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Nonlinear optical (NLO) crystals are indispensable for the solid-state lasers for their ability to expand wavelength spectral to the regions where the directing lasing is difficult or even impossible, yet the rational design of a high-performance NLO crystal remains a great challenge owing to the severe structural and properties' requirements. Herein, a new noncentrosymmetric (NCS) and polar gallium iodate, LiGa(IO3 )4 , with a novel 2D anionic layer, is successfully designed and synthesized by the aliovalent substitution strategy based on classic α-LiIO3 . The 2D [Ga(IO3 )4 ]∞ - layer in LiGa(IO3 )4 is built from the GaO6 octahedra and highly polarizable units IO3 . Compared with its parent compound, the partial replacement of A-site Li+ cation with main group Ga3+ cation facilitates LiGa(IO3 )4 to possess excellent NLO properties, including the large second-harmonic generation (SHG) response (14 × KH2 PO4 (KDP) @ 1064 nm), wide bandgap (4.25 eV), large birefringence (0.23 @ 1064 nm), and wide optical transparency from UV to mid-IR. These reveal that LiGa(IO3 )4 will be a promising NLO crystal.
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Introducing F- anions or substituting F- anions with IO3- groups has been proven to be ideal strategies for designing novel noncentrosymmetric (NCS) and polar materials, yet systematic investigation into the effect of F- anions or the substitution of IO3- for F- anions on structures and properties remains rarely explored. Herein, two new gallium iodates, NaGa(IO3)2F2 (1) and NaGa(IO3)4 (2), were successfully designed and synthesized based on NaGa(IO3)3F by introducing more F- anions and replacing F- anions with IO3 groups, respectively. Structurally, in compound 1, the adjacent [GaF3(IO3)3]3- polyanions are connected in an antiparallel manner, resulting in a complete cancellation of local polarity. While in compound 2, all IO3 groups in 2D [Ga(IO3)4]∞- layers are aligned, leading to large macroscopic polarization. Additionally, chemical substitution also results in a qualitative improvement in the functional properties of compound 2. It possesses strong SHG response (12 × KDP @1064 nm) and broad optical transparency, coupled with large birefringence (0.21 @1064 nm), showcasing its promise as a promising nonlinear optical (NLO) crystal. The effects of chemical substitution between F- anions and IO3- groups on the structures and properties are discussed in detail.
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Nonlinear optical (NLO) coherent light sources are widely applied in many areas of science and technology. As the core medium, the NLO material is required to have a wide transparent range, a large NLO response, and a high laser damaged threshold (LDT). It is common knowledge that langasite (La3Ga5SiO14, LGS) crystal has an underdeveloped second-harmonic generation (SHG) coefficient and a small birefringence, which seriously restrict its application in the NLO field, despite that it has a broad transmittance spectrum and a moderate LDT. Herein, we have successfully obtained novel langasite NLO crystals LGSS (La3Ga5Si0.5Sn0.5O14) and LGGS (La3Ga5Ge0.5Sn0.5O14), with short UV absorption edges of 209 and 212 nm, respectively. Incorporating heavy ions Sn4+ into the structure, a distorted BO6 octahedron was adjusted by the radius difference between Sn4+ and Si4+/Ge4+, which caused the strong SHG responses in LGSS (â¼10.77 × KDP) and LGGS (â¼9.23 × KDP) and increased birefringences of 0.034 and 0.025, respectively. Besides, they also had large energy band gaps (4.95 eV for LGSS, and 4.93 eV for LGGS), which allowed high LDTs with LGSS of 1.3 GW/cm2 and LGGS of 813 MW/cm2. This work demonstrates a new strategy to enhance SHG responses and birefringence for existing NLO materials and enriches langasite family crystals.
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Two new congruently melting Pb-containing halogen silicates, Pb3[O10Pb20](SiO4)4X10 (X = Cl, Br), have been synthesized using a high-temperature solution method. Their crystal structures were determined by single-crystal X-ray diffraction, and both compounds crystallize in the orthorhombic space group Cmca. In both structures, the mirror-symmetric bilayer composed of Pb-O polyhedra is observed for the first time in Pb-containing silicates and belongs to α-PbO derivatives and is related to the Aurivillius phase. Thermal behavior analysis, UV-vis diffuse-reflectance spectroscopy, and IR spectroscopy were also performed. The Pb3[O10Pb20](SiO4)4Cl10 matrix was doped with Eu3+ ions as a dopant, and its potential application in fluorescence was confirmed from the resulting orange-red emission.
