The β-diketiminate bonded Al(I)-compound (L)Al (L = HC2, Ar = 2,6-iPr2C6H3) reacted with the C=E (E = Se, Te) bonds of N-heterocyclic selenourea and tellurourea (iPrNHC=E) to exclusively afford [(LAl(iPrNHC)=E] (E = Se, 1; Te, 2), respectively. Structural and spectroscopic characterization were done, and the bonding details were experiementally and theoretically studied.

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