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Keywords = strong SHG responses

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13 pages, 3840 KiB  
Article
Second Harmonic Generation Imaging of Strain-Induced Domain Evolution Across Grain Boundaries in SrTiO3 Bicrystals
by Yuhang Ren and Piyali Maity
Surfaces 2025, 8(3), 47; https://doi.org/10.3390/surfaces8030047 - 1 Jul 2025
Viewed by 371
Abstract
Understanding strain behavior near grain boundaries is critical for controlling structural distortions and oxygen vacancy migration in perovskite oxides. However, conventional techniques often lack the spatial resolution needed to analyze phase and domain evolution at the nanoscale. In this paper, polarization-dependent second-harmonic generation [...] Read more.
Understanding strain behavior near grain boundaries is critical for controlling structural distortions and oxygen vacancy migration in perovskite oxides. However, conventional techniques often lack the spatial resolution needed to analyze phase and domain evolution at the nanoscale. In this paper, polarization-dependent second-harmonic generation (SHG) imaging is employed as a tool to probe local symmetry breaking and complex domain structures in the vicinity of a low-angle grain boundary of SrTiO3 (STO) bicrystals. We show that the anisotropic strain introduced by a tilted grain boundary produces strong local distortions, leading to the coexistence of tetragonal and rhombohedral domains. By analyzing SHG intensity and variations in the second-order nonlinear optical susceptibility, we map the distribution of strain fields and domain configurations near the boundary. In pristine samples, the grain boundary acts as a localized source of strain accumulation and symmetry breaking, while in samples subjected to intentional electrical stressing, the SHG response becomes broader and more uniform, suggesting strain relaxation. This work highlights SHG imaging as a powerful technique for visualizing grain-boundary-driven structural changes, with broad implications for the design of strain-engineered functional oxide devices. Full article
(This article belongs to the Collection Featured Articles for Surfaces)
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13 pages, 2985 KiB  
Article
Characterization of the Second Harmonic Generation of Boron Nitride Nanotube Macroscopic Assemblies
by Ping Lu, Jingwen Guan, Cyril Hnatovsky, Huimin Ding, Kasthuri De Silva, Liliana Gaburici, Christopher Kingston and Stephen J. Mihailov
Nanomaterials 2025, 15(11), 861; https://doi.org/10.3390/nano15110861 - 3 Jun 2025
Viewed by 695
Abstract
Boron nitride nanotubes (BNNTs) are predicted to be promising one-dimensional nonlinear optical materials, but to date, only one experimental observation has been made using individual nanotubes. In this work, second harmonic generation (SHG) was achieved from free-standing bulk BNNT sheets and BNNT coatings [...] Read more.
Boron nitride nanotubes (BNNTs) are predicted to be promising one-dimensional nonlinear optical materials, but to date, only one experimental observation has been made using individual nanotubes. In this work, second harmonic generation (SHG) was achieved from free-standing bulk BNNT sheets and BNNT coatings on silica substrates. Focusing femtosecond infrared (fs-IR) laser pulses with a wavelength of 800 nm onto the BNNT assemblies resulted in strong SHG at a wavelength of 400 nm. It was observed that due to the thickness variation of the BNNT assemblies and orientational alignment of BNNTs in the assemblies, the intensity of the second-harmonic (SH) radiation changed dramatically when different locations on the samples were investigated. Among all the BNNT assemblies tested, the localized SH response and its dependence on the polarization of the excitation fs-IR pulses were the strongest in BNNT coatings produced by a dip-coating process. By measuring the SH response, the uniformity, reproducibility, and efficiency of BNNT deposition processes could be assessed. For applications requiring a high SH response from BNNT assemblies, the process of dip coating is preferred. Full article
(This article belongs to the Special Issue Linear and Nonlinear Optical Properties of Nanomaterials)
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13 pages, 3143 KiB  
Article
Investigation of the Nonlinear Optical Properties of Silk Fibroin (SF) Using the Z-Scan Method
by Georgi Yankov, Victoria Atanassova, Stefan Karatodorov, Radostin Stefanov, Krum Shumanov, Ekaterina Iordanova, Albena Daskalova, Liliya Angelova and Emil Filipov
Materials 2025, 18(5), 1052; https://doi.org/10.3390/ma18051052 - 27 Feb 2025
Viewed by 767
Abstract
Silk fibroin (SF), the primary protein in silkworm silk, has emerged as a promising organic nonlinear optical material due to its unique combination of optical transparency, biocompatibility, and environmental sustainability. In this study, we investigate the nonlinear optical properties of SF thin films [...] Read more.
