Bucket Effect to Improve Third-Order Nonlinear Optical Response on Metal-Heteroaromatic Compounds

Carbolong compounds as a metal-heteroaromatic compound with both organometallic properties andπ-conjugated systems exhibit great potential in organic catalysis and optoelectronic devices.In this work,for the first time,the“Bucket Effect”is revealed to promote the third-order nonlinear optical(NLO)performance in metal-heteroaromatic compounds.We have successfully constructed and investigated a series of novel metallapentalenes with higher third-order NLO performance benefited from the“Bucket Effect”.Meanwhile,aromaticity and electron−hole analysis further confirm the internal homogeneity of organometallic rings,reduced bandgap,and enhanced low-energy peak response resulted in the enhanced third-order NLO effects.The success of this work is discovering an emerging material library of high third-order NLO effects,and illustrating the feasibility of engineering the high response metal-heteroaromatic optical devices at the electronic structure level.