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A synergetic strategy of NIR-Ⅱ squaraine dyes with ultrahigh photothermal conversion efficiency for photothermal therapy

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Science China Chemistry 2024年第2期67卷 612-621页

作者： Yigang Wang Guomin Xia Junhui Wang Mingda Wang Weihan Guo Manman Tan Leilei Si Yang Yang Hua Wang Hongming Wang Institute for Advanced Study and School of Chemistry and Chemical Engineering Nanchang UniversityNanchang330031China State Key Laboratory of Molecular Reaction Dynamics and Dynamics Research Center for Energy and Environmental Materials Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian116023China The Second Affiliated Hospital of Nanchang University Nanchang330031China

Recent research on photothermal therapy(PTT) has sparked significant interest in the development of new organic photothermal agents(PTAs),ranging from single-molecule to aggregated levels.However,controlling aggregation pathways for PTAs with ultrahigh photothermal conversion efficiency(PCE) remains a major challenge.Herein,a two-pronged approach utilizing “Haggregation” and “Intramolecular motion” was employed to enhance the PCE of an acceptor-substituted squaraine dye(NSQs).The C2vmolecular symmetry of the NSQs,which possess a ground state dipole moment(μg),promotes H-dimeric aggregates through dipole-dipole counteraction.Peripheral triphenylethylene or diphenylamine groups were added to this H-dimeric nanoplatform.This was done to enhance Intramolecular motions for heat generation and also to extend conjugation,which redshifted the optical absorption and balanced the blue-shift induced by H-aggregation.With this technique,an organic PTA with NIR-II absorption was developed,and its nanoparticle achieved a remarkable PCE of 86.3% under 1,064 nm laser excitation.Femtosecond transient absorption spectroscopy and quantum mechanical calculations demonstrated the accelerated internal conversion process in NIR-II PTAs for rapid heat generation.The NSQs nanoparticles exhibit superior photothermal therapeutic properties for in vivo photoacoustic imaging-guided PTT,demonstrating the potential of bottom-up design to enable synergistic engineering strategies towards efficient phototheranostic agents.

关键词： squaraine dyes second near-infrared window H-aggregation Intramolecular motion photothermal therapy

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Ligand-dependent aggregation-enhanced photoacoustic of atomically precise metal nanocluster

Aggregate

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Aggregate 2024年第1期5卷 196-203页

作者： Changlin Zhou Meng Wang Qiaofeng Yao Yu Zhou Chuantao Hou Jianfei Xia Zonghua Wang Jishi Chen Jianping Xie College of Chemistry and Chemical Engineering Shandong Sino-Japanese Center for Collaborative Research of Carbon NanomaterialsInstrumental Analysis Center of Qingdao UniversityQingdao UniversityQingdaoP.R.China Tianjin Key Laboratory of Molecular Optoelectronic Sciences Department of ChemistrySchool of ScienceTianjin UniversityTianjinP.R.China Qingdao Boting Hydrogen Age Ocean Technol R&D Ctr. Qingdao Boting Technol Co.Ltd.Shandong Hydrogen Times Marine Technology Co.Ltd.QingdaoP.R.China Department of Chemical and Biomolecular Engineering National University of SingaporeSingapore Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New CityFuzhouP.R.China

Atomically precise metal nanoclusters(MNCs),as a potential type of photoacoustic(PA)contrast agent,are limited in application due to their low PA conversion efficiency(PACE).Here,with hydrophilic Au25SR18(SR=thiolate)as model NCs,we present a result that weakly polar solvent induces aggregation,which effectively enhances PA intensity and PACE.The PA intensity and PACE are highly dependent on the degree of aggregation,while the aggregation-enhanced PA intensity(AEPA)positively correlates to the protected ligands.Such an AEPA phenomenon indicates that aggregation actually accelerates the Intramolecular motion of Au NCs,and enlarges the proportion of excited state energy dissipated through vibrational relaxation.This result conflicts with the restriction of Intramolecular motion mechanism of aggregation-induced emission.Further experiments show that the increased energy of AEPA originates from the aggregation inhibiting the intermolecular energy transfer from excited Au NCs to their surrounding medium molecules,including solvent molecule and dissolved oxygen,rather than restricting radiative relaxations.This study develops a new strategy for enhancing the PA intensity of Au NCs,and contributes to a deeper understanding of the origin of the PA signal and the excited state energy dissipation processes for MNCs.

关键词： aggregation-enhanced photoacoustic gold nanocluster intermolecular excited state energy transfer Intramolecular motion ligand effect

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Polymerization-Amplified Photoacoustic Signal by Enhancing Near-Infrared Light-Harvesting Capacity and Thermal-to-Acoustic Conversion

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Chinese Journal of Polymer Science 2022年第9期40卷 1090-1100页

作者： He-Qi Gao Jing-Tian Zhang Xin-Wen Qi Di Jiao Yu-Ning Hong Ke Shan Xiang-Long Kong Dan Ding Key Laboratory of Bioactive Materials Ministry of Educationand College of Life SciencesNankai UniversityTianjin 300071China Center for AIE Research Shenzhen Key Laboratory of Polymer Science and TechnologyGuangdong Research Center for Interfacial Engineering of Functional MaterialsCollege of Materials Science and EngineeringCollege of Physics and Optoelectronic EngineeringShenzhen UniversityShenzhen 518060China Department of Chemistry and Physics La Trobe Institute for Molecular ScienceLa Trobe UniversityMelbourneVictoria3086Australia Shandong Artificial intelligence Institute and Shandong Computer Science Center Qilu University of TechnologyJinan 250353China

