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Issue 11, 2015
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Chemically directing d-block heterometallics to nanocrystal surfaces as molecular beacons of surface structure

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Abstract

Our understanding of structure and bonding in nanoscale materials is incomplete without knowledge of their surface structure. Needed are better surveying capabilities responsive not only to different atoms at the surface, but also their respective coordination environments. We report here that d-block organometallics, when placed at nanocrystal surfaces through heterometallic bonds, serve as molecular beacons broadcasting local surface structure in atomic detail. This unique ability stems from their elemental specificity and the sensitivity of their d-orbital level alignment to local coordination environment, which can be assessed spectroscopically. Re-surfacing cadmium and lead chalcogenide nanocrystals with iron- or ruthenium-based molecular beacons is readily accomplished with trimethylsilylated cyclopentadienyl metal carbonyls. For PbSe nanocrystals with iron-based beacons, we show how core-level X-ray spectroscopies and DFT calculations enrich our understanding of both charge and atomic reorganization at the surface when beacons are bound.

Graphical abstract: Chemically directing d-block heterometallics to nanocrystal surfaces as molecular beacons of surface structure

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Publication details

The article was received on 22 Apr 2015, accepted on 28 Jul 2015 and first published on 28 Jul 2015


Article type: Edge Article
DOI: 10.1039/C5SC01474C
Citation: Chem. Sci., 2015,6, 6295-6304
  • Open access: Creative Commons BY license
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    Chemically directing d-block heterometallics to nanocrystal surfaces as molecular beacons of surface structure

    E. L. Rosen, K. Gilmore, A. M. Sawvel, A. T. Hammack, S. E. Doris, S. Aloni, V. Altoe, D. Nordlund, T. Weng, D. Sokaras, B. E. Cohen, J. J. Urban, D. F. Ogletree, D. J. Milliron, D. Prendergast and B. A. Helms, Chem. Sci., 2015, 6, 6295
    DOI: 10.1039/C5SC01474C

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