Silk fibroin (SF), the primary protein in silkworm silk, has emerged as a promising organic nonlinear optical material due to its unique combination of optical transparency, biocompatibility, and environmental sustainability. In this study, we investigate the nonlinear optical properties of SF thin films using the z-scan technique with femtosecond laser pulses (35 fs, 800 nm, 1 kHz). Our results reveal a strong self-defocusing effect (negative nonlinear refractive index) and significant multiphoton absorption, demonstrating SF’s tunable nonlinear response. Additionally, optical transmittance measurements confirm SF’s partial transparency in the deep UV region, enhancing its potential for second-harmonic generation (SHG) and efficient light frequency conversion. These findings address a key knowledge gap in nonlinear optics, positioning SF as a versatile biopolymer for advanced photonic applications. Full article
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25 pages, 4658 KiB  
Review
Nonlinear Optics in Two-Dimensional Magnetic Materials: Advancements and Opportunities
by Ziqian Xin, Bingyuan Xue, Wenbo Chang, Xinping Zhang and Jia Shi
Nanomaterials 2025, 15(1), 63; https://doi.org/10.3390/nano15010063 - 2 Jan 2025
Cited by 1 | Viewed by 1851
Abstract
Nonlinear optics, a critical branch of modern optics, presents unique potential in the study of two-dimensional (2D) magnetic materials. These materials, characterized by their ultra-thin geometry, long-range magnetic order, and diverse electronic properties, serve as an exceptional platform for exploring nonlinear optical effects. [...] Read more.
Nonlinear optics, a critical branch of modern optics, presents unique potential in the study of two-dimensional (2D) magnetic materials. These materials, characterized by their ultra-thin geometry, long-range magnetic order, and diverse electronic properties, serve as an exceptional platform for exploring nonlinear optical effects. Under strong light fields, 2D magnetic materials exhibit significant nonlinear optical responses, enabling advancements in novel optoelectronic devices. This paper outlines the principles of nonlinear optics and the magnetic structures of 2D materials, reviews recent progress in nonlinear optical studies, including magnetic structure detection and nonlinear optical imaging, and highlights their role in probing magnetic properties by combining second harmonic generation (SHG) and multispectral integration. Finally, we discuss the prospects and challenges for applying nonlinear optics to 2D magnetic materials, emphasizing their potential in next-generation photonic and spintronic devices. Full article
(This article belongs to the Special Issue Nonlinear Optics in Low-Dimensional Nanomaterials)
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11 pages, 10802 KiB  
Article
Simultaneous 3D Construction and Imaging of Plant Cells Using Plasmonic Nanoprobe-Assisted Multimodal Nonlinear Optical Microscopy
by Kun Liu, Yutian Lei and Dawei Li
Nanomaterials 2023, 13(19), 2626; https://doi.org/10.3390/nano13192626 - 23 Sep 2023
Cited by 2 | Viewed by 1637
Abstract
Nonlinear optical (NLO) imaging has emerged as a promising plant cell imaging technique due to its large optical penetration, inherent 3D spatial resolution, and reduced photodamage; exogenous nanoprobes are usually needed for nonsignal target cell analysis. Here, we report in vivo, simultaneous 3D [...] Read more.
