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CCS Chemistry 2024年第2期6卷 497-506页

作者： Lifeng Wang Hanxun Zou Hebo Ye Yu Hai Hanwei Lu Junmiao Deng Lei You State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002 College of Chemistry and Material Science Fujian Normal UniversityFuzhou 350007 University of Chinese Academy of Sciences Beijing 100049 Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108

Light-induced recognition,assemblies,and materials are intensive areas of research due to their high spatiotemporal resolution.Herein,we demonstrated photoswitchable molecular recognition via dithienylethene-triggeredreversible structural regulation of dynamic covalent hydrazone bonds.By combining dithienylethenes and cyclic hemiacetals,the photochemical open-ring and closed-ring forms enabled turningoff and on the creation of awide range of hydrazones when desired.Light-induced bidirectional switching between hydrazones and their cyclization structures promoted by a neighboring carboxyl group was further achieved.By taking advantage of reversible structural changes totoggleon andoff the binding pocket,photoswitchable recognitionofmetal ionswas realized.Finally,the construction of an acylhydrazone polymer offered a facile way for light-mediated selective extraction/release.The strategies and results reported here should find applications in many contexts,such asdynamicassemblies,molecular switches,and smart materials.

关键词： molecular recognition photoswitch dynamic covalent chemistry hydrazone selective extraction/release

Optical control of neuronal activities with photoswitchable nanovesicles

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Nano Research 2023年第1期16卷 1033-1041页

作者： Hejian Xiong Kevin AAlberto Jonghae Youn Jaume Taura Johannes Morstein Xiuying Li Yang Wang Dirk Trauner Paul A.Slesinger Steven O.Nielsen Zhenpeng Qin Department of Mechanical Engineering The University of Texas at DallasRichardsonTX 75080USA Department of Chemistry and Biochemistry The University of Texas at DallasRichardsonTX 75080USA Nash Family Department of Neuroscience Icahn School of Medicine at Mount SinaiNew YorkNY 10029USA Department of Chemistry New York UniversityNew YorkNY 10012USA Department of Bioengineering The University of Texas at DallasRichardsonTX 75080USA Department of Surgery The University of Texas at Southwestern Medical CenterDallasTX 75080USA Center for Advanced Pain Studies The University of Texas at DallasRichardsonTX 75080USA

Precise modulation of neuronal activity by neuroactive molecules is essential for understanding brain circuits and behavior.However,tools for highly controllable molecular release are lacking.Here,we developed a photoswitchable nanovesicle with azobenzene-containing phosphatidylcholine(azo-PC),coined‘azosome’,for neuromodulation.Irradiation with 365 nm light triggers the trans-to-cis isomerization of azo-PC,resulting in a disordered lipid bilayer with decreased thickness and cargo release.Irradiation with 455 nm light induces reverse isomerization and switches the release off.Real-time fluorescence imaging shows controllable and repeatable cargo release within seconds(<3 s).Importantly,we demonstrate that SKF-81297,a dopamine D1-receptor agonist,can be repeatedly released from the azosome to activate cultures of primary striatal neurons.Azosome shows promise for precise optical control over the molecular release and can be a valuable tool for molecular neuroscience studies.

关键词： azobenzene photoswitch liposome controlled release neuromodulation

Photo-Modulation of Gene-Editing Enzymes CRISPR/Cas9 with Bifunctional Small-Molecule Ligands

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Chinese Journal of Chemistry 2023年第24期41卷 3639-3644页

作者： Yidan Zhang Yixin Zhang Lili Han Qiaoling Che Jiawei Tan Peng Zou Yiyun Chen State Key Laboratory of Chemical Biology Shanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of Sciences345 Lingling RoadShanghai200032 China School of Chemistry and Material Sciences Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of Sciences1 Sub-lane XiangshanHangzhouZhejiang310024 China School of Physical Science and Technology ShanghaiTech University100 Haike RoadShanghai201210 China

The control of protein functions with light is valuable for spatiotemporal probing of biological systems.Current small-molecule photo-modulation methods include the light-induced uncaging of inhibitors and chromophore-assisted light inactivation with reactive oxygen species(ROS).However,the constant target protein expression results in inadequate photo-modulation efficiency,particularly for less potent inhibitors and chromophores.Herein,we report a novel bifunctional small-molecule ligands strategy to photo-modulate gene-editing enzymes CRISPR/Cas9.A coumarin-derived small-molecule ligand Bhc-BRD0539 is developed to uncage the active inhibitor upon light irradiation and to generate ROS in the Cas9 proximity for the dual inhibition of Cas9 activity.Our results highlight the synergistic photo-modulation with bifunctional small-molecule ligands,which offers a valuable addition to current CRISPR/Cas9 photo-modulation technologies and may extend to other protein classes.

