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

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.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1360788

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

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Ligand manipulation of charge transfer excited state relaxation and spin crossover in [Fe(2,2′-bipyridine) ₂ (CN) ₂ ] Kjær, Kasper S.; Zhang, Wenkai; Alonso-Mori, Roberto Structural Dynamics, Vol. 4, Issue 4 https://doi.org/10.1063/1.4985017	journal	July 2017
Photoinduced valence tautomerism of a cobalt-dioxolene complex revealed with femtosecond M-edge XANES Ash, Ryan; Zhang, Kaili; Vura-Weis, Josh The Journal of Chemical Physics, Vol. 151, Issue 10 https://doi.org/10.1063/1.5115227	journal	September 2019

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