Nonlinear optical (NLO) imaging has emerged as a promising plant cell imaging technique due to its large optical penetration, inherent 3D spatial resolution, and reduced photodamage; exogenous nanoprobes are usually needed for nonsignal target cell analysis. Here, we report in vivo, simultaneous 3D labeling and imaging of potato cell structures using plasmonic nanoprobe-assisted multimodal NLO microscopy. Experimental results show that the complete cell structure can be imaged via the combination of second-harmonic generation (SHG) and two-photon luminescence (TPL) when noble metal silver or gold ions are added. In contrast, without the noble metal ion solution, no NLO signals from the cell wall were acquired. The mechanism can be attributed to noble metal nanoprobes with strong nonlinear optical responses formed along the cell walls via a femtosecond laser scan. During the SHG-TPL imaging process, noble metal ions that crossed the cell wall were rapidly reduced to plasmonic nanoparticles with the fs laser and selectively anchored onto both sides of the cell wall, thereby leading to simultaneous 3D labeling and imaging of the potato cells. Compared with the traditional labeling technique that needs in vitro nanoprobe fabrication and cell labeling, our approach allows for one-step, in vivo labeling of plant cells, thus providing a rapid, cost-effective method for cellular structure construction and imaging. Full article
(This article belongs to the Special Issue Nonlinear Optics in Low-Dimensional Nanomaterials)
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11 pages, 1426 KiB  
Article
Laser-Activated Second Harmonic Generation in Flexible Membrane with Si Nanowires
by Viktoriia Mastalieva, Vladimir Neplokh, Arseniy Aybush, Vladimir Fedorov, Anastasiya Yakubova, Olga Koval, Alexander Gudovskikh, Sergey Makarov and Ivan Mukhin
Nanomaterials 2023, 13(9), 1563; https://doi.org/10.3390/nano13091563 - 6 May 2023
Cited by 3 | Viewed by 2469
Abstract
Nonlinear silicon photonics has a high compatibility with CMOS technology and therefore is particularly attractive for various purposes and applications. Second harmonic generation (SHG) in silicon nanowires (NWs) is widely studied for its high sensitivity to structural changes, low-cost fabrication, and efficient tunability [...] Read more.
Nonlinear silicon photonics has a high compatibility with CMOS technology and therefore is particularly attractive for various purposes and applications. Second harmonic generation (SHG) in silicon nanowires (NWs) is widely studied for its high sensitivity to structural changes, low-cost fabrication, and efficient tunability of photonic properties. In this study, we report a fabrication and SHG study of Si nanowire/siloxane flexible membranes. The proposed highly transparent flexible membranes revealed a strong nonlinear response, which was enhanced via activation by an infrared laser beam. The vertical arrays of several nanometer-thin Si NWs effectively generate the SH signal after being exposed to femtosecond infrared laser irradiation in the spectral range of 800–1020 nm. The stable enhancement of SHG induced by laser exposure can be attributed to the functional modifications of the Si NW surface, which can be used for the development of efficient nonlinear platforms based on silicon. This study delivers a valuable contribution to the advancement of optical devices based on silicon and presents novel design and fabrication methods for infrared converters. Full article
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10 pages, 1830 KiB  
Article
Synthesis, Crystal and Electronic Structures, Nonlinear Optical Properties, and Magnetic Properties of Two Thiophosphates: KInP2S7 and KCrP2S7
by Craig Cropek, Vivian Nguyen, Santosh Karki Chhetri, Jin Hu, Shengping Guo and Jian Wang
Crystals 2022, 12(11), 1505; https://doi.org/10.3390/cryst12111505 - 22 Oct 2022
Cited by 6 | Viewed by 3253
Abstract
Two thiophosphates, KInP2S7 and KCrP2S7, were structurally characterized without investigating any optical properties. Herein in this work, KInP2S7 and KCrP2S7 were revisited to investigate their optical and magnetic properties, respectively. [...] Read more.
