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Highly crystallization-induced emissive luminophores with mechanoluminescent features for two-photon harvesting fluorescence imaging and latent fingerprint identification

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Nano Research 2024年第7期17卷 6475-6482页

作者： Jian Lu Juan Gao Rui-Xuan Qian Shuai-Hua Wang Fa-Kun Zheng guo-cong guo Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China

Fluorescence imaging can be employed in fields of medical treatment,astronomical exploration,and national defense *** fluorescence imaging often takes the single-photon techniques,which is vulnerable to background interference and ***,two-photon fluorescence imaging can achieve much higher-resolution fluorescence imaging for reducing scattering and deeper ***,by assembling the tetraphenylethylene backbones with nontoxic and non-noble K^(+)ions,compound 1([(Hdma)K(H_(2)ettc)]_(n),H_(4)ettc=4',4''',4''''',4'''''''-(ethene-1,1,2,2-tetrayl)tetrakis(([1,1'-biphenyl]-4-carboxylic acid)))with the crystallization-induced emissions exhibited charming fluorescence imaging under two-photon excitation microscopy(TPEM).Besides,luminescent powders based on compound 1 can achieve high-resolution fingerprint recognition,providing secure access control and identification for a novel authentication *** with the commercial fluorescent dyes coumarin-6,the as-synthesized compound 1 showed great solvent stability,indicating its durability against harsh ***,compound 1 shows mechanoluminescent properties for the perturbation of weak supramolecular interactions within ordered arrangements of the H_(2)ettc^(2−)*** novel compound has provided an important insight to the development of twophoton fluorescence imaging and advanced external-stimuli responsive materials.

关键词： crystallization-induced emission fluorescence imaging two-photon absorption fingerprint recognition mechanoluminescence

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The centrosymmetric to non-centrosymmetric transformation induced by alkaline-earth cations producing infrared nonlinear optical AeMn_(6)Ga_(6)S_(16)(Ae=Ca,Sr)

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Science China Chemistry 2024年第9期67卷 2941-2948页

作者： Yang-Ping Zhang Shao-Min Pei Wen-Fa Chen Bin-Wen Liu Xiao-Ming Jiang guo-cong guo State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China School of Physical Science and Technology Shanghai Tech UniversityShanghai 201210China

Non-centrosymmetric(NCS)structure is an indispensable prerequisite for second-order nonlinear optical(NLO)***,the mainstream approach for designing new NCS structures still relies on chemical substitution,necessitating an urgent infusion of fresh *** this work,two isomorphic sulfides AeMn_(6)Ga_(6)S_(16)(Ae=Ca,1;Sr,2)are afforded by modifying the skeleton of centrosymmetric(CS)Mn_(2)Ga_(2)S_(5) via introducing strong electropositive alkaline-earth ***,the incorporation of Ca^(2+)/Sr^(2+)cations allows the elementary[MnGaS_(9)]_(∞)chains to reconfigure into bumpy[MnS_(6)]-[GaS_(4)]layers in a new engagement manner,thus enabling the conversion from CS to NCS *** modifications cause not only strong second-harmonic generation(SHG)responses(~1.5×benchmark AgGaS_(2)@1,700 nm),but also significantly feasible bandgaps(2.60-2.64 e V)compared to the sulfide Mn_(2)Ga_(2)S_(5)(1.36 e V),which ultimately facilitate ultrahigh laser-induced damage thresholds(4.4-6.6×AgGaS_(2)@1,064 nm for compounds 1 and 2).The present study offers an ingenious approach for the transformation of CS to NCS structure.

关键词： second-harmonic generation non-centrosymmetrical structure NLO functional motif solid-state method

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The centrosymmetric to non-centrosymmetric transformation induced by alkaline-earth cations producing infrared nonlinear optical AeMnGaS（Ae = Ca, Sr）

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Science China Chemistry 2024年

作者： Yang-Ping Zhang Shao-Min Pei Wen-Fa Chen Bin-Wen Liu Xiao-Ming Jiang guo-cong guo State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences School of Physical Science and Technology Shanghai Tech University Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China

