Article
Chemistry, Multidisciplinary
Wei-Jie Xie, Ru-Ling Tang, Sheng-Nan Yan, Nan Ma, Chun-Li Hu, Jiang-Gao Mao
Summary: Discovering new DUV nonlinear optical materials is a current research focus. However, integrating stringent performances, such as wide band gap and large NLO coefficient, into a crystal is challenging due to their natural incompatibility. This study proposes a boron-rich closed-loop strategy and successfully designs and synthesizes a new barium borate material, Ba4B14O25, which exhibits excellent NLO properties and holds promise as a DUV-transparent NLO candidate.
Article
Materials Science, Ceramics
R. S. Bubnova, A. P. Shablinskii, S. Yu Stefanovich, M. Yu Arsent'ev, M. G. Krzhizhanovskaya, B. I. Lazoryak, V. L. Ugolkov, S. K. Filatov
Summary: This paper presents the synthesis, crystal structure, and characterization of several new noncentrosymmetric rare-earth borates of the gaudefroyite family Sr2MBi(REEO)3(BO3)4 (M = Ca, Sr, Ba; REE = Y, Eu). Sr2MBi (YO)3(BO3)4 (M = Ca, Sr, Ba) borates were synthesized through multi-step solid state reactions. The crystal structures of Sr3Bi(YO)3(BO3)4, Sr2CaBi(YO)3(BO3)4, and Sr2BaBi(YO)3(BO3)4 were refined and their thermal expansion coefficients were calculated. Second-harmonic generation measurements showed an increase in the nonlinear optical activity of the materials when Sr was partially substituted with Ca and Ba, and a decrease when Y atoms were replaced by Eu.
CERAMICS INTERNATIONAL
(2023)
Article
Chemistry, Multidisciplinary
Yu Chu, Hongshan Wang, Tudi Abutukadi, Zhi Li, Miriding Mutailipu, Xin Su, Zhihua Yang, Junjie Li, Shilie Pan
Summary: An unprecedented wide bandgap Hg-based IR NLO material Zn2HgP2S8 (ZHPS) with diamond-like structure is rationally designed and fabricated by a tetrahedron re-organization strategy with the aid of structure and property predictions. ZHPS exhibits a wide bandgap of 3.37 eV, which is the largest one among the reported Hg-based chalcogenide IR NLO materials and first breaks the 3.0 eV bandgap wall in this system, resulting in a high laser-induced damage threshold (LIDT) of similar to 2.2 x AgGaS2 (AGS). Meanwhile, it shows a large NLO response (1.1 x AGS), achieving a good balance between bandgap (>= 3.0 eV) and NLO effect (>= 1 x AGS) for an excellent IR NLO material.
Article
Crystallography
Runqing Liu, Hongping Wu, Hongwei Yu, Zhanggui Hu, Jiyang Wang, Yicheng Wu
Summary: CIBO is a new noncentrosymmetric cadmium indium borate with good optical and thermal properties. Its structure includes distorted InO6 and CdOn polyhedra and exhibits strong second harmonic generation and moderate birefringence due to the approximately parallel arrangement of BO3 triangles.
Article
Optics
Junjun Ma, Fei Xie, Weijin Chen, Jiaxin Chen, Wei Wu, Wei Liu, Yuntian Chen, Wei Cai, Mengxin Ren, Jingjun Xu
Summary: LN metasurfaces with controllable SHG properties have been experimentally demonstrated, showing distinct enhancements for the SHG efficiency at Mie resonances. By changing geometric parameters and resonances of metasurfaces, authors manage to selectively boost the SHG efficiency at different wavelengths, paving the way for developing novel compact nonlinear light sources with high flexibility for applications like biosensing and optical communications.
LASER & PHOTONICS REVIEWS
(2021)
Article
Optics
Marc Jankowski, Carsten Langrock, Boris Desiatov, Marko Loncar, M. M. Fejer
Summary: We propose a new approach to supercontinuum generation and carrier-envelope-offset detection based on saturated second-order nonlinear interactions in dispersion-engineered nanowaveguides. The technique developed here broadens the interacting harmonics by forming stable bifurcations of the pulse envelopes due to an interplay between phase-mismatch and pump depletion. The scaling laws suggest that future realization based on this approach could enable supercontinuum generation with orders of magnitude less energy than current state-of-the-art devices.
Article
Chemistry, Physical
Xuefei Wang, Yang Li, Zilong Chen, Jihyun Lee, Fangfang Zhang, Kenneth R. Poeppelmeier, Shilie Pan, Kang Min Ok
Summary: In this study, a novel nonlinear optical material Sr(NO3)(NH2SO3).H2O was successfully designed and synthesized. The compound exhibits unique structure, excellent second harmonic generation response, and optimized birefringence. It also forms large single crystals. This discovery introduces a new class of NLO materials and significantly expands the scope of structural chemistry.