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Achieving the extreme balance of the key performance requirements is the crucial to breakthrough the application bottleneck for nonlinear optical (NLO) materials. Herein, by assembly of the π-conjugated [B3O6] functional species with the aid of structure-directing property of mer-isomer [YO3F3] octahedra, a new ultraviolet (UV) NLO material, Cs2YB3O6F2 with aligned arrangement of coplanar [B3O6] groups has been synthesized. The polar material exhibits the rare coexistence of the largest second harmonic generation response of 5.6×KDP, the largest birefringence of 0.091 at 532â nm, the shortest Type I phase-matching down to 200.5â nm and deep-ultraviolet transparency among reported acentric rare-earth borates with [B3O6] groups. Remarkably, benefiting from the enhanced bonding force among functional units [B3O6], a firm three-dimensional framework is constructed, which facilitates the growth of large crystals. This can be proved by a block shape crystal with dimensional of 6×5×4â mm3, indicating that it was a promising UV NLO crystal. This work provides a powerful strategy to design UV NLO materials with good performances.
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Non-centrosymmetric (NCS) and polar materials capable of exhibiting many important functional properties are indispensable for electro-optical technologies, yet their rational structural design remains a significant challenge. Here, we report a "group grafting" strategy for designing the first multi-chromophore selenophosphate, Cs3In(In4Se7)(P2Se6), that crystallizes in a NCS and polar space group of Cm. The structure features a unique basic building unit (BBU) [In(In4Se10)(P2Se6)], formed through "grafting [In4Se10] supertetrahedra on the root of [In(P2Se6)2] groups". Theoretical calculations confirm that this [In(In4Se10)(P2Se6)] BBU can achieve a "1+1>2" combination of properties from two chromophores, [In4Se10] supertetrahedron and ethane-like [P2Se6] dimer. That makes Cs3In(In4Se7)(P2Se6) exhibit excellent linear and nonlinear optical (NLO) properties, including a strong second harmonic generation (SHG) response (~6×AgGaS2), a large band gap (2.45â eV), broad infrared (IR) transmission (up to 19.5â µm), a significant birefringence (0.26 @1064â nm) as well as the congruently-melting property at ~700 °C. Therefore, Cs3In(In4Se7)(P2Se6) will be a promising NLO crystal, especially in the IR region, and this research also demonstrates that "group grafting" will be an effective strategy for constructing novel polar BBUs with multi-chromophore to design NCS structures and high-performance IR NLO materials.
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Deep-ultraviolet nonlinear optical (DUV NLO) crystals are indispensable for solid-state lasers to produce coherent light with wavelengths shorter than 200 nm, yet their structure design still faces great challenges because two groups of conflicting properties must be satisfied simultaneously, i.e., "large second harmonic generation (SHG) response-large band gap" and "large birefringence-weak growth anisotropy". Clearly, hitherto, no crystal can perfectly satisfy these properties, including KBe2BO3F2. Herein, we design a new mixed-coordinated borophosphate Cs3[(BOP)2(B3O7)3] (CBPO) by optimizing the matching of cation and anion groups, which unprecedentedly achieves a balance for two groups of contradictions concurrently for the first time. In the structure of CBPO, it has the coplanar and π-conjugated B3O7 groups, which can make it possess a large SHG response (3 × KDP) and large birefringence (0.075@532 nm). Then, terminal O atoms of these B3O7 groups are connected by BO4 and PO4 tetrahedra, which eliminates all dangling bonds and blue shifts the UV absorption edge to the DUV region (165 nm). More importantly, owing to the judicious selection of cations, the size of cations and void of anion groups is a perfect match, which makes CBPO possess a very stable three-dimensional anion framework and thus reduces the crystal growth anisotropy. A CBPO single crystal with a size of up to 20 × 17 × 8 mm3 has been successfully grown, through which a DUV coherent light has also been achieved in Be-free DUV NLO crystals for the first time. These indicate CBPO will be the next generation of DUV NLO crystals.
