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配体对金及金纳米团簇在单光子和双光子激发下活性氧生成的影响。

Ligand impact on reactive oxygen species generation of Au and Au nanoclusters upon one- and two-photon excitation.

作者信息

Fakhouri Hussein, Bakulić Martina Perić, Zhang Issan, Yuan Hao, Bain Dipankar, Rondepierre Fabien, Brevet Pierre-François, Maršić Željka Sanader, Antoine Rodolphe, Bonačić-Koutecký Vlasta, Maysinger Dusica

机构信息

Institut Lumière Matière, University of Lyon, Université Claude Bernard Lyon 1, CNRS, F-69622, Lyon, France.

Center of Excellence for Science and Technology, Integration of Mediterranean Region (STIM), Faculty of Science, University of Split, Ruđera Boškovića 33, 21000, Split, Croatia.

出版信息

Commun Chem. 2023 May 22;6(1):97. doi: 10.1038/s42004-023-00895-5.

DOI:10.1038/s42004-023-00895-5
PMID:37217712
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10203263/
Abstract

In photodynamic therapy (PDT), light-sensitive photosensitizers produce reactive oxygen species (ROS) after irradiation in the presence of oxygen. Atomically-precise thiolate-protected gold nanoclusters are molecule-like nanostructures with discrete energy levels presenting long lifetimes, surface biofunctionality, and strong near-infrared excitation ideal for ROS generation in PDT. We directly compare thiolate-gold macromolecular complexes (Au) and atomically-precise gold nanoclusters (Au), and investigate the influence of ligands on their photoexcitation. With the ability of atomically-precise nanochemistry, we produce AuSG, AuAcCys, AuSG, and AuAcCys (SG: glutathione; AcCys: N-acetyl-cysteine) fully characterized by high-resolution mass spectrometry. Our theoretical investigation reveals key factors (energetics of excited states and structural influence of surface ligands) and their relative importance in singlet oxygen formation upon one- and two-photon excitation. Finally, we explore ROS generation by gold nanoclusters in living cells with one- and two-photon excitation. Our study presents in-depth analyses of events within gold nanoclusters when photo-excited both in the linear and nonlinear optical regimes, and possible biological consequences in cells.

摘要

在光动力疗法（PDT）中，光敏性光敏剂在有氧存在的情况下经照射后会产生活性氧（ROS）。原子精确的硫醇盐保护金纳米团簇是具有离散能级的分子状纳米结构，具有长寿命、表面生物功能性以及适合在光动力疗法中产生ROS的强近红外激发特性。我们直接比较硫醇盐 - 金大分子复合物（Au）和原子精确的金纳米团簇（Au），并研究配体对其光激发的影响。借助原子精确的纳米化学能力，我们制备了通过高分辨率质谱完全表征的AuSG、AuAcCys、AuSG和AuAcCys（SG：谷胱甘肽；AcCys：N - 乙酰 - 半胱氨酸）。我们的理论研究揭示了关键因素（激发态能量学和表面配体的结构影响）及其在单光子和双光子激发下单线态氧形成中的相对重要性。最后，我们探索了金纳米团簇在活细胞中通过单光子和双光子激发产生ROS的情况。我们的研究对金纳米团簇在线性和非线性光学区域光激发时内部发生的事件以及细胞中可能的生物学后果进行了深入分析。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d09b/10203263/3f0cfe9331b6/42004_2023_895_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d09b/10203263/4e4c5dd50c5f/42004_2023_895_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d09b/10203263/ba9caf4ac052/42004_2023_895_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d09b/10203263/eae67febd35e/42004_2023_895_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d09b/10203263/b2567ed9e70a/42004_2023_895_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d09b/10203263/aa039f750ee9/42004_2023_895_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d09b/10203263/3f0cfe9331b6/42004_2023_895_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d09b/10203263/4e4c5dd50c5f/42004_2023_895_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d09b/10203263/ba9caf4ac052/42004_2023_895_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d09b/10203263/eae67febd35e/42004_2023_895_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d09b/10203263/b2567ed9e70a/42004_2023_895_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d09b/10203263/aa039f750ee9/42004_2023_895_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d09b/10203263/3f0cfe9331b6/42004_2023_895_Fig6_HTML.jpg

相似文献

[1]
Ligand impact on reactive oxygen species generation of Au and Au nanoclusters upon one- and two-photon excitation.

Commun Chem. 2023-5-22

[2]
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[3]
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[4]
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[5]
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[6]
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[7]
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[8]
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[9]
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[10]
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引用本文的文献

[1]
BioGoldNCDB: A Database of Gold Nanoclusters and Related Nanoparticles with Biomedical Activity.

Molecules. 2025-8-7

[2]
Gold Nanoclusters as High Resolution NIR-II Theranostic Agents.

Chem Biomed Imaging. 2024-6-18

[3]
Dual-quartet phosphorescent emission in the open-shell MAg (M = Pt, Pd) nanoclusters.

Nat Commun. 2024-7-16

本文引用的文献

[1]
Atomistic insight into the aggregation of [Au(SR)] nanoclusters.

Nanoscale Adv. 2020-5-18

[2]
Gold Nanoclusters-Based NIR-II Photosensitizers with Catalase-like Activity for Boosted Photodynamic Therapy.

Pharmaceutics. 2022-8-7

[3]
Direct Interaction between -Acetylcysteine and Cytotoxic Electrophile-An Overlooked In Vitro Mechanism of Protection.

Antioxidants (Basel). 2022-7-29

[4]
Defining roles of specific reactive oxygen species (ROS) in cell biology and physiology.

Nat Rev Mol Cell Biol. 2022-7

[5]
Insights into the Impact of Gold Nanoclusters AuSG on Human Microglia.

ACS Chem Neurosci. 2022-2-16

[6]
Singlet Oxygen Generation, Quenching and Reactivity with Metal Thiolates.

Photochem Photobiol. 2021-11

[7]
The mechanism of action of N-acetylcysteine (NAC): The emerging role of HS and sulfane sulfur species.

Pharmacol Ther. 2021-12

[8]
Quantitative kinetics of intracellular singlet oxygen generation using a fluorescence probe.

Sci Rep. 2020-6-30

[9]
BSA-capped gold nanoclusters as potential theragnostic for skin diseases: Photoactivation, skin penetration, in vitro, and in vivo toxicity.

Mater Sci Eng C Mater Biol Appl. 2020-7

[10]
The Molecular Mechanisms Regulating the KEAP1-NRF2 Pathway.

Mol Cell Biol. 2020-6-15

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