DFT studies on the electronic properties of organometallic-polyoxomolybdate anions [Cpn∗Mo6O19−n](2−n)− (n = 1 or 2): Revealing bonding features of Cp∗-Mo

► This study reports the DFT studies on POM-incorporated organometallics. ► The structure-property relationship of these polyanions is presented. ► The Cp∗-Mo bond features two nonclassical σ bonds and two π bonds. ► These polyanions show poor NLO responses in comparison with [Mo6O18NPh]2−.