Non-centrosymmetric （NCS） structure is an indispensable prerequisite for second-order nonlinear optical （NLO） ***,the mainstream approach for designing new NCS structures still relies on chemical substitution,necessitating an urgent infusion of fresh *** this work,two isomorphic sulfides AeMn6Ga6S16（Ae=Ca,1;Sr,2） are afforded by modifying the skeleton of centrosymmetric （CS） Mn2Ga2S5via introducing strong electropositive alkaline-earth ***,the incorporation of Ca2+/Sr2+cations allows the elementary[MnGaS9]∞chains to reconfigure into bumpy[MnS6]-[GaS4]layers in a new engagement manner,thus enabling the conversion from CS to NCS *** modifications cause not only strong second-harmonic generation （SHG） responses （～1.5×benchmark AgGaS2@1,700 nm）,but also significantly feasible bandgaps（2.60–2.64 e V） compared to the sulfide Mn2Ga2S5（1.36 eV）,which ultimately facilitate ultrahigh laser-induced damage thresholds （4.4–6.6×AgGaS2@1,064 nm for compounds 1 and 2）.The present study offers an ingenious approach for the transformation of CS to NCS structure.

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通过聚阳离子取代策略实现压缩黄铜矿型硒化物[Rb3BaCl][In_(8)Se_(14)]以获得优异的非线性光学性能

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Science China Materials 2024年第6期67卷 2000-2007页

作者：吴帆陈文发吴子璇姜小明刘彬文郭国聪 State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China College of Chemistry and Materials Science Fujian Normal UniversityFuzhou 350007China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China University of Chinese Academy of Sciences Beijing 100049China Fujian College University of Chinese Academy of SciencesFuzhou 350002China

单价Ag+或Li+引入到类金刚石结构的MQ22-(M=Ga,In;Q=S,Se)阴离子基团中能合成出良好的二阶非线性光学(NLO)晶体材料.然而,这些晶体分别面临着较低的抗激光损伤阈值(LIDT)或二氧化硅易被腐蚀等缺点,严重限制了其在高功率激光应用中的实用... 详细信息

单价Ag+或Li+引入到类金刚石结构的MQ22-(M=Ga,In;Q=S,Se)阴离子基团中能合成出良好的二阶非线性光学(NLO)晶体材料.然而,这些晶体分别面临着较低的抗激光损伤阈值(LIDT)或二氧化硅易被腐蚀等缺点,严重限制了其在高功率激光应用中的实用性.在本研究中,基于类金刚石结构的ZnSe,我们采用[Se_(4)Zn_(13)]Se_(2)4→[ClRb_(3)Ba]Se_(24)非常规的聚阳离子取代策略,设计并合成了一种新型的盐包硫属化合物[Rb_(3)BaCl][In_(8)Se_(14)](1).化合物1属于压缩黄铜矿型硒化物并保持了与AgInSe_(2)相同的晶体对称性(I-42d空间群).值得注意的是,由于InSe_(4)四面体结构单元的平行排列,化合物1具有相位匹配的强二次谐波(SHG)响应(2.0倍于AgGaS_(2)@2.90μm).此外,聚阳离子[Rb_(3)BaCl]^(4+)的引入促进了光学带隙(2.02 eV)的增强,有效地避免了对2.09μm激光的双光子吸收;同时结合较低的热膨胀系数,使得化合物1表现出高的LIDT(3.2倍于AgGaS2@2.09μm).本研究验证了在类金刚石结构中进行聚阳离子取代的可行性,并成功获得了性能优异的中远红外NLO材料.

关键词： chalcogenide nonlinear optical material substitution strategy diamond-like structure structure-property relationship

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Material research from the viewpoint of functional motifs

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National Science Review 2022年第7期9卷 181-197页

作者： Xiao-Ming Jiang Shuiquan Deng Myung-Hwan Whangbo guo-cong guo State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Department of Chemistry North Carolina State University

As early as 2001,the need for the ’functional motif theory’ was pointed out,to assist the rational design of functional *** properties of materials are determined by their functional motifs and how they are arranged in the *** functional motifs and their arrangements is crucial in understanding the properties of materials and rationally designing new materials of desired *** functional motifs of materials are the critical microstructural units(*** components and building blocks)that play a decisive role in generating certain material functions,and can not be replaced with other structural units without the loss,or significant suppression,of relevant *** role of functional motifs and their arrangement in materials,with representative examples,is *** microscopic structures of these examples can be classified into six types on a length scale smaller than ～10 nm with maximum subatomic resolution,***,magnetic,aperio dic,defect,local and electronic *** motif analysis can be employed in the function-oriented design of materials,as elucidated by taking infrared non-linear optical materials as an *** learning is more efficient in predicting material properties and screening materials with high efficiency than high-throughput experimentation and high-throughput *** order to extract functional motifs and find their quantitative relationships,the development of sufficiently reliable databases for material structures and properties is imperative.

