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Importance of double-resonance effects in two-photon absorption properties of Au₂₅(SR)₁₈.

ABSTRACT: The two-photon absorption (TPA) cross-sections of small thiolate-protected gold clusters have been shown to be much larger than typical small organic molecules. In comparison with larger nanoparticles, their TPA cross-sections per gold atom are also found to be larger. Theoretical simulations have suggested that the large enhancement of these TPA cross-sections comes from a one-photon double-resonance mechanism. However, it remains difficult to simulate TPA cross-sections of thiolate-protected gold clusters due to their large system size and a high density of states. In this work, we report a time-dependent density functional theory (TDDFT) study of the TPA spectra of the Au₂₅(SR)₁₈^- cluster based on a damped response theory formalism. Damped response theory enables a consistent treatment of on- and off-resonance molecular properties even for molecules with a high density of states, and thus is well-suited for studying the TPA properties of gold clusters. Our results indicate that the one- and two-photon double-resonance effect is much smaller than previously found, and thus is unlikely to be the main cause of the large TPA cross-sections found experimentally. The effect of symmetry breaking of the Au₂₅(SR)₁₈^- cluster due to the ligands on the TPA cross-sections has been studied and was found to only slightly increase the cross-section. Furthermore, by comparing with larger nanoparticles we find that the TPA cross-section per gold atom scales linearly with the diameter of the particles, and that the Kerr non-linear response of the Au₂₅(SR)₁₈^- cluster is on the same order as that of bulk gold films.

SUBMITTER: Hu Z

PROVIDER: S-EPMC5471455 | biostudies-literature | 2017 Jun

REPOSITORIES: biostudies-literature

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Importance of double-resonance effects in two-photon absorption properties of Au<sub>25</sub>(SR)<sub>18</sub>.

Hu Zhongwei Z Jensen Lasse L

Chemical science 20170419 6

The two-photon absorption (TPA) cross-sections of small thiolate-protected gold clusters have been shown to be much larger than typical small organic molecules. In comparison with larger nanoparticles, their TPA cross-sections per gold atom are also found to be larger. Theoretical simulations have suggested that the large enhancement of these TPA cross-sections comes from a one-photon double-resonance mechanism. However, it remains difficult to simulate TPA cross-sections of thiolate-protected g ...[more]

PMID: 28626569

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Project description:Antimicrobial photodynamic therapy (aPDT) has beneficial effects in dental treatment. We applied captopril-protected gold (Au25(Capt)18) clusters as a novel photosensitizer for aPDT. Photoexcited Au clusters under light irradiation generated singlet oxygen (1O2). Accordingly, the antimicrobial and cytotoxic effects of Au25(Capt)18 clusters under dental blue light-emitting diode (LED) irradiation were evaluated. 1O2 generation of Au25(Capt)18 clusters under blue LED irradiation (420-460 nm) was detected by a methotrexate (MTX) probe. The antimicrobial effects of photoexcited Au clusters (0, 5, 50, and 500 μg/mL) on oral bacterial cells, such as Streptococcus mutans, Aggregatibacter actinomycetemcomitans, and Porphyromonas gingivalis, were assessed by morphological observations and bacterial growth experiments. Cytotoxicity testing of Au clusters and blue LED irradiation was then performed against NIH3T3 and MC3T3-E1 cells. In addition, the biological performance of Au clusters (500 μg/mL) was compared to an organic dye photosensitizer, methylene blue (MB; 10 and 100 μg/mL). We confirmed the 1O2 generation ability of Au25(Capt)18 clusters through the fluorescence spectra of oxidized MTX. Successful application of photoexcited Au clusters to aPDT was demonstrated by dose-dependent decreases in the turbidity of oral bacterial cells. Morphological observation revealed that application of Au clusters stimulated destruction of bacterial cell walls and inhibited biofilm formation. Aggregation of Au clusters around bacterial cells was fluorescently observed. However, photoexcited Au clusters did not negatively affect the adhesion, spreading, and proliferation of mammalian cells, particularly at lower doses. In addition, application of Au clusters demonstrated significantly better cytocompatibility compared to MB. We found that a combination of Au25(Capt)18 clusters and blue LED irradiation exhibited good antimicrobial effects through 1O2 generation and biosafe characteristics, which is desirable for aPDT in dentistry.

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Importance of double-resonance effects in two-photon absorption properties of Au25(SR)18.

Publications

Importance of double-resonance effects in two-photon absorption properties of Au<sub>25</sub>(SR)<sub>18</sub>.

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Importance of double-resonance effects in two-photon absorption properties of Au₂₅(SR)₁₈.