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Salt-inclusion chalcogenides (SICs) have been receiving widespread attention due to their large second harmonic generation (SHG) responses and wide bandgaps, however most of them suffer from small birefringence limiting their technical application. Herein, by introducing the π-conjugated (S2 )2- units in the ionic guest of salt-inclusion structure, the first disulfide-bond-containing SIC, [Ba4 (S2 )][ZnGa4 S10 ] has been synthesized. It exhibits the widest bandgap up to 3.39 eV among polychalcogenides and strong SHG response as large as that of AgGaS2 (AGS). Importantly, its birefringence reaches a max value of 0.053@1064 nm among AGS-like SICs, indicating it is a promising IR nonlinear optical (NLO) material. Theoretical calculations reveal that the π-conjugated (S2 )2- units and covalent GaS layers favor the enhanced birefringence and large SHG response. This work provides not only a new type of SIC for the first time, but also new lights on the design of IR NLO materials.
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Infrared nonlinear optical (IR NLO) materials are of great significance in the development of IR laser technology. But rationally designing high-performance IR NLO materials remains a huge challenge due to the conflict between the necessary properties required for NLO materials. Notably, oxychalcogenides with mixed-anion groups have drawn extensive interest as a family of important IR NLO candidates because they integrate the property advantages of oxides and chalcogenides by chemical substitution engineering. In this review, we provide a survey of reported oxychalcogenides and aim to present the development of NLO oxychalcogenides from the perspective of rational design of their structural chemistry. Furthermore, we focus on the relationships between partial substitution and structural symmetry as well as optical properties. These provide some helpful guidance for the further exploration and design of novel oxychalcogenide materials with excellent NLO performance in the future.
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Nonlinear optical (NLO) crystals assume an irreplaceable role in the development of laser science and technologies, yet the reasonable design of a high-performance NLO crystal remains difficult owing to the unpredictability of inorganic structures. In this research, we report the fourth polymorph of KMoO3(IO3), i.e., δ-KMoO3(IO3), to understand the effect of different packing patterns of basic building units on structures and properties. Among four polymorphs of KMoO3(IO3), the different stacking patterns of Λ-shaped cis-MoO4(IO3)2 units result in α- and ß-KMoO3(IO3) featuring nonpolar layered structures, whereas γ- and δ-KMoO3(IO3) display polar frameworks. Theoretical calculations and structure analysis reveal that IO3 units can be regarded as the main source of its polarization in δ-KMoO3(IO3). Further property measurements show that δ-KMoO3(IO3) exhibits a large second-harmonic generation response (6.6 × KDP), a wide band gap (3.34 eV), and a broad mid-infrared transparency region (â¼10 µm), which demonstrates that adjusting the arrangement of the Λ-shaped basic building units is an effective approach for rationally designing NLO crystals.
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Inorganic phosphates are of great interest, because of their rich structural chemistry and multiple functional properties. Compared with the phosphates that only contain the solely condensed P-O groups, the phosphates with various condensed P-O groups are less reported, especially for the noncentrosymmetric (NCS) ones. Here, two new bismuth phosphates, Na6Sr2Bi3(PO4)(P2O7)4 and Cs2CaBi2(PO4)2(P2O7), were synthesized by the solid-state reaction and both structures contain two types of isolated P-O groups. Remarkably, Na6Sr2Bi3(PO4)(P2O7)4 crystallizes in the tetragonal space group P4Ì 21c, which represents the first NCS bismuth phosphate with PO4 and P2O7 groups. Detailed structural comparisons among Bi3+-containing alkali/alkaline-earth metal phosphates show that the ratios of cations/phosphorus profoundly influence the condensed degree of P-O groups. Ultraviolet-visible-near-infrared (UV-vis-NIR) diffusion spectra show that both compounds have the relatively short UV cutoff edges. And Na6Sr2Bi3(PO4)(P2O7)4 has a second-harmonic generation response of 1.1 × KDP. The first-principles calculations are carried out to understand the structure-performance relationship.