Article
Nanoscience & Nanotechnology
Hongkun Liu, Bingbing Zhang, Ling Li, Ying Wang
Summary: Deep-UV nonlinear optical (NLO) materials are crucial for demanding DUV laser applications, and the two synthesized fluoroaluminoborates exhibit NLO activity with short UV cutoff edges. Despite having the same fundamental structural units, their crystal structures and second harmonic generation (SHG) responses differ significantly due to the cation effect.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Nanoscience & Nanotechnology
Jicheng Jin, Jian Lu, Bo Zhen
Summary: Second harmonic dipoles generated in a nonlinear photonic crystal slab can be completely nonradiative, resulting in no energy transfer from the fundamental frequency to the second harmonic even when the phase-matching condition is satisfied - a phenomenon known as resonance-forbidden second-harmonic generation. Through numerical simulation, two mechanisms for achieving this phenomenon have been identified: symmetry protection and parameter tuning. The finite-size effect and the topological origin of this phenomenon are also discussed.
Article
Materials Science, Multidisciplinary
Mengran Sun, Chunxiao Li, Jinlong Shi, Ming-Hsien Lee, Jiyong Yao
Summary: This study investigates the structural characteristics and nonlinear optical (NLO) properties of defect diamond-like (DL) MGa2Te4 (M = Zn, Cd) for the first time. The results show that MGa2Te4 (M = Zn, Cd) has moderate band gaps, strong second harmonic generation (SHG) intensities, and congruent-melting behavior. The lone-pair packets of Te ions in [GaTe4] units are found to be the main source of SHG responses. This work demonstrates the potential applications of these two defect DL tellurides in the mid- and far-infrared (MFIR) NLO field.
MATERIALS TODAY PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Yoonsoo Rho, SeokJae Yoo, Daniel B. Durham, DongJun Kang, Andrew M. Minor, Costas P. Grigoropoulos
Summary: Nonlinear optical response is a useful tool for studying the properties of materials, but its weak signal and limited reach make it difficult to probe deep-subwavelength-scale nonlinear optics. In this study, we propose a new method using an SHG-active plasmonic nanotip to achieve efficient second harmonic generation (SHG) nanoscopy. Our simulations suggest that enhancing the nonlinear response of the sample or suppressing the tip's response can lead to a high near-field SHG contrast, providing evidence of quantum mechanical nonlinear energy transfer. Furthermore, this technique can be used to study nanoscale corrosion and other physicochemical phenomena.
Article
Nanoscience & Nanotechnology
Shuang-Cheng Li, Zi-Long Geng, Rui-Biao Fu, Zu-Ju Ma, Xin-Tao Wu
Summary: Researchers have developed a new nonlinear optical (NLO) crystal, K(H2O)[KI][PbI(C4H4O4)], by modifying halide perovskite materials with a 2-methylmalonate group. This crystal exhibits a highly distorted [PbO4I2] polyhedron with large hyperpolarizability and prominent polarizability anisotropy, serving as a bifunctional unit. The oriented arrangement of the distorted [PbO4I2] polyhedrons leads to the effective superposition of their microscopic second-order nonlinear susceptibilities and enhances optical anisotropy. The crystal demonstrates a strong phase-matching second harmonic generation (SHG) response and a large birefringence, making it a promising candidate for high-performance NLO crystals.
SCRIPTA MATERIALIA
(2024)
Article
Optics
Gia Quyet Ngo, Emad Najafidehaghani, Ziyang Gan, Sara Khazaee, Malte Per Siems, Antony George, Erik P. Schartner, Stefan Nolte, Heike Ebendorff-Heidepriem, Thomas Pertsch, Alessandro Tuniz, Markus A. Schmidt, Ulf Peschel, Andrey Turchanin, Falk Eilenberger
Summary: This study demonstrates a method to achieve second-harmonic generation in functionalized optical fibers by directly growing highly nonlinear MoS2 monolayers on the fiber's core. The approach is scalable and can be generalized to other materials and waveguide systems.
Article
Chemistry, Physical
Jiaxing Du, Jianwei Shi, Chun Li, Qiuyu Shang, Xinfeng Liu, Yuan Huang, Qing Zhang
Summary: Researchers demonstrated a directional second harmonic generation (SHG) amplifier formed by MoS2/WS2 monolayer heterostructures, achieving significant enhancement of SHG and improved radiation angle, attributed to the excitation and emission field concentration induced by a vertical Fabry-Perot microcavity.
