Size and Structure Dependence of Electronic States in Thiolate-Protected Gold Nanoclusters of Au25(SR)18, Au38(SR)24, and Au144(SR)60

Ohta, Tsutomu; Shibuta, Masahiro; Tsunoyama, Hironori; Negishi, Yuichi; Eguchi, Toyoaki; Nakajima, Atsushi

doi:10.1021/jp400785f

Cited by 54 publications

(59 citation statements)

References 56 publications

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“….7-eV separation between the maximum intensity of the peaks at 83.5 and 87.2 eV perceived in the Au-ZnO heterostructure could be ascribed to the spin-orbit components Au 4f 7/2 and Au 4f 5/2 of the metallic gold [59][60][61][62][63]. Quite intriguing was the fact that the recorded 3.7-eV peak separation is very similar to the separation of the same peaks in the previous report [63].…”

Section: Resultssupporting

confidence: 81%

Nanoscale Au-ZnO Heterostructure Developed by Atomic Layer Deposition Towards Amperometric H2O2 Detection

Wei

Verpoort

et al. 2020

Nanoscale Res Lett

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Nanoscale Au-ZnO heterostructures were fabricated on 4-in. SiO 2 /Si wafers by the atomic layer deposition (ALD) technique. Developed Au-ZnO heterostructures after post-deposition annealing at 250°C were tested for amperometric hydrogen peroxide (H 2 O 2) detection. The surface morphology and nanostructure of Au-ZnO heterostructures were examined by field emission scanning electron microscopy (FE-SEM), Raman spectroscopy, atomic force microscopy (AFM), X-ray photoelectron spectroscopy (XPS), etc. Additionally, the electrochemical behavior of Au-ZnO heterostructures towards H 2 O 2 sensing under various conditions is assessed by chronoamperometry and electrochemical impedance spectroscopy (EIS). The results showed that ALD-fabricated Au-ZnO heterostructures exhibited one of the highest sensitivities of 0.53 μA μM −1 cm −2 , the widest linear H 2 O 2 detection range of 1.0 μM-120 mM, a low limit of detection (LOD) of 0.78 μM, excellent selectivity under the normal operation conditions, and great long-term stability. Utilization of the ALD deposition method opens up a unique opportunity for the improvement of the various capabilities of the devices based on Au-ZnO heterostructures for amperometric detection of different chemicals.

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Section: Resultssupporting

confidence: 81%

Nanoscale Au-ZnO Heterostructure Developed by Atomic Layer Deposition Towards Amperometric H2O2 Detection

Wei

Verpoort

et al. 2020

Nanoscale Res Lett

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“…Chemie withdrawing nature of the thiol ligands. [37] Notably,t he Au 4f 7/2 binding energies sequenced slightly positive shifts from Au 25 À ,A u 25 0 ,t oA u 25 + ,w hich was consistent with X-ray absorption near edge structure (XANES) studies (Figure 6d). Extended X-ray absorption fine structure (EXAFS) experiments indicated that local coordination environments in the Au 25 clusters were not obviously different (Supporting Information, Figure S12, Table S1).…”

Section: Methodssupporting

confidence: 77%

Reactivity and Lability Modulated by a Valence Electron Moving in and out of 25‐Atom Gold Nanoclusters

Sun

et al. 2020

Angew Chem Int Ed

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The emergence of atomically precise metal nanoclusters with unique electronic structures provides access to currently inaccessible catalytic challenges at the single‐electron level. We investigate the catalytic behavior of gold Au25(SR)18 nanoclusters by monitoring an incoming and outgoing free valence electron of Au 6s1. Distinct performances are revealed: Au25(SR)18− is generated upon donation of an electron to neutral Au25(SR)180 and this is associated with a loss in reactivity, whereas Au25(SR)18+ is generated from dislodgment of an electron from neutral Au25(SR)180 with a loss in stability. The reactivity diversity of the three Au25(SR)18 clusters stems from different affinities with reactants and the extent of intramolecular charge migration during the reactions, which are closely associated with the valence occupancies of the clusters varied by one electron. The stability difference in the three clusters is attributed to their different equilibria, which are established between the AuSR dissociation and polymerization influenced by one electron.

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“…1,2 Compared to larger size gold nanoparticles, they do not possess plasmonic properties but exhibit long-lived excited states. 3,4 The long-lived excited state of the gold cluster has an excited triple state character and it is attributed to the formation of the ligand-to-metal charge transfer (LMCT) state. These clusters which carry a metal core of few gold atoms and a shell of chemically bound thiols are known to exhibit molecularlike properties.…”

Section: Introductionmentioning

confidence: 99%

Glutathione-capped gold nanoclusters: photoinduced energy transfer and singlet oxygen generation $$^{\S }$$ §

Talavera

Kamat

2018

J Chem Sci

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Glutathione-capped gold clusters prepared in an aqueous medium are known to exhibit excellent photosensitizing properties. We have now successfully transferred these gold clusters in an organic medium while retaining all the characteristic excited state properties. These gold clusters can be further modified with organic ligands such as 2-Phenylethanethiol (PET). The gold clusters in organic medium exhibit enhanced emission yield (f = 0.15) compared to that in an aqueous medium (f = 0.08). The excited state lifetimes of 3.7 μs (untreated) and 1.5 μs (PET treated) in toluene are also greater than the lifetime observed in aqueous solution (0.77 μs). By employing laser flash photolysis we are able to induce triplet energy transfer to β-carotene and oxygen. A singlet oxygen generation with the efficiency of 13% was observed in these experiments. The excited state properties of glutathione-capped gold clusters further shows its importance as a photosensitizer in light energy conversion and biomedical applications

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Size and Structure Dependence of Electronic States in Thiolate-Protected Gold Nanoclusters of Au₂₅(SR)₁₈, Au₃₈(SR)₂₄, and Au₁₄₄(SR)₆₀

Cited by 54 publications

References 56 publications

Nanoscale Au-ZnO Heterostructure Developed by Atomic Layer Deposition Towards Amperometric H2O2 Detection

Nanoscale Au-ZnO Heterostructure Developed by Atomic Layer Deposition Towards Amperometric H2O2 Detection

Reactivity and Lability Modulated by a Valence Electron Moving in and out of 25‐Atom Gold Nanoclusters

Glutathione-capped gold nanoclusters: photoinduced energy transfer and singlet oxygen generation $$^{\S }$$ §

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