Two thiophosphates, KInP2S7 and KCrP2S7, were structurally characterized without investigating any optical properties. Herein in this work, KInP2S7 and KCrP2S7 were revisited to investigate their optical and magnetic properties, respectively. Pure polycrystalline samples and crystals of KInP2S7 and KCrP2S7 were grown by high temperature solid state reactions, where mm-sized crystals of KCrP2S7 were collected. KCrP2S7 is isostructural to KInP2S7, which features a layered structure. KInP2S7 and KCrP2S7 possess close relationship to the layered thiophosphate M2P2S6 (M = Fe, Co, Zn, etc.). The bonding pictures of KInP2S7 were studied using the electron localization function (ELF) coupled with crystal orbital Hamilton population (COHP) calculations. The intrinsically distorted [PS4] tetrahedra and [InS6] octahedra are made by strong covalent P-S interactions and ionic In-S interactions, respectively. Electronic structure analysis confirmed that the optical properties of KInP2S7 are mainly contributed to by [PS4] tetrahedra together with small amounts of the contributions coming from [InS6] octahedra. Magnetic measurement on mm-sized crystals of KCrP2S7 verified that there is an antiferromagnetic transition around 21 K, and the Cr atoms are trivalent. KInP2S7 is predicated to be an indirect bandgap semiconductor of 2.38 eV, which is confirmed by the UV-Vis measurement of 2.4(1) eV. KInP2S7 is not a type-I phase-matching material and exhibits moderate second harmonic generation (SHG) response (0.51 × AgGaS2, sample of particle size of 100 µm). The laser damage threshold (LDT) of KInP2S7 is very high of 5.2 × AgGaS2. Bandgap engineering were undergone to enhance the SHG response of KInP2S7. Full article
(This article belongs to the Special Issue Recent Advances in Nonlinear Optical Crystals)
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9 pages, 1810 KiB  
Communication
Femtosecond Laser Fabrication of Hybrid Metal-Dielectric Structures with Nonlinear Photoluminescence
by Ekaterina Ponkratova, Eduard Ageev, Filipp Komissarenko, Sergei Koromyslov, Dmitry Kudryashov, Ivan Mukhin, Vadim Veiko, Aleksandr Kuchmizhak and Dmitry Zuev
Photonics 2021, 8(4), 121; https://doi.org/10.3390/photonics8040121 - 13 Apr 2021
Cited by 5 | Viewed by 3348
Abstract
Fabrication of hybrid micro- and nanostructures with a strong nonlinear response is challenging and represents a great interest due to a wide range of photonic applications. Usually, such structures are produced by quite complicated and time-consuming techniques. This work demonstrates laser-induced hybrid metal-dielectric [...] Read more.
Fabrication of hybrid micro- and nanostructures with a strong nonlinear response is challenging and represents a great interest due to a wide range of photonic applications. Usually, such structures are produced by quite complicated and time-consuming techniques. This work demonstrates laser-induced hybrid metal-dielectric structures with strong nonlinear properties obtained by a single-step fabrication process. We determine the influence of several incident femtosecond pulses on the Au/Si bi-layer film on produced structure morphology. The created hybrid systems represent isolated nanoparticles with a height of 250–500 nm exceeding the total thickness of the Au-Si bi-layer. It is shown that fabricated hybrid nanostructures demonstrate enhancement of the SHG signal (up to two orders of magnitude) compared to the initial planar sample and a broadband photoluminescence signal (more than 200 nm in width) in the visible spectral region. We establish the correlation between nonlinear signal and phase composition provided by Raman scattering measurements. Such laser-induced structures have significant potential in optical sensing applications and can be used as components for different nanophotonic devices. Full article
(This article belongs to the Special Issue Advanced/Novel Photonics Nanostructures)
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13 pages, 2359 KiB  
Article
Effect of UV-Irradiation and ZnO Nanoparticles on Nonlinear Optical Response of Specific Photochromic Polymers
by Karolina Waszkowska, Tarek Chtouki, Oksana Krupka, Vitaliy Smokal, Viviana Figà and Bouchta Sahraoui
Nanomaterials 2021, 11(2), 492; https://doi.org/10.3390/nano11020492 - 16 Feb 2021
Cited by 15 | Viewed by 3128
Abstract
A series of methacrylic styrylquinoline polymers have been synthesized and characterized by spectroscopic and nonlinear optical (NLO) investigations. The NLO properties of studied polymer compounds in the form of thin films prepared by a spin coating method have been investigated by means of [...] Read more.
