Alleviating NIR-II emission quenching in ring-fused fluorophore via manipulating dimer populations for superior fluorescence imaging DOI Creative Commons

Xiaofei Miao,

Mingxuan Jia,

Xiaole Weng

et al.

Light Science & Applications, Journal Year: 2025, Volume and Issue: 14(1)

Published: March 4, 2025

Emission quenching resulting from fluorophore aggregation has long been a significant challenge in optimizing emission-based technologies, such as fluorescence imaging and optoelectronic devices. Alleviating this aggregates is crucial, yet progress impeded by the limited understanding of nature impact on emission. Here, we elucidate critical role dimeric aggregate (dimer) alleviating second near-infrared (NIR-II, 900-1700 nm) emission ring-fused 4F for superior imaging. Spectral decomposition molecular dynamics simulations demonstrate predominance dimer populations aggregates. Notably, dimers exhibit significantly weaker but intense intermolecular nonradiative (interNR) decay compared to monomers, demonstrated ultrafast spectra quantum calculation. Therefore, predominant population with weak pronounced interNR feature underlies This discovery guides preparation ultrabright NIR-II nanofluorophore (4F NP3s) decreasing populations, which show 5-fold greater brightness than indocyanine green, enabling resolution visualizing blood vessels. work offers valuable insights into aggregation-caused quenching, broad implications extending far beyond

Language: Английский

Photo‐Induced Disproportionation‐Mediated Photodynamic Therapy: Simultaneous Oxidation of Tetrahydrobiopterin and Generation of Superoxide Radicals DOI
Kun‐Xu Teng, Dongsheng Zhang,

Bin‐Kai Liu

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(12)

Published: Jan. 23, 2024

We herein present an approach of photo-induced disproportionation for preparation Type-I photodynamic agents. As a proof concept, BODIPY-based photosensitizers were rationally designed and prepared. The intermolecular electron transfer between homotypic chromophores leads to the reaction, resulting in formation charged intermediates, cationic anionic radicals. radicals efficiently oxidize cellularimportant coenzyme, tetrahydrobiopterin (BH

Language: Английский

Citations

43
Supramolecular systems for bioapplications: recent research progress in China DOI
Yue‐Yang Liu, Xiao-Yong Yu, Yu‐Chen Pan

et al.

Science China Chemistry, Journal Year: 2024, Volume and Issue: 67(5), P. 1397 - 1441

Published: March 22, 2024

Language: Английский

Citations

28
Deciphering Oxygen‐Independent Augmented Photodynamic Oncotherapy by Facilitating the Separation of Electron‐Hole Pairs DOI
Xiaoming Hu, Zhu-ting Fang,

Fengwei Sun

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(15)

Published: Feb. 16, 2024

Developing Type-I photosensitizers provides an attractive approach to solve the dilemma of inadequate efficacy photodynamic therapy (PDT) caused by inherent oxygen consumption traditional Type-II PDT and anoxic tumor microenvironment. The challenge for exploration PSs is facilitate electron transfer ability photosensitization molecules transforming or H

Language: Английский

Citations

20
Less is More: Asymmetric D‐A Type Agent to Achieve Dynamic Self‐Assembled Nanoaggregates for Long‐Acting Photodynamic Therapy DOI

Ruohan Xu,

Qifei Shen,

Peijuan Zhang

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(28)

Published: April 30, 2024

Abstract To enhance the phototheranostic performance, agents with high reactive oxygen species (ROS) generation, good tumor‐targeting ability, and prolonged retention are urgently needed. However, symmetric donor–acceptor (D–A) type usually produce spherical nanoaggregates, leading to tumor targeting but inferior retention. Rod‐like nanoaggregates desired extend their in tumors; however, this remains a challenge. In particular, dynamically changeable shapes that integrate merits of different morphologies seldomly reported. Therefore, self‐assembled organic smart shape tunability designed here using an asymmetric D–A TIBT. The photoluminescence quantum yield solids is up 52.24% for TIBT also exhibits ROS generation corresponding (TIBT‐NCs). Moreover, dynamic self‐assembly changing from nanospheres nanorods occurrs TIBT‐NCs, contributing enhancement 0.55 0.72. addition, can be observed both vitro vivo, conferring TIBT‐NCs strong Finally, efficient photodynamic therapy inhibit growth achieved inhibition rate 90%. This work demonstrates play significant roles forming thus showing great potential long‐acting cancer therapy.

Language: Английский

Citations

16
Zwitterionic Photosensitizer‐Assembled Nanocluster Produces Efficient Photogenerated Radicals via Autoionization for Superior Antibacterial Photodynamic Therapy DOI Open Access

Ping He,

Mingxuan Jia,

Linfang Yang

et al.

Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 9, 2025

Abstract Photodynamic therapy (PDT) holds significant promise for antibacterial treatment, with its potential markedly amplified when using Type I photosensitizers (PSs). However, developing PSs remains a challenge due to lack of reliable design strategy. Herein, PS nanocluster is developed via self‐assembly zwitterionic small molecule (C3TH) superior PDT in vivo. Mechanism studies demonstrate that unique cross‐arranged C3TH within not only shortens intermolecular distance but also inhibits electronic‐vibrational coupling, thus facilitating photoinduced electron transfer form radical cation and anion autoionization reaction. Subsequently, these highly oxidizing or reducing radicals engage cascade photoredox generate efficient ·OH O 2 ‾·. As result, nanoclusters achieve 97.6% efficacy against MRSA at an ultralow dose, surpassing the commercial antibiotic Vancomycin by more than 8.8‐fold. These findings deepen understanding PDT, providing novel strategy PSs.

Language: Английский

Citations

2
Towards bioresource-based aggregation-induced emission luminogens from lignin β-O-4 motifs as renewable resources DOI Creative Commons
Tenglong Guo, Yuting Lin, Deng Pan

et al.