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Infrared nonlinear optical (IR NLO) crystals play a significant role in the development of IR laser technology. But rationally designing a new IR NLO crystal remains a huge challenge because of the unpredictability of inorganic structures. Herein, inspired by phase transformation of the famous BaB2 O4 (BBO) crystal, a temperature-induced centrosymmetric (CS) to noncentrosymmetric (NCS) transformation approach is employed in CS BaGa2 Se4 to uncover a new NCS ternary chalcogenide, ß-BaGa2 Se4 which can exhibit the well-balanced NLO properties, including moderate phase-matching SHG response (≈0.6×AgGaS2 ), high LDT (10×AgGaS2 ), and large birefringence (Δn=0.18 in the visible region). Therefore, ß-BaGa2 Se4 will be a promising IR NLO crystal. The analysis for the structure-property relationship shows that the excellent NLO properties of ß-BaGa2 Se4 mainly originate from edge-sharing GaSe4 tetrahedral chains, which are different from B3 O6 groups in ß-BBO and respect a new direction for the design of IR NLO crystals. So, we believe that the current research provides not only a new IR NLO crystal but also some insights for the design of new IR NLO crystals.
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Inorganic heteroanionic materials are attracting increasing attention for exploring new nonlinear optical (NLO) materials because they could better satisfy the necessary but conflicting properties of NLO crystals, e.g. large SHG response and wide band-gap. Up to now, the reports on heteroanionic NLO materials have mainly focused on ultraviolet or visible oxide-based fluoroborates, fluorophosphates, borate-phosphates and borate-iodates. However, chalcogenides containing different kinds of anionic groups have barely been reported. Herein, we have synthesized the first oxychalcogenide-carbonate, Sr3 [SnOSe3 ][CO3 ] that contains two different kinds of anionic groups, [SnOSe3 ] and [CO3 ]. It crystallizes in a noncentrosymmetric space group and exhibits fascinating NLO properties, including a large SHG response (≈1×AGS), sufficient birefringence (0.12 @1064â nm), wide band-gap (3.46â eV) and high laser damage threshold (240â MW cm-2 ). These make Sr3 [SnOSe3 ][CO3 ] a promising NLO crystal.
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BACKGROUND: Left bundle branch (LBB) pacing has emerged as a novel pacing modality. Left ventricular activation time (LVAT) was reported to be associated with the activation via LBB, but the value of LVAT for determining LBB pacing was unknown. We conducted a pilot study to determine if LVAT could define LBB capture by validating left ventricular (LV) mechanical synchrony. METHODS: We analyzed LVAT in 68 bradycardia-indicated patients who received LBB pacing. LVAT was measured from the stimulus to R-wave peak in lead V5 and V6. LV mechanical synchrony assessed by SPECT MPI was compared according to the value of LVAT and the presence of LBB potential. RESULTS: The mean LVAT was 75.4 ± 12.7 ms. LBB potential was recorded in 47 patients (69.1%). Patients with LVAT < 76 ms had better LV mechanical synchrony than those with LVAT ≥ 76 ms. Patients with LVAT < 76 ms or LBB potential had better mechanical synchrony than those with LVAT ≥ 76 ms and no potential. LVAT < 76 ms could predict the normal synchrony with a sensitivity of 88.9% and a specificity of 87.5%. CONCLUSION: A short LVAT indicated favorable mechanical synchrony in SPECT imaging. LVAT < 76 ms might be a practical parameter for defining LBB capture.
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Arritmias Cardíacas/terapia , Estimulação Cardíaca Artificial , Sistema de Condução Cardíaco/fisiopatologia , Disfunção Ventricular Esquerda/diagnóstico por imagem , Disfunção Ventricular Esquerda/fisiopatologia , Idoso , Arritmias Cardíacas/diagnóstico por imagem , Arritmias Cardíacas/fisiopatologia , Tomografia Computadorizada por Emissão de Fóton Único de Sincronização Cardíaca , Feminino , Humanos , Masculino , Pessoa de Meia-Idade , Imagem de Perfusão do Miocárdio , Projetos Piloto , Valor Preditivo dos Testes , Reprodutibilidade dos Testes , Septo InterventricularRESUMO
The birefringent crystals capable of modulating the polarization of lights are of the current research interests. Although many oxide crystals have been discovered and widely used in UV and visible regions, the birefringent crystals in the infrared (IR) region are still rare. Herein, two new chalcogenides, K2Na2Sn3S8 and Rb3NaSn3Se8, have been synthesized by the solid-state method. We have used the single crystal X-ray diffraction to determine their structures. K2Na2Sn3S8 crystallizes in the monoclinic space group C2/c and exhibits a three-dimensional framework constructed by the corner-sharing SnS4 and SnS5 units, whereas Rb3NaSn3Se8 crystallizes in the tetragonal space group P4/nbm and features a zero-dimensional [Sn3Se8]4- trimer built by the three edge-sharing SnSe4 tetrahedra. The physical property measurements indicate that Rb3NaSn3Se8 has a wide IR transparent window up to 20 µm and large birefringence, â¼0.196, suggesting its potential application as a birefringent crystal in the IR region. However, compared with Rb3NaSn3Se8, the birefringence of K2Na2Sn3S8 is relatively small, â¼0.070. The study of their structure-property relationship indicates that the different connection modes of SnQn (Q = S, Se; n = 4, 5) polyhedra are the main reason for the large difference of birefringence between the two compounds. These studies will provide a new insight for the origin of birefringence and will facilitate the exploration of new IR birefringent crystals.