关键词： Gene-editing Small-molecule ligands Enzyme modulation DNA cleavage photoswitch Inhibitors

基于可重构光开关多态荧光聚合物的信息加密工具箱

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Science China Materials 2023年第5期66卷 1949-1958页

作者：姜佳伟张培盛田勇林众张崇华崔家喜陈建陈旭东 Key Laboratory of Theoretical Organic Chemistry and Functional Molecule of Ministry of Education Hunan Provincial Key Laboratory of Controllable Preparation and Functional Application of Fine PolymersHunan Province College Key Laboratory of QSAR/QSPRSchool of Chemistry and Chemical EngineeringHunan University of Science and TechnologyXiangtan 411201China College of Chemistry and Key Laboratory of Polymeric Materials&Application Technology of Hunan Province and Key Laboratory of Advanced Functional Polymeric Materials of College of Hunan ProvinceXiangtan UniversityXiangtan 411105China Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 610054China Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education School of ChemistrySun Yat-sen UniversityGuangzhou 510006China Jieyang Branch of Chemistry and Chemical Engineering Guangdong Laboratory Jieyang 515200China

具有坚固、智能、且易于编程等特性的信息加密材料对于防止信息泄露和打击造假具有重要意义.为此,我们开发了一种信息加密材料工具箱,该工具箱基于一系列新型的自修复光开关双态(P1和P2)和多态(P3)荧光聚合物.这类聚合物含有两种二芳基... 详细信息

具有坚固、智能、且易于编程等特性的信息加密材料对于防止信息泄露和打击造假具有重要意义.为此,我们开发了一种信息加密材料工具箱,该工具箱基于一系列新型的自修复光开关双态(P1和P2)和多态(P3)荧光聚合物.这类聚合物含有两种二芳基乙烯光致变色荧光基团(SDTE和BTBA)和四重氢键构筑单元(UPy).在不同波长的光照射下,P1/P2可以在绿-猝灭/红-猝灭两态之间交替,而P3可以在红-绿-猝灭三态之间变化.它们可以作为像素单元用来制备可重构的图案和代码;所得到的图案和代码均显示出良好的机械性能和优异的光学特性,包括快速的光响应性、突出的光可逆性、优异的荧光热稳定性和抗酸碱腐蚀的能力.本文展示了该工具箱在3D代码阵列和二维码信息加密中的应用潜能.

关键词： photoswitch diarylethene self-healing polymer thermal stability information encryption

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Giant negative photoresistance of epitaxial manganite La2/3Ca1/3MnO3-δ film

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Science China(Information Sciences) 2015年第12期58卷 204-210页

作者： XI JianFeng ZHAO Kun NI Hao XIANG WenFeng FENG Xin SUN Qi LU ZhiQing XIAO LiZhi State Key Laboratory of Petroleum Resources and Prospecting China University of Petroleum Beijing Key Laboratory of Optical Detection Technology for Oil and Gas China University of Petroleum

The La2/3Ca1/3Mn O3-δ film has been deposited on the(001) Sr Ti O3 substrate and its temperature-dependent photoconductive properties have been investigated from 80 to 300 K. The La2/3Ca1/3Mn O3-δfilm has a novel photoelectric property due to its oxygen-deficient structure. We observed laser-induced giant negative photoresistance of the sample in a wide temperature range. The change rate of negative photoresistance was nearly 100% at the low temperature when the sample was irradiated by 532 nm laser. In addition, this effect was sensitive to the power of laser irradiation. The oxygen-deficiency of La2/3Ca1/3Mn O3-δfilm seems to have an impact on the laser-induced resistance variation. The experimental results made the La2/3Ca1/3Mn O3-δfilm a promising application as a photoswitch device.

关键词： giant negative photoresistance oxygen-deficient photoswitch thin film manganite oxide

Direct van der Waals epitaxial growth of 1D/2D Sb2Se3/WS2 mixed-dimensional p-n heterojunctions

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Nano Research 2019年第5期12卷 1139-1145页

作者： Guangzhuang Sun Bo Li Jia Li Zhengwei Zhang Huifang Ma Peng Chen Bei Zhao Ruixia Wu Weiqi Dang Xiangdong Yang Xuwan Tang Chen Dai Ziwei Huang Yuan Liu Xidong Duan Xiangfeng Duan State Key Laboratory for Chemo/Biosensing and Chemometrics and Hunan Key Laboratory of Two-Dimensional Materials College of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China Department of Applied Physics School of Physics and ElectronicsHunan UniversityChangsha 410082China Department of Chemistry and Biochemistry University of CaliforniaLos AngelesCalifornia 90095USA

