Four chalcogenophene-fused acenes containing O, S, Se, or Te, respectively, were presented, and the chalcogenophene effect on linear and nonlinear optics was systematically investigated. Their excited-state absorption performance and two-photon absorption (TPA) capacity could be modulated by the incorporating chalcogen atoms. The experimental results showed that the heavy chalcogen facilitated the intersystem crossing resulting in the presence of the triplet state absorption for and , and the TPA capacity gradually increased with the atomic size of the chalcogens. The theoretical calculation inferred that their nonlinear optical performance was closely related to the contributions of the chalcogenophene component to heterotwistacenes in the final excited state. In addition, was able to work under various laser pulses from femtoseconds to nanoseconds.
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