Journal
NANO RESEARCH
Volume 11, Issue 11, Pages 5787-5798Publisher
TSINGHUA UNIV PRESS
DOI: 10.1007/s12274-017-1935-2
Keywords
gold nanoclusters; Au-13; chirality; singlet oxygen; synchrotron radiation X-ray diffraction (XRD)
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Funding
- National Natural Science Foundation of China [21701168]
- Liaoning Natural Science Foundation [20170540897]
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In this study, 1,2-bis(diphenylphosphino)ethane (dppe) ligands are used to synthesize gold nanoclusters with an icosahedral Au-13 core. The nanoclusters are characterized and formulated as [Au-13(dppe)5Cl(2)]Cl-3 using synchrotron radiation X-ray diffraction, UV/Vis absorption spectroscopy, electrospray ionization mass spectrometry, and density functional theory (DFT) calculations. The bidentate feature of dppe ligands and the positions of coordinating surface gold atoms induce a helical arrangement that forms a propeller-like structure, which reduces the symmetry of the gold nanocluster to C-1. Therefore, dppe ligands perform as a directing agent to create chiral an ansa metallamacrocycle [Au-13(dppe)(5)Cl-2](3+) nanocluster, as confirmed by simulated electronic circular dichroism spectrum. The highest occupied molecular orbital (HOMO)-lowest unoccupied molecular orbital (LUMO) gap of the [Au-13(dppe)(5)Cl-2](3+) cluster is determined as approx. 1.9 eV, and further confirmed by ultraviolet photoemission spectroscopy analysis and DFT simulation. Furthermore, the photoactivity of [Au-13(dppe)(5)Cl-2](3+) is investigated, with the nanocluster shown to possess near-infrared photoluminescence properties, which can be employed for O-1(2) photogeneration. The quantum yield of O-1(2) photogeneration using the [Au-13(dppe)(5)Cl-2](3+) nanocluster is up to 0.71, which is considerably higher than those of anthracene (an organic dye), and Au-25 and Au-38 nanoclusters.
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