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BACKGROUND: Chronic right ventricular (RV) pacing is associated with an increased incidence of heart failure and mortality. Left bundle branch (LBB) pacing could produce near-physiological electrical activation and mechanical synchrony. We aimed to report the effects of upgrading to LBB pacing in heart failure patients after chronic RV pacing. METHODS: The indications included pacing-induced cardiomyopathy (PICM) in Group 1 and heart failure after RV pacing with left ventricular ejection fraction (LVEF) ≥ 50% in Group 2. LBB pacing was achieved by penetrating the pacing lead to the subendocardium of left-sided interventricular septum through the venous access. Left ventricular activation time (LVAT) was measured from the pacing stimulus to the ascending peak of lead V5 or V6. All patients underwent clinical and echocardiographic evaluations before and after upgrading. RESULTS: Totally 27 patients (13 in Group 1 and 14 in Group 2) were consecutively enrolled. The mean follow-up time after upgrade was 10.4 ± 6.1 months. Paced QRS duration was significantly shortened from 174.1 ± 15.8 milliseconds to 116.6 ± 11.7 milliseconds (p < .0001). The mean LVAT was 83.2 ± 11.7 milliseconds. LVEF increased from 40.3 ± 5.2% before upgrading to 48.1 ± 9.5% at follow-up in patients with PICM. Serum N-terminal probrain natriuretic peptide levels decreased and New York Heart Association classification improved in both groups. No upgrade-related complications were observed. CONCLUSIONS: Upgrading to LBB pacing was feasible and effective with improved cardiac function in heart failure patients with both reduced and preserved LVEF after RV pacing.
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Fascículo Atrioventricular/fisiopatologia , Estimulação Cardíaca Artificial/métodos , Insuficiência Cardíaca/fisiopatologia , Insuficiência Cardíaca/terapia , Disfunção Ventricular Direita/fisiopatologia , Disfunção Ventricular Direita/terapia , Idoso , Estimulação Cardíaca Artificial/efeitos adversos , Feminino , Sistema de Condução Cardíaco/fisiopatologia , Humanos , Masculino , Volume SistólicoRESUMO
Hepatocytes are the main cell components of the liver and perform metabolic, detoxification, and endocrine functions. Functional hepatocytes are of great value in drug development, toxicity evaluation, and cell therapy for liver diseases. In recent years, an increasing number of in vitro models have been developed to screen drugs and test their toxicity. However, maintaining hepatocyte function in vitro for a long time is a serious challenge. Even freshly isolated liver cells cultured for a short time may lose function via spontaneous dedifferentiation. Thus, novel cell culture systems allowing extended hepatocyte maintenance and more predictive long-term in vitro studies are required. In this study, we developed a conditioned culture system composed of a small-molecule combination that can maintain hepatocyte morphology and functions over the long term. Two-month culture of primary human hepatocytes showed that the conditioned medium was able to stably preserve hepatic functions such as albumin and α-antitrypsin secretion, hepatic transport activity, urea synthesis, and ammonia elimination. Furthermore, this culture model can be used to assess drug-induced hepatotoxicity in vitro. In summary, our work suggests a feasible approach to maintain hepatocyte function in vitro and proposes a promising model for long-term toxicological studies and drug development.
