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Crystalline Divinyldiarsene Radical Cations and Dications.

Mahendra K Sharma¹, Sebastian Blomeyer¹, Beate Neumann¹

¹Anorganische Molekülchemie und Katalyse, Lehrstuhl für Anorganische Chemie und Strukturchemie, Centrum für Molekulare Materialien, Fakultät für Chemie, Universität Bielefeld, Universitätsstr. 25, 33615, Bielefeld, Germany.

Angewandte Chemie (International Ed. in English)

|September 26, 2019

Summary

New arsenic compounds, divinyldiarsene radical cations and dications, were synthesized and characterized. Sequential oxidation alters arsenic-arsenic and carbon-arsenic bond lengths, impacting their electronic and optical properties.

Keywords:

arsenic dications main-group compounds radicals π ligands

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Area of Science:

Organometallic Chemistry
Inorganic Chemistry
Materials Science

Background:

Divinyldiarsenes are precursors to arsenic-containing compounds.
Understanding the electronic structure of arsenic species is crucial for developing new materials.

Purpose of the Study:

To synthesize and characterize novel divinyldiarsene radical cations and dications.
To investigate the structural and electronic changes upon sequential one-electron oxidation.
To explore the properties of these arsenic compounds using spectroscopic and computational methods.

Main Methods:

Synthesis of divinyldiarsene radical cations and dications using sequential oxidation with GaCl3.
Characterization using X-ray diffraction, cyclic voltammetry, EPR/NMR spectroscopy, and UV/vis absorption spectroscopy.
Theoretical analysis using Density Functional Theory (DFT) calculations.

Main Results:

Readily accessible crystalline solids of divinyldiarsene radical cations [{(NHC)C(Ph)}As]2(GaCl4) and dications [{(NHC)C(Ph)}As]2(GaCl4)2 were obtained.
Sequential oxidation led to predictable changes in bond lengths: elongation of the As=As bond and contraction of C-As bonds.
UV/vis spectra showed strong visible absorptions, and EPR spectra revealed coupling with 75As nuclei.

Conclusions:

The study successfully synthesized and characterized new arsenic radical cations and dications.
Electronic and structural properties are tunable via sequential oxidation.
These findings contribute to the understanding of arsenic bonding and reactivity.