Article
Materials Science, Multidisciplinary
Haotian. Tian, Chensheng Lin, Xin Zhao, Shenghao Fang, Han Li, Chao Wang, Ning Ye, Min Luo
Summary: KNO3SO3NH3 is a new polar non-centrosymmetric compound with a strong second-harmonic generation (SHG) response and large birefringence. The enhanced SHG response is attributed to the effect of hydrogen bond according to theoretical calculations. It also has the shortest absorption edge in the UV-visible spectrum among known materials with strong SHG responses.
MATERIALS TODAY PHYSICS
(2022)
Article
Chemistry, Inorganic & Nuclear
Abbey J. Neer, Joanna Milam-Guerrero, Veronika A. Fischer, Michelle Zheng, Nicole R. Spence, Clayton Cozzan, Mingqiang Gu, James M. Rondinelli, Craig M. Brown, Brent C. Melot
Summary: We conducted a comparative study on the magnetic and crystal chemical properties of two Co2+-containing garnets. It was found that CaY2Co2Ge3O12 and NaCa2Co2V3O12 exhibited different magnetic structures and properties under similar external conditions. Crystal-chemistry analyses and density functional theory calculations were performed to explain these differences based on minor changes in the local environment of the Co ions.
INORGANIC CHEMISTRY
(2022)
Article
Multidisciplinary Sciences
Hari Padmanabhan, Maxwell Poore, Peter K. Kim, Nathan Z. Koocher, Vladimir A. Stoica, Danilo Puggioni, Huaiyu (Hugo) Wang, Xiaozhe Shen, Alexander H. Reid, Mingqiang Gu, Maxwell Wetherington, Seng Huat Lee, Richard D. Schaller, Zhiqiang Mao, Aaron M. Lindenberg, Xijie Wang, James M. Rondinelli, Richard D. Averitt, Venkatraman Gopalan
Summary: This study provides evidence for interlayer magnetophononic coupling in layered magnetic topological insulator MnBi2Te4. The anomalies in phonon scattering intensities across magnetic field-driven phase transitions are observed using magneto-Raman spectroscopy, which is attributed to phonons modulating the interlayer exchange coupling. The signatures of magnetophononic coupling are also observed in the time domain through ultrafast excitation and detection of coherent phonons.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Donghoon Shin, Minliang Lai, Yongjin Shin, Jingshan S. S. Du, Liban Jibril, James M. Rondinelli, Chad A. Mirkin
Summary: The stability, reliability, and performance of halide-perovskite-based devices are determined by the structure, composition, and particle size of the device-enabling materials. A new method called evaporation-crystallization polymer pen lithography is used to synthesize and study Cs(0.5)FA(0.5)PbX(3) crystals and discover heterostructure morphology. The heterostructures are formed due to differences in solubility of ions and enthalpic preference for ion segregation, and solid-solution nanocrystals are synthesized to suppress photoinduced anion migration for photostable optoelectronic materials.
ADVANCED MATERIALS
(2023)
Article
Engineering, Mechanical
Akshay Iyer, Suraj Yerramilli, James M. Rondinelli, Daniel W. Apley, Wei Chen
Summary: Engineering design often involves qualitative and quantitative variables. High-dimensional qualitative variables impose a large design cost. We address this challenge by utilizing domain knowledge to infer the effect of unobserved levels. Our method is robust and reduces design cost for problems with high-dimensional qualitative variables.
JOURNAL OF MECHANICAL DESIGN
(2023)
Article
Chemistry, Inorganic & Nuclear
Ming-Li Liang, Matthew Lacroix, Ce Tao, Michael J. Waters, James M. Rondinelli, P. Shiv Halasyamani
Summary: The synthesis and optical properties of noncentrosymmetric (NCS) gamma-Cs2I4O11 were reported, which was obtained through IO4 polyhedral rearrangements from centrosymmetric (CS) beta-Cs2I4O11. Trifluoroacetic acid (TFA) played a key role in the synthesis as a structure-directing agent. The material exhibited strong second-harmonic-generation (SHG) response and was type I phase matchable.
INORGANIC CHEMISTRY
(2023)
Article
Materials Science, Multidisciplinary
Zhaowei Hu, Lili Liu, Ruixin Zhang, Qun Jing, Huan Wang, Jindan Tian, Jiayue Xu, P. Shiv Halasyamani
Summary: The construction of new functional crystals by integrating multiple structural motifs has been achieved. Two compounds with good crystal growth habits and promising UV birefringent properties were synthesized.