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Doença Hepática Induzida por Substâncias e Drogas , Hepatopatias , Células Cultivadas , Doença Hepática Induzida por Substâncias e Drogas/etiologia , Doença Hepática Induzida por Substâncias e Drogas/metabolismo , Hepatócitos/metabolismo , Humanos , Fígado/metabolismo , Hepatopatias/metabolismoRESUMO
Rationally designing a high-performance nonlinear optical (NLO) crystal remains a great ongoing challenge. It involves not only the design of noncentrosymmetric structures but also property optimization. In this communication, a new strategy for effectively designing the NLO crystal has been put forward, that is, using the structure-directing property of oxyfluoride anions to obtain a noncentrosymmetric and polar structure, and then by substitution of IO3 - for isovalent F- anions to further enhance the SHG response. With this strategy, a new iodate fluoride, Ba2 [MoO3 F(IO3 )](MoO3 F2 ) has been successfully designed from the Ba2 (MoO3 F2 )F2 with the cis-directing [MoO4 F2 ]4- groups. It exhibits a large SHG response (≈8×KDP), a wide transparent region (0.30-10.92â µm), a high laser-induced damage threshold (LDT) (88.53â MW cm-2 ), and a large birefringence (≈0.264@532â nm). These indicate Ba2 [MoO3 F(IO3 )](MoO3 F2 ) would be a promising NLO crystal.
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Tumor microenvironment (TME) is a critical determinant for hepatocellular carcinoma (HCC). Hepatic stellate cells (HSCs) are main interstitial cells in TME and play a vital role in early intrahepatic invasion and metastasis of HCC. The potential mechanism on the interactions between HSCs and HCC cells remains unclear. In this study, the effects of extracellular vesicles (EVs)-derived OncomiRs that mediate communication between HCC cells and cancer-associated hepatic stellate cells (caHSCs) and remold TME were investigated. The results found that the HCC cells-released EVs contained more various OncomiRs, which could activate HSCs (LX2 cells) and transform them to caHSCs, the caHSCs in turn exerted promotion effects on HCC cells through HSCs-released EVs. To further simulate the effects of OncomiRs in EVs on construction of pro-metastatic TME, a group of OncomiRs, miR-21, miR-221 and miR-151 was transfected into HCC cells and LX2 cells. These microRNAs in the EVs from OncomiRs-enhanced cells were demonstrated to have oncogenic effects on HCC cells by upregulating the activities of protein kinase B (AKT)/extracellular signal-regulated kinase (ERK) signal pathways. Equivalent results were also found in HCC xenografted tumor models. The findings suggested that the OncomiR secretion and transference by cancer cells-released EVs can mediate the communication between HCC cells and HSCs. HCC cells and caHSCs, as well as their secreted EVs, jointly construct a pro-metastatic TME suitable for invasion and metastasis of cancer cells, all these TME components form a positive feedback loop to promote HCC progression and metastasis.
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Carcinoma Hepatocelular/genética , Comunicação Celular/genética , Neoplasias Hepáticas/genética , MicroRNAs/metabolismo , Microambiente Tumoral/genética , Animais , Carcinoma Hepatocelular/patologia , Linhagem Celular Tumoral , Progressão da Doença , Vesículas Extracelulares/metabolismo , Regulação Neoplásica da Expressão Gênica , Células Estreladas do Fígado/citologia , Células Estreladas do Fígado/patologia , Humanos , Fígado/citologia , Fígado/patologia , Neoplasias Hepáticas/patologia , Sistema de Sinalização das MAP Quinases/genética , Masculino , Camundongos , Invasividade Neoplásica/genética , Proteínas Proto-Oncogênicas c-akt/metabolismo , Ensaios Antitumorais Modelo de XenoenxertoRESUMO
Balancing the wide band gap, large second harmonic generation (SHG) response, and moderate birefringence are significant but addressable challenges for designing nonlinear optical (NLO) materials. Based on the band-gap engineering in perovskite solar cell materials, we have successfully synthesized a new fluorotellurite, BaF2TeF2(OH)2, which exhibits a pseudo-Aurivillius structure and crystallizes in a noncentrosymmetric and polar space group Pmn21. The physical property measurements show that this material can effectively balance the requirements among the short UV absorption edge (â¼205 nm), large SHG response (â¼3 × KDP) and moderate birefringence (â¼0.078@350-700 nm) and is a promising ultraviolet NLO crystal.