As a frontier imaging technique for biomedical applications,photoacoustic(PA)imaging has been developed rapidly.The development of new design strategies and excellent PA imaging reagents to boost PA conversion is eagerly desirable for high quality PA imaging but complicated to realize.Herein,we develop a new strategy in which PA imaging reagents with better properties can be easily optimized by polymerization.A series of new PA imaging reagents were designed and synthesized.The polymerization strategy can effectively promote the PA signal by specifically increasing the thermal-to-acoustic conversion efficiency.As these materials shared the same building units,the optimized effectiveness of polymerization strategy in terms of near-infrared light-harvesting capacity and thermal-to-acoustic conversion efficiency are discussed,rationally.The polymers with intense Intramolecular motion exhibit an amplified PA signal by elevating thermal-to-acoustic conversion and its higher light-harvesting capability at redshifted region.The simultaneously strong PA signal and photothermal conversion efficiency of p-TTmB NPs enable precise PA imaging and effective photothermal therapy.This work highlights a simple and available design guideline of polymerization for amplifying the PA effect and optimizing existing materials.

关键词： Intramolecular motion Thermal-to-acoustic conversion Photoacoustic imaging Photothermal conversion efficiency Polymerization

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Molecular motions in Polymer Matrix for Microenvironment Sensing

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Chemical Research in Chinese Universities 2021年第1期37卷 90-99页

作者： GAO Mengyue CHENG Yanhua ZHANG Junyan XU Chengjian YU Xiaoxiao ZHU Meifang State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and EngineeringDonghua UniversityShanghai201620P.R.China

Polymer science entails the structural study at multi-levels from nano-to micro-and mesoscale,which is highly important to transfer or even amplify the molecular information to macroscopic materials.Multiple polymer structural transitions from lower-order to higher-order superstructures are normally involved to achieve selective,efficient and sophisticated functions.Therefore,in-situ visualization of these processes is highly important,not only for fundamental understanding the structural evolution,but also for the optimization of the process flow during the materials processing.Fluorescence imaging based on aggregation-induced emission(AIE)provides an ideal tool that offers a simple,accurate,and easy-readable method to fulfill the above requirements.Owing to the twisted propeller-like structure of AIE luminogens(AIEgens),they show high fluorescence sensitivity to the surrounding microenvironment(e.g.,viscosity,rigidity,and polarity)through Intramolecular motions.In this short review,we summarize the recent applications of AIEgens to serve as“built-in”sensors to analyze the process of polymerization,microphase separation,glass/vitrification transition,polymer solvation,crystallization,etc.The perspective on the future application of AIE technology in polymer engineering,especially fiber materials,is also discussed.

关键词： Aggregation-induced emission(AIE) Intramolecular motion Polymer structure Polymer microenvironment Visualization

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Gathering brings strength:How organic aggregates boost disease phototheranostics

聚集体(英文)

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聚集体(英文) 2021年第1期2卷 95-113页

作者： Ji Qi Hanlin Ou Qian Liu Dan Ding State Key Laboratory of Medicinal Chemical Biology Nankai UniversityTianjinChina Key Laboratory of Bioactive Materials Ministry of Educationand College of Life SciencesNankai UniversityTianjinChina Department of Urology Tianjin First Central HospitalTianjinChina

Phototheranostics that concurrently and complementarily integrate real-time diagnosis and in situ therapeutic capabilities in one platform has become the advancing edge of precision medicine.Organic agents possess the merits of facile preparation,high purity,tunable photophysical property,good biocompatibility,and potential biodegradability,which have shown great promise for disease theranostics.This review summarizes the recent achievements of organic phototheranostic agents and applications,especially which rationally utilize energy dissipation pathways of Jablonski diagram to modulate the fluorescence emission,photoacoustic/photothermal production,and photodynamic processes.Of particular interest are the systems exhibiting huge differences in aggregate state as compared with the solution or single molecule form,during which the Intramolecular motions play an important role in regulating the photophysical properties.The recent advances from such an aspect for biomedical applications including high-resolution imaging,activatable imaging and therapy,adaptive theranostics,image-guided surgery,immunotherapy,and afterglow imaging are discussed.A brief summary and perspective in this field are also presented.We hope this review will be helpful to the researchers interested in bioprobe design and theranostic applications,and inspire new insights into the linkage between aggregate science and biomedical field.

关键词： activatable probe aggregate aggregation-induced emission Intramolecular motion Jablonski diagram phototheranostics

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Decomposition of Molecular motions into Translational, Rotational, and intramolecular Parts by a Projection Operator Technique

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Communications in Computational Physics 2009年第7期6卷 231-246页

作者： F.Y.Hansen H.Taub Department of Chemistry Technical University of DenmarkIK 207 DTUDK-2800 LyngbyDenmark Department of Physics and Astronomy and the University of Missouri Research Reactor University of MissouriColumbiaMissouri 65211USA

The motion of the atoms in a molecule may be described as a superposition of translational motion of the molecular center-of-mass,rotational motion about the principal molecular axes,and an Intramolecular motion that may be associated with vibrations and librations as well as molecular conformational changes.We have constructed projection operators that use the atomic coordinates and velocities at any two times,t=0 and a later time t,to determine the molecular center-of-mass,rotational,and Intramolecular motions in a molecular dynamics simulation.This model-independent technique facilitates characterization of the atomic motions within a system of complex molecules and is important for the interpretation of experiments that rely on time correlation functions of atomic and molecular positions and velocities.The application of the projection operator technique is illustrated for the inelastic neutron scattering functions and for the translational and rotational velocity autocorrelation functions.

关键词： Molecular dynamics projection operator correlation functions scattering functions translational motion rotational motion Intramolecular motion

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