The mixed-dimensional integration of two-dimensional (2D) materials with non-2D materials can give rise to prominent advances in performance or function.To date,the mixed-dimensional one-dimensional (1D)/2D heterostructures have been fabricated using various physical assembly approaches.However,direct epitaxial growth method which has notable advantages in preparing large-scale products and obtaining perfect interfaces is rarely investigated.Herein,we demonstrate for the first time the direct synthesis of the 1D/2D mixed-dimensional heterostructures by sequential vapor-phase growth of Sb2Se3 nanowires on WS2 monolayers.X-ray diffraction (XRD) pattern and Raman spectrum confirm the composition of the Sb2Se3/NS2 heterostructures.Transmission electron microscope (TEM) measurement demonstrates high quality of the heterostructures.Electrical transport characterization reveals that Sb2Se3 nanowire exhibits p-type characteristic and that WS2 monolayer exhibits n-type behavior,and that the p-n diode from 1D/2D mixed-dimensional Sb2Se3/WS2 heterostructure possesses obvious current rectification behavior.Optoelectronic measurements of the heterostructures show apparent photovoltaic response with an open-circuit voltage of 0.19 V,photoresponsivity of 1.51 A/W (Vds =5 V) and fast response time of less than 8 ms.The van der Waals epitaxial growth mode of Sb2Se3 nanowires on WS2 monolayers is verified by stripping the Sb2Se3 nanowire from the heterostructures using tape.Together,the direct van der Waals epitaxy opens a facile pathway to 1D/2D mixed-dimensional heterostructures for functional electronic and optoelectronic devices.

关键词： van der Waals epitaxy Sb2Se3/WS2heterostructures rectification behavior photovoltaic effect photoswitch

Rational construction of self-assembly azobenzene derivative monolayers with photoswitchable surface properties

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Chinese Chemical Letters 2018年第11期29卷 1661-1665页

作者： Yu Zhang Peng Gao Qin Yue Peter Trefonas Yonghui Deng Department of Chemistry State Key Laboratory of Molecular Engineering of Polymers Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials iChEM Fudan University Shanghai 200433 China Dow Chemical (China) Investment Company Shanghai 201203 China Rohm & Haas Electronic Materials LLC Marlborough MA 01752 United States State Key Laboratory of Transducer Technology Shanghai Institute of Microsystem and Information Technology Chinese Academy of Sciences Shanghai 200050 China

Photo-responsive azobenzene （ABZ） derivatives with different end groups （R） as photoswitchable molecules were employed to construct self-assembled monolayers （SAMs） on silicon substrate by using 3-glycidoxypropyltrimethoxysilane （GPTS） as the bridging molecules. The assembly process was optimized by changing various parameters, including the type and concentration of ABZ derivatives, reaction time, etc. The obtained SAMs were fully characterized and evaluated using UV spectroscopy, atomic force microscope （AFM）, elllipsometer, static contact angle and X-ray photoelectron spectroscopy （XPS）. It is found that the end group property of azobenzene derivatives is critical to the obtained SAMs＇ photoresponsive properties. Compared with hydrophobic compounds （4-（4＇-aminophenylazo） benzoic acid, ABZ-CF3）, the hydrophilic compounds （4-（4＇-aminophenylazo） benzoic acid, ABZ-COOH） show excellent reversible photoswitching performance with a large contact angle change of 35° under oDtimized process, and the SAMs are removable bv thermal treatment at 240 ℃ in air for onlv 5 min.

关键词： Self-assembly Monolayer Azobenzene photoswitch Surface treatment

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Comparison of two thioxopeptide bond photoswitches in insect kinin

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Chinese Chemical Letters 2010年第4期21卷 476-479页

作者： Cong, Zhi Yuan Yang, Long Fei Jiang, Ling Ye, Dan Dong, Shou Liang Lanzhou Univ Inst Biochem & Mol Biol Sch Life Sci Lanzhou 730000 Peoples R China

The photoisomerization abilities of secondary thioxopeptide bond(CS-NH) and thioxo prolyl bond(CS-N) incorporated into the C-terminal pentapeptide of insect kinin were compared.H-Phe-Phe-Ψ[CS-NH]-D-Ala-Trp-Gly-NH_2 and H-Phe-Tyr-Ψ[CS-N]- Pro-Trp-Gly-NH_2 were studied by UV-vis absorption.The isomerization energy barriers of the two segments,Ac-Phe-Ψ[CS-NH]- D-Ala-NH_2 and Ac-Tyr-Ψ[CS-N]-Pro-NH_2 picked from the two peptides,were calculated using ab initio method.The cis isomer of CS-N is more stable than th...

关键词： photoswitch Thioxopeptide bond Energy barrier

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Synthesis of Spiropyran-based photoswitchable Cross-linkers for Labeling Biomolecular Probes

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Synthesis of Spiropyran-based Photoswitchable Cross-linkers ...