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: Sept. 28, 2023

One-pot synthesis of heterocyclic aromatics with good optical properties from phenolic β-O-4 lignin segments is high importance to meet value added biorefinery demands. However, executing this process remains a huge challenge due the incompatible reaction conditions depolymerization containing γ-OH functionalities and bioresource-based aggregation-induced emission luminogens (BioAIEgens) formation desired properties. In work, benzannulation reactions starting moieties 3-alkenylated indoles catalyzed by vanadium-based complexes have been successfully developed, affording wide range functionalized carbazoles up 92% yield. Experiments density functional theory calculations suggest that pathway involves selective cleavage double C-O bonds/Diels-Alder cycloaddition/dehydrogenative aromatization. Photophysical investigations show these carbazole products represent class BioAIEgens twisted intramolecular charge transfer. Distinctions behavior were revealed based on unique acceptor-donor-acceptor-type molecular conformations as well packings. This work features motifs renewable substrates, without need apply external oxidant/reductant systems. Here, we concise sustainable route AIE properties, building bridge between BioAIE materials.

Language: Английский

Citations

23
Piezofluorochromism in Hierarchical Porous π‐stacked Supermolecular Spring Frameworks from Aromatic Chiral Cages DOI
Dongxu Cui, Fu‐Quan Bai, Long Zhang

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(12)

Published: Feb. 1, 2024

Abstract Piezochromic materials that exhibit pressure‐dependent luminescence variations are attracting interest with wide potential applications in mechanical sensors, anticounterfeiting and storage devices. Crystalline porous (CPMs) have been widely studied piezochromism for highly tunable luminescence. Nevertheless, reversible high‐contrast emission response a pressure range is still challenging. Herein, the first example of hierarchical cage‐based πOF ( Cage ‐ 1 ) spring structure was synthesized by using aromatic chiral cages as building blocks. Its elastic properties evaluated based on bulk modulus (9.5 GPa) softer than most reported CPMs collapse point (20.0 significantly exceeds ever CPMs. As smart materials, displays linear achieves difference up to 154 nm. Pressure‐responsive limit 16 GPa, outperforming so far. Dedicated experiments density functional theory (DFT) calculations illustrate π–π interactions‐dominated controllable structural shrinkage porous‐spring‐structure‐mediated elasticity responsible outstanding piezofluorochromism.

Language: Английский

Citations

12
Electron-Withdrawing Substituents Enhance the Type I PDT and NIR-II Fluorescence of BODIPY J Aggregates for Bioimaging and Cancer Therapy DOI
Yu Zhu,

Fapu Wu,

Bingbing Zheng

et al.

Nano Letters, Journal Year: 2024, Volume and Issue: 24(27), P. 8287 - 8295

Published: June 28, 2024

Organic dyes with simultaneously boosted near-infrared-II (NIR-II) fluorescence, type I photodynamic therapy (PDT), and photothermal (PTT) in the aggregate state are still elusive due to unclear structure-function relationship. Herein, electron-withdrawing substituents introduced at 5-indolyl positions of BODIPY form tight J-aggregates for enhanced NIR-II fluorescence PDT/PTT. The introduction an electron-rich julolidine group

Language: Английский

Citations

11
A NIR‐II‐Emissive Organic Nanomedicine with Biomimetic Engineering for High‐Contrast Targeted Bioimaging and Multiple Phototherapies of Pancreatic Tumors DOI
Yiwei Wang, Jie Zhang, Yu Wang

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: July 2, 2024

Abstract Recent advances are achieved in the design and development of efficient organic photosensitizers (PSs), especially with fluorescence imaging navigation second near‐infrared (NIR‐II, 1000–1700 nm) region. However, there simply a handful NIR‐II emissive PSs oxygen‐independent capability due to scarcity high‐performance NIR‐responsive materials targeted delivery. Herein, NIR‐II‐emissive nanomedicine biomimetic engineering for multiple phototherapies pancreatic tumors is reported. An A‐D‐A‐type conjugated small‐molecule TPC designed used prepare water‐dispersive nanoparticles, which demonstrated high efficiency type I II photodynamic performances, good photothermal conversion 57%, bright emission quantum yield 9.8% under 808 nm light irradiation. With cancer cell membrane camouflage, high‐resolution bioimaging whole‐body blood vessels tumors. Antitumor experiments tumor elimination biosafety This work versatile enhanced tumor‐targeting superior phototheranostics, providing feasible idea evolution theranostics.

Language: Английский

Citations

9
Fluorination of Aza-BODIPY for Cancer Cell Plasma Membrane-Targeted Imaging and Therapy DOI Creative Commons

Anfeng Li,

Fang Wang, Yu Li

et al.

ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 2, 2025

Photodynamic therapy (PDT) holds great potential in cancer treatment, leveraging photosensitizers (PSs) to deliver targeted therapy. Fluorination can optimize the physicochemical and biological properties of PSs for better PDT performance. Here, we report some high-performance multifunctional specifically designed by fluorinating aza-BODIPY with perfluoro-tert-butoxymethyl (PFBM) groups. plays several roles, including enhancing selective cell uptake, plasma membrane (PM) targeting, inducing pyroptosis. It also enables fluorescence imaging (FLI) fluorine-19 magnetic resonance (19F MRI) as well facilitates oxygen delivery partial pressure (pO2) measurements. Comparative studies, along molecular dynamics simulations, reveal that fluorinated selectively eradicate cells oxidizing PM phospholipids singlet (1O2) pyroptosis, which effectively suppressed tumor growth self-oxygenated 19F MRI-FLI-guided mice. This study demonstrates a fluorination strategy tailoring PM-targeting materials beyond.

Language: Английский

Citations

1