JOURNAL OF MATERIALS CHEMISTRY C
(2023)
Article
Nanoscience & Nanotechnology
Megan A. Cassingham, Yang G. Goh, Eric T. McClure, Taylor L. Hodgkins, Weiguo Zhang, Mingli Liang, Jahan M. Dawlaty, Peter I. Djurovich, Ralf Haiges, P. Shiv Halasyamani, Christopher N. Savory, Mark E. Thompson, Brent C. Melot
Summary: We report the growth and photophysical characterization of two polar hybrid lead halide phases, methylenedianiline lead iodide and bromide, (MDA)Pb2I6 and (MDA)Pb2Br6, respectively. The noncentrosymmetric crystal structure of these phases leads to highly oriented molecular dipole moments, resulting in second harmonic generation (SHG) upon excitation at 1064 nm. The size dependence of the SHG signal indicates that the bromide exhibits a stronger phase-matching response while the iodide exhibits a significantly weaker non-phase-matching signal. Fluorescence from (MDA)Pb2Br6 is observed around 630 nm below 75 K, whereas (MDA)Pb2I6 exhibits very weak luminescence. The contrasting optical properties are attributed to differences in the character of the halide sublattice, with the increased polarizability of the iodide ions reducing the local electric field in the crystals.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Assael Cohen, Pranab K. Mohapatra, Simon Hettler, Avinash Patsha, K. V. L. V. Narayanachari, Pini Shekhter, John Cavin, James M. Rondinelli, Michael Bedzyk, Oswaldo Dieguez, Raul Arenal, Ariel Ismach
Summary: Conventional epitaxy is essential for semiconductor technology, but there are still unresolved differences in terms of orientation registry and interface chemistry in quasi-vdW epitaxy. This study focuses on the growth of WS2 using metal-organic chemical vapor deposition (MOCVD) and a metal-seeding approach, which allows for the formation of a continuous WO3 layer on a sapphire substrate. The presence of this interfacial layer strongly influences the subsequent growth of the WS2 layer. This work provides insights into the epitaxial growth mechanism and demonstrates the effectiveness of the metal-seeding approach for the growth of other TMDC layers.
Article
Chemistry, Multidisciplinary
Fenghua Ding, Kent J. Griffith, Weiguo Zhang, Shaoxin Cui, Chi Zhang, Yiran Wang, Kendall Kamp, Hongwei Yu, P. Shiv Halasyamani, Zhihua Yang, Shilie Pan, Kenneth R. Poeppelmeier
Summary: An NCS and chiral mixed-alkali-metal borate with a linear BO2- unit was synthesized and characterized. The structure includes three types of basic building units, [BO2], [BO3], and [BO4], with sp-, sp2-, and sp3-hybridization of boron atoms, respectively. This study expands the small family of NCS structures with the rare linear BO2- unit and highlights the existence of two enantiomers in achiral Sohncke space groups, which has been generally overlooked in NLO materials.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Editorial Material
Optics
P. Shiv Halasyamani
Summary: A nonlinear optical crystal enables the generation of harmonic radiation in the deep ultraviolet region, extending below 200 nm.
Article
Physics, Multidisciplinary
Alexander C. Tyner, Shouvik Sur, Danilo Puggioni, James M. Rondinelli, Pallab Goswami
Summary: In this study, it is discovered that three-dimensional stable Dirac semimetals demonstrate the quantum spin Hall effect, with bound states on n-fold symmetric momentum planes. These planes support the same non-Abelian Berry flux and exhibit identical topological response.
PHYSICAL REVIEW RESEARCH
(2023)
Article
Materials Science, Multidisciplinary
Sean Koyama, James M. Rondinelli
Summary: In this study, a new type of persistent spin texture (PST) material is discovered, called symmetry-assisted PSTs, which can enhance the performance of spintronic devices. Chemical substitution can be used to tune the properties of these materials, such as spin lifetime. Additionally, it is found that existing two-dimensional models are insufficient to fully describe the spin texture state in these materials, indicating the need for higher-order models.
Article
Materials Science, Multidisciplinary
Xue-Zeng Lu, James M. Rondinelli
Summary: Through electronic structure calculations and algebraic representation analysis, we have discovered that high-quality persistent spin textures can be hidden in complex ternary layered and perovskite structures with large electric polarizations, offering potential for future quantum microelectronic devices.
Article
Materials Science, Multidisciplinary
Haonan Liu, Hongping Wu, Zhanggui Hu, Jiyang Wang, Yicheng Wu, P. Shiv Halasyamani, Hongwei Yu
Summary: KBBF is currently the only material capable of producing deep-ultraviolet coherent light, but its rigid growth characteristics and high toxicity make safe growth a major challenge. This study reports a new chemically benign deep-ultraviolet nonlinear optical crystal RBPO, which inherits the structural genes of KBBF and demonstrates comparable optical properties. RBPO can overcome the processing limitations of KBBF and has the potential to become the next generation of deep-ultraviolet nonlinear optical crystals.
ACS MATERIALS LETTERS
(2023)
