Charge and Spin-State Characterization of Cobalt Bis(o-dioxolene) Valence Tautomers Using Co Kβ X-ray Emission and L-Edge X-ray Absorption Spectroscopies

Liang, H. Winnie; Kroll, Thomas; Nordlund, Dennis; Weng, Tsu -Chien; Sokaras, Dimosthenis; Pierpont, Cortlandt G.; Gaffney, Kelly J.

doi:10.1021/acs.inorgchem.6b01666

Title: Charge and Spin-State Characterization of Cobalt Bis(o-dioxolene) Valence Tautomers Using Co Kβ X-ray Emission and L-Edge X-ray Absorption Spectroscopies

Journal Article · Fri Dec 30 00:00:00 EST 2016 · Inorganic Chemistry

DOI:https://doi.org/10.1021/acs.inorgchem.6b01666· OSTI ID:1360788

^[1]; Kroll, Thomas ^[2]; Nordlund, Dennis ^[2]; Weng, Tsu -Chien ^[3]; Sokaras, Dimosthenis ^[2]; Pierpont, Cortlandt G. ^[4]; Gaffney, Kelly J. ^[2]

Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Center for High Pressure Science & Technology Advanced Research, Shanghai (People's Republic of China)
Univ. of Colorado, Boulder, CO (United States)

The valence tautomeric states of Co(phen)(3,5-DBQ)₂ and Co(tmeda)(3,5-DBQ)₂, where 3,5-DBQ is either the semiquinone (SQ^–) or catecholate (Cat^2–) form of 3,5-di-tert-butyl-1,2-benzoquinone, have been examined by a series of cobalt-specific X-ray spectroscopies. In this work, we have utilized the sensitivity of 1s3p X-ray emission spectroscopy (Kβ XES) to the oxidation and spin states of 3d transition-metal ions to determine the cobalt-specific electronic structure of valence tautomers. A comparison of their Kβ XES spectra with the spectra of cobalt coordination complexes with known oxidation and spin states demonstrates that the low-temperature valence tautomer can be described as a low-spin Co^III configuration and the high-temperature valence tautomer as a high-spin Co^II configuration. This conclusion is further supported by Co L-edge X-ray absorption spectroscopy (L-edge XAS) of the high-temperature valence tautomers and ligand-field atomic-multiplet calculations of the Kβ XES and L-edge XAS spectra. In conclusion, the nature and strength of the magnetic exchange interaction between the cobalt center and SQ^– in cobalt valence tautomers is discussed in view of the effective spin at the Co site from Kβ XES and the molecular spin moment from magnetic susceptibility measurements.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: P41 GM103393; AC02-76SF00515

OSTI ID:: 1360788

Journal Information:: Inorganic Chemistry, Vol. 56, Issue 2; ISSN 0020-1669

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 27 works

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Tracking excited-state charge and spin dynamics in iron coordination complexes Zhang, Wenkai; Alonso-Mori, Roberto; Bergmann, Uwe Nature, Vol. 509, Issue 7500 https://doi.org/10.1038/nature13252	journal	May 2014
Picosecond Time-Resolved X-Ray Emission Spectroscopy: Ultrafast Spin-State Determination in an Iron Complex Vankó, György; Glatzel, Pieter; Pham, Van-Thai Angewandte Chemie International Edition, Vol. 49, Issue 34 https://doi.org/10.1002/anie.201000844	journal	July 2010

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