期刊
ACS NANO
卷 8, 期 6, 页码 6431-6439出版社
AMER CHEMICAL SOC
DOI: 10.1021/nn501970v
关键词
nanoclusters; monolayer-protected clusters; atomic PDF
类别
资金
- NSF [CHE-1255519]
- U.S. DOE [DE-AC02-06CH11357]
- ORNL's Center for Nanophase Materials Sciences (CNMS) - Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1255519] Funding Source: National Science Foundation
Obtaining monodisperse nanocrystals and determining their composition to the atomic level and their atomic structure is highly desirable but is generally lacking. Here, we report the discovery and comprehensive characterization of a 2.9 nm plasmonic nanocrystal with a composition of Au-940 +/- 20(SCH2CH2Ph)(160 +/- 4), which is the largest mass spectrometrically characterized gold thiolate nanoparticle produced to date. The compositional assignment has been made using electrospray ionization and matrix-assisted laser desorption ionization mass spectrometry (MS). The MS results show an unprecedented size monodispersity, where the number of Au atoms varies by only 40 atoms (940 +/- 20). The mass spectrometrically determined composition and size are supported by aberration-corrected scanning transmission electron microscopy (STEM) and synchrotron-based methods such as atomic pair distribution function (PEW) and small-angle X-ray scattering (SAXS). Lower-resolution STEM images show an ensemble of particles-1000s per frame visually demonstrating monodispersity. Modeling of SAXS data on statistically significant nanoparticle population approximately 10(12) individual nanoparticles shows that the diameter is 3.0 +/- 0.2 nm, supporting mass spectrometry and electron microscopy results on monodispersity. Atomic PDF based on high-energy X-ray diffraction experiments shows decent match with either a Marks decahedral or truncated octahedral structure. Atomic resolution STEM images of single particles and their fast Fourier transform suggest face-centered cubic arrangement. UV-visible spectroscopy data show that Faradaurate-940 supports a surface plasmon resonance peak at similar to 505 nm. These monodisperse plasmonic nanoparticles minimize averaging effects and have potential application in solar cells, nano-optical devices, catalysis, and drug delivery.
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