A series of methacrylic styrylquinoline polymers have been synthesized and characterized by spectroscopic and nonlinear optical (NLO) investigations. The NLO properties of studied polymer compounds in the form of thin films prepared by a spin coating method have been investigated by means of second and third harmonic generation via Maker fringe setup with a laser source at 1064 nm and a pulse duration of 30 ps. The results show strong second harmonic signal dependence on polarization configurations. This second harmonic generation (SHG) response was enhanced by UV-irradiation at 366 nm and doping by ZnO nanoparticles (NPs) (100 nm), while the opposite effect was achieved for a third harmonic generation experiment. Thus, values of second and third order nonlinear susceptibilities were determined by theoretical calculations based on comparative models. The remarkable NLO results presented in this paper expose potential optoelectronic and photonic applications. Full article
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11 pages, 2395 KiB  
Article
Influences of Ga Doping on Crystal Structure and Polarimetric Pattern of SHG in ZnO Nanofilms
by Hua Long, Ammar Ayesh Habeeb, Dickson Mwenda Kinyua, Kai Wang, Bing Wang and Peixiang Lu
Nanomaterials 2019, 9(6), 905; https://doi.org/10.3390/nano9060905 - 21 Jun 2019
Cited by 8 | Viewed by 4437
Abstract
The second-harmonic generation (SHG) in gallium doped ZnO (GZO) nanofilms was studied. The Ga doping in GZO nanofilms influenced the crystal structure of the films, which affected SHG characteristics of the nanofilms. In our experiments, a strong SHG response was obtained in GZO [...] Read more.
The second-harmonic generation (SHG) in gallium doped ZnO (GZO) nanofilms was studied. The Ga doping in GZO nanofilms influenced the crystal structure of the films, which affected SHG characteristics of the nanofilms. In our experiments, a strong SHG response was obtained in GZO nanofilms, which was excited by 790 nm femtosecond laser. It was observed that the Ga doping concentrations affected, not only the intensity, but also the polarimetric pattern of SHG in GZO nanofilms. For 5.0% doped GZO films, the SHG intensity increased about 70%. The intensity ratio of SHG between the incident light polarization angle of 90° and 0°changed with the Ga doping concentrations. It showed the most significant increase for 7.3% doped GZO films, with an increased ratio of c/a crystal constants. This result was attributed to the differences of the ratios of d33/d31 (the second-order nonlinear susceptibility components) induced by the crystal distortion. The results are helpful to investigate nanofilms doping levels and crystal distortion by SHG microscopy, which is a non-destructive and sensitive method. Full article
(This article belongs to the Special Issue Synthesis and Modification of Nanostructured Thin Films)
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14 pages, 2162 KiB  
Article
Rb2Na(NO3)3: A Congruently Melting UV-NLO Crystal with a Very Strong Second-Harmonic Generation Response
by Guohong Zou, Chensheng Lin, Hyung Gu Kim, Hongil Jo and Kang Min Ok
Crystals 2016, 6(4), 42; https://doi.org/10.3390/cryst6040042 - 13 Apr 2016
Cited by 67 | Viewed by 7629
Abstract
Crystals of congruently melting noncentrosymmetric (NCS) mixed alkali metal nitrate, Rb2Na(NO3)3, have been grown through solid state reactions. The material possesses layers with NaO8 hexagonal bipyramids and NO3 triangular units. Rb+ cations are residing [...] Read more.
Crystals of congruently melting noncentrosymmetric (NCS) mixed alkali metal nitrate, Rb2Na(NO3)3, have been grown through solid state reactions. The material possesses layers with NaO8 hexagonal bipyramids and NO3 triangular units. Rb+ cations are residing in the interlayer space. Each NaO8 hexagonal bipyramid shares its corners and edges with two and three NO3 units, respectively, in order to fulfill a highly dense stacking in the unit cell. The NaO8 groups share their six oxygen atoms in equatorial positions with three different NO3 groups to generate a NaO6-NO3 layer with a parallel alignment. The optimized arrangement of the NO3 groups and their high density in the structure together produce a strong second-harmonic generation (SHG) response. Powder SHG measurements indicate that Rb2Na(NO3)3 has a strong SHG efficiency of five times that of KH2PO4 (KDP) and is type I phase-matchable. The calculated average nonlinear optical (NLO) susceptibility of Rb2Na(NO3)3 turns out to be the largest value among the NLO materials composed of only [NO3] anion. In addition, Rb2Na(NO3)3 exhibits a wide transparency region ranging from UV to near IR, which suggests that the compound is a promising NLO material. Full article
(This article belongs to the Special Issue Nonlinear Optical Crystals)
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