏ３－ＳｉＯ２系为基础玻璃，以ＣｕＯ／ＳｎＯ、ＮａＩ为原料，分别引入Ｃｕ＾＋、Ｉ＾－，成功地制备出ＣｕＩ微晶掺杂硼硅酸盐玻璃。通过Ｘ射线粉末衍射（ＸＲＤ）和高分辨透射电镜（ＨＲＴＥＭ）分析观察到了玻璃中的晶相及其分布；由玻璃的室温透射光谱研究了玻璃的热处理条件下光吸收性的关系。首次报道了该半导体微昌掺杂玻璃中的电致二次谱波发生，并讨论了该效应的机理。     

碘化亚铜微晶掺杂硼硅酸盐玻璃的制备及其电致二阶非线性光学效应

采用可分相的Na2－Al2O3－B2O3－SiO2系为基础玻璃，以CuO／SnO、NaI为原料；分别引入Cu 、I－，成功地制备出CuI微晶掺杂硼硅酸盐玻璃·通过X射线粉末衍射（XRD）和高分辨透射电镜（HRTEM）分析观察到了玻璃中的晶相及其分布；由玻璃的室温透射光谱研究了玻璃的热处理条件与光吸收性的关系．首次报道了该半导体微晶掺杂玻璃中的电致二次谐波发生，并讨论了该效应的机理．     

Metrology of Multiphoton Microscopes Using Second Harmonic Generation Nanoprobes

In multiphoton microscopy, the ongoing trend toward the use of excitation wavelengths spanning the entire near‐infrared range calls for new standards in order to quantify and compare the performances of microscopes. This article describes a new method for characterizing the imaging properties of multiphoton microscopes over a broad range of excitation wavelengths in a straightforward and efficient manner. It demonstrates how second harmonic generation (SHG) nanoprobes can be used to map the spatial resolution, field curvature, and chromatic aberrations across the microscope field of view with a precision below the diffraction limit and with unique advantages over methods based on fluorescence. KTiOPO4 nanocrystals are used as SHG nanoprobes to measure and compare the performances over the 850–1100 nm wavelength range of several microscope objectives designed for multiphoton microscopy. Finally, this approach is extended to the post‐acquisition correction of chromatic aberrations in multicolor multiphoton imaging. Overall, the use of SHG nanoprobes appears as a uniquely suited method to standardize the metrology of multiphoton microscopes.