Hard X‑ray-Induced Valence Tautomeric Interconversion
in Cobalt‑o‑Dioxolene Complexes
Version 2 2017-11-18, 01:03
Version 1 2017-09-19, 15:52
Posted on 2017-11-18 - 01:03
Valence
tautomeric interconversion (VTI) is a reversible process
occurring in metal complexes in which an intramolecular metal–ligand
electron transfer is accompanied by a change of metal ion spin state,
creating two switchable electronic states (redox isomers). Herein,
we describe the low-temperature, 30–100 K, single-crystal study
of the [Co(diox)2(4-CN-py)2]·benzene complex (1) (diox =
3,5-di-t-butylsemiquinonate (SQ•‑) and/or 3,5-di-t-butylcatecholate (Cat2–) radical; 4-CN-py = 4-cyano-pyridine) using hard synchrotron X-ray
radiation with different intensities. We demonstrate for the first
time that hard X-rays can induce VTI, and that the interconversion
molar fraction is dependent on both intensity and exposure time. This
in turn shows that X-rays, as a probe, might be altering the very
nature of many structures under investigation at low temperatures,
and consequently their properties. Our findings add new perspectives
to VTI studies and might be of significant interest to the entire
community investigating photoresponsive complexes.
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Francisco, Thiago
M.; Gee, William J.; Shepherd, Helena J.; Warren, Mark R.; Shultz, David A.; Raithby, Paul R.; et al. (2017). Hard X‑ray-Induced Valence Tautomeric Interconversion
in Cobalt‑o‑Dioxolene Complexes. ACS Publications. Collection. https://doi.org/10.1021/acs.jpclett.7b01794
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AUTHORS (7)
TF
Thiago
M. Francisco
WG
William J. Gee
HS
Helena J. Shepherd
MW
Mark R. Warren
DS
David A. Shultz
PR
Paul R. Raithby
CP
Carlos B. Pinheiro