关键词： functional motif functional motif arrangements microscopic structures structure–property relationship

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Salt-inclusion chalcogenides:Double functional moieties design strategy toward excellent nonlinear optical materials

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Chinese Journal of Structural Chemistry 2023年第3期42卷 24-34页

作者： Chao-Hong Xie Bin-Wen Liu guo-cong guo State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhouFujian350002People's Republic of China University of Chinese Academy of Sciences Beijing100190People's Republic of China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China FuzhouFujian350108People's Republic of China

Nonlinear optical(NLO)material are of great importance in converting the frequency to extend the laser spectrum in mid-and far-infrared(IR)regions where lasers operate poorly or are ***,the contradiction between large second-harmonic generation(SHG)intensity and wide band gap(E_(g))is a long-standing problem for IR NLO *** address the issue,metal chalcogenides have been successfully synthesized and developed excellent optical properties in the past few *** a newly discovered category of chalcogenides,salt-inclusion chalcogenides with distinctive structures and brilliant performances have been placed great expecta-tions to be a novel *** this review,52 compounds in this thriving family are categorized via dimensions of host and guest parts,further discussing the relationships between their structures and NLO properties,as well as future perspectives of this family.

关键词： Salt-inclusion chalcogenide Nonlinear optical material Host and guest parts Structural crystal

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Synthesis,Crystal Structure and Fluorescent Properties of New Layered Thiophosphate Cs_(2)Ga_(3)PS_(8)

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Chinese Journal of Structural Chemistry 2021年第10期40卷 1271-1276页

作者： CHEN Wen-Fa LIU Bin-Wen JIANG Xiao-Ming guo guo-cong State Key Laboratory of Structural Chemistiy Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China University of Chinese Academy of Sciences Beijing 100190China

A new quaternary metal thiophosphate,Cs_(2)Ga_(3)PS_(8),in triclinic P1^(-) space group has been successfully synthesized by a reactive-flux *** structural framework is derived from well-known AM^(Ⅲ)M^(Ⅳ)Q_(4) (A=alkali metal;M^(Ⅲ)=Al,Ga,In;M^(Ⅳ)=Si,Ge,Sn;Q=S,Se) system and composed of two-dimensional ^(2)∞[Ga_(3)PS_(8)]^(2-) layers separated by Cs^(+).The compound exhibits a wide band gap of 3.08 eV and congruent-melting behavior with melt point of 645℃.Interestingly,Cs_(2)Ga_(3)PS_(8) exhibits a broad photoluminescent emission band at 420 nm upon excitation at 295 ***,electronic structure calculations indicate that Cs_(2)Ga_(3)PS_(8) is a direct band gap compound and its luminescent process can be mainly ascribed to electron transfer from the S-3p and Ga-4p states to S-3p and P-3p.

关键词： chalcogenide thiophosphate crystal structure solid-state phase synthesis

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Synthesis and Structural Characterization of a New Cadmium(II) Complex with a Double Betaine

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Chinese Journal of Structural Chemistry 2005年第8期24卷 940-944页

作者： ZHENG Fa-Kun WU A-Qing LI Yan guo guo-cong HUANG Jin-Shun State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter The Chinese Academy of Sciences Fuzhou Fujian 350002 China Graduate School The Chinese Academy of Sciences Beijing 100039 China

A new flexible double betaine L （L = 1,4-bis（pyridinio-4-carboxylato-N-methyl）benzene, C20H16N2O4） and its cadmium（Ⅱ） complex [Cd（H2O）aL（NO3）]NO3.H2O 1 were synthesized. Complex 1 was obtained by self-assembly reaction of [Cd（NO3）2]-4H2O and L in hot water,and its crystal structure was determined by single-crystal X-ray diffraction analysis. Crystallographic data for complex 1： C20H24CdN4O14.H2O, Mr = 674.85, monoclinic, space group P21/c, a =13.7854（3）, b = 14.2820（3）, c = 14.9188（4） ,A°, β = 116.418（1）°, V = 2630.5（1）A°^3, Z = 4, Dc= 1.704g/cm^3,/J（MoKα） = 0.911 mm^-1, F（000） = 1368, the final R = 0.0315 and wR = 0.0768 for 3637 observed reflections with I 〉 2σ（I）. In complex 1, L acts as a monodentate ligand to link a Cd（Ⅱ） ion in a novel coordination mode of double betaines. The mononuclear [Cd（H2O）aL（NO3）] units are connected through intermolecular hydrogen bonds and π-π stacking reactions to generate a 3D network.

