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Ba(CO)+ and Ba(CO)− have been produced and isolated in a low‐temperature neon matrix. The observed C−O stretching wavenumber for Ba(CO)+ of 1911.2 cm−1 is the most red‐shifted value measured for any metal carbonyl cations, indicating strong π backdonation of electron density from Ba+ to CO. Quantum chemical calculations indicate that Ba(CO)+ has a 2Π reference state, which correlates with the 2D(5d...
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