Electron Cartography in Clusters

Hernández Sánchez, Raúl; Champsaur, Anouck M.; Choi, Bonnie; Wang, Suyin Grass; Bu, Wei; Roy, Xavier; Chen, Yu‐Sheng; Steigerwald, Michael L.; Nuckolls, Colin; Paley, Daniel W.

doi:10.1002/anie.201806426

Title: Electron Cartography in Clusters

Journal Article · 21 September 2018 · Angewandte Chemie (International Edition)

DOI: https://doi.org/10.1002/anie.201806426 · OSTI ID:1472173

^[1]; Champsaur, Anouck M. ^[1]; Choi, Bonnie ^[1]; Wang, Suyin Grass ^[2]; Bu, Wei ^[2]; Roy, Xavier ^[1]; Chen, Yu‐Sheng ^[2]; Steigerwald, Michael L. ^[1];

^[1]; Paley, Daniel W. ^[1]

Department of Chemistry Columbia University New York NY 10027 USA
ChemMatCARS The University of Chicago Argonne IL 60439 USA

Abstract Deconvoluting the atom‐specific electron density within polynuclear systems remains a challenge. A multiple‐wavelength anomalous diffraction study on four clusters that share the same [Co ₆ Se ₈ ] core was performed. Two cluster types were designed, one having a symmetric ligand sphere and the other having an asymmetric ligand sphere. It was found that in the neutral, asymmetric, CO‐bound cluster, the Co−CO site is more highly oxidized than the other five Co atoms; when an electron is removed, the hole is distributed among the Se atoms. In the neutral, symmetric cluster, the Co atoms divide by electron population into two sets of three, each set being meridional; upon removal of an electron, the hole is distributed among all the Co atoms. This ligand‐dependent tuning of the electron/hole distribution relates directly to the performance of clusters in biological and synthetic systems.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1472173

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 42 Vol. 57; ISSN 1433-7851

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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