关键词： cadmium(Ⅱ) complex crystal structure double betaine hydrogen bonds

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Synthesis and Crystal Structure of a New Lanthanum(III) 4-Cyanobenzoate Complex

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Chinese Journal of Structural Chemistry 2007年第5期26卷 575-579页

作者： LI guo-Qing LI Yanb ZOU Wen-Qiang CHEN Qi-Yong ZHENG Fa-Kun guo guo-cong Chemistry and Life Science School Quanzhou Normal University Quanzhou Fujian 362000 China State Key Laboratory of Structural Chemistry Fujian Institute of Research on theStructure of Matter The Chinese Academy of Sciences Fuzhou Fujian 350002 China Graduate School of the Chinese Academy of Sciences Beijing 100039 China

A new dinuclear La（Ⅲ） complex [La2（4-cba）4[H（4-cba）2]2（phen）2（H2O）4] （4-Hcba = 4-cyanobenzoic acid and phen = 1,10-phenanthroline） 1 has been synthesized by solvothermal reaction in an ethanol/water mixed solution at 100 ℃ and structurally characterized by singlecrystal X-ray diffraction. Crystallographic data： C88H58La2N12O20, Mr = 1881.28, triclinic P1, a = 7.518（3）, b = 17.033（6）, c = 17.551（6）A, α = 115.333（4）, β = 92.9910（10）, γ = 99.366（5）°, V = 1985.3（12）A^3, Z = 1, Dc = 1.574 g/cm^3, F（000） = 944 μ = 1.145 mm^–1, the final R = 0.0281 and wR = 0.0686 for 6708 reflections with Ⅰ 〉 2σ（I）. In 1, two nine-coordinated La（Ⅲ） ions are connected by two 4-cba ligands in a syn-syn bidentate coordination mode, and the other six 4-cba ligands terminate the La（Ⅲ） ions, resulting in an isolated dinuclear structure. Two different types of intramolecular hydrogen bonds, asymmetrical O-H…O and symmetrical O…H…O, exist in the crystal. The title complex molecules are connected through hydrogen bonds and weak π-π stacking interactions to generate a 2-D layered network. The thermogravimetric analysis of 1 has also been discussed.

关键词： lanthanum(Ⅲ) complex 4-cyanobenzoic acid crystal structure hydrogen bonds

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Synthesis, Single-crystal Structure, and Optical and Magnetic Properties of CaEr_2S_4

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Chinese Journal of Structural Chemistry 2007年第8期26卷 973-979页

作者： ZENG Hui-Yi Mattausch Hansjtirgen ZHENG Fa-Kun DONG Zhen-Chao guo guo-cong HUANG Jin-Shun State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter The Chinese Academy of Sciences Fuzhou Fujian 350002 China Max Planck Institute for Solid State Research Heisenbergstrasse 1 D-70569 Stuttgart Germany Hefei National Laboratory for Physical Sciences at Microscale University of Science and Technology of China Hefei Anhui 230026 China

Brown needle-like crystals of CaEr2S4 were isolated as the major product from a reaction of elements and binary sulfides by a two-step flux technique. CaEr2S4 crystallizes in the orthorhombic space group Pnma with a=12.845（4）, b=3.862（4）, c=13.001（2）（A）, V=645.0（7）（A）3,Z=4, F（000）=880,μ（MoKα）=27.794 mm^-1, the final R=0.0528 and wR=0.0562 for 1070observed reflections with I 〉 3σ（I）. The CaEr2S4 structure forms a three-dimensional framework that consists of interconnected tetra-octahedral Er4S18 fragments. Ca^2＋cations, in a monocapped trigonal prism geometry, are stuffed in two parallel rows into the one-dimensional channels along the b direction. CaEr2S4 is an infrared-transparent semiconductor with a band gap of 1.81 eV. Magnetic susceptibility measurements over 6～300 K indicate a Curie-Weiss paramagnetic behavior for the phase, with an effective magnetic moment of 9.64（1） μB per Er^3＋ ion.

关键词： rare-earth chalcogenides flux crystal growth crystal structure optical and magnetic properties

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