Ligand impact on reactive oxygen species generation of Au10 and Au25 nanoclusters upon one- and two-photon excitation
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,...
| Main Authors: | , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2023-05-01
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| Series: | Communications Chemistry |
| Online Access: | https://doi.org/10.1038/s42004-023-00895-5 |
| _version_ | 1797818138442596352 |
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| author | Hussein Fakhouri Martina Perić Bakulić Issan Zhang Hao Yuan Dipankar Bain Fabien Rondepierre Pierre-François Brevet Željka Sanader Maršić Rodolphe Antoine Vlasta Bonačić-Koutecký Dusica Maysinger |
| author_facet | Hussein Fakhouri Martina Perić Bakulić Issan Zhang Hao Yuan Dipankar Bain Fabien Rondepierre Pierre-François Brevet Željka Sanader Maršić Rodolphe Antoine Vlasta Bonačić-Koutecký Dusica Maysinger |
| author_sort | Hussein Fakhouri |
| collection | DOAJ |
| description | 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 (Au10) and atomically-precise gold nanoclusters (Au25), and investigate the influence of ligands on their photoexcitation. With the ability of atomically-precise nanochemistry, we produce Au10SG10, Au10AcCys10, Au25SG18, and Au25AcCys18 (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. |
| first_indexed | 2024-03-13T09:03:33Z |
| format | Article |
| id | doaj.art-53fda083639543d8a168882e9fc0a27d |
| institution | Directory Open Access Journal |
| issn | 2399-3669 |
| language | English |
| last_indexed | 2024-03-13T09:03:33Z |
| publishDate | 2023-05-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Communications Chemistry |
| spelling | doaj.art-53fda083639543d8a168882e9fc0a27d2023-05-28T11:10:35ZengNature PortfolioCommunications Chemistry2399-36692023-05-016111010.1038/s42004-023-00895-5Ligand impact on reactive oxygen species generation of Au10 and Au25 nanoclusters upon one- and two-photon excitationHussein Fakhouri0Martina Perić Bakulić1Issan Zhang2Hao Yuan3Dipankar Bain4Fabien Rondepierre5Pierre-François Brevet6Željka Sanader Maršić7Rodolphe Antoine8Vlasta Bonačić-Koutecký9Dusica Maysinger10Institut Lumière Matière, University of Lyon, Université Claude Bernard Lyon 1, CNRSCenter of Excellence for Science and Technology, Integration of Mediterranean Region (STIM), Faculty of Science, University of SplitDepartment of Pharmacology and Therapeutics, McGill UniversityInstitut Lumière Matière, University of Lyon, Université Claude Bernard Lyon 1, CNRSInstitut Lumière Matière, University of Lyon, Université Claude Bernard Lyon 1, CNRSInstitut Lumière Matière, University of Lyon, Université Claude Bernard Lyon 1, CNRSInstitut Lumière Matière, University of Lyon, Université Claude Bernard Lyon 1, CNRSFaculty of Science, University of SplitInstitut Lumière Matière, University of Lyon, Université Claude Bernard Lyon 1, CNRSCenter of Excellence for Science and Technology, Integration of Mediterranean Region (STIM), Faculty of Science, University of SplitDepartment of Pharmacology and Therapeutics, McGill UniversityAbstract 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 (Au10) and atomically-precise gold nanoclusters (Au25), and investigate the influence of ligands on their photoexcitation. With the ability of atomically-precise nanochemistry, we produce Au10SG10, Au10AcCys10, Au25SG18, and Au25AcCys18 (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.https://doi.org/10.1038/s42004-023-00895-5 |
| spellingShingle | Hussein Fakhouri Martina Perić Bakulić Issan Zhang Hao Yuan Dipankar Bain Fabien Rondepierre Pierre-François Brevet Željka Sanader Maršić Rodolphe Antoine Vlasta Bonačić-Koutecký Dusica Maysinger Ligand impact on reactive oxygen species generation of Au10 and Au25 nanoclusters upon one- and two-photon excitation Communications Chemistry |
| title | Ligand impact on reactive oxygen species generation of Au10 and Au25 nanoclusters upon one- and two-photon excitation |
| title_full | Ligand impact on reactive oxygen species generation of Au10 and Au25 nanoclusters upon one- and two-photon excitation |
| title_fullStr | Ligand impact on reactive oxygen species generation of Au10 and Au25 nanoclusters upon one- and two-photon excitation |
| title_full_unstemmed | Ligand impact on reactive oxygen species generation of Au10 and Au25 nanoclusters upon one- and two-photon excitation |
| title_short | Ligand impact on reactive oxygen species generation of Au10 and Au25 nanoclusters upon one- and two-photon excitation |
| title_sort | ligand impact on reactive oxygen species generation of au10 and au25 nanoclusters upon one and two photon excitation |
| url | https://doi.org/10.1038/s42004-023-00895-5 |
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