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Three new heterocyclic-chalcone (HC) derivatives consisting of the π-conjugated system attached to anthracene moiety were proposed for nonlinear optical properties and optical limiting application. The NLO behavior is confirmed through obtained χ 3  by Z-scan method. The closed aperture z-scan showed the HC possesses a self-defocusing effect with a negative nonlinear refractive index,  n2  ∼ 10 −8  cm/W, with a magnitude of real part of the third-order nonlinear optical susceptibilities, Re χ (3)  of the order of 10 −7  esu. Open Z-scan results showed that the HC samples demonstrate a reverse saturable absorption (RSA), β ∼ 10 −4  cm/W, corresponding to large imaginary parts, Im χ (3)  in the order of 10 −6  esu. Overall, the Z-scan analysis unveils an excellent value of χ 3  in order of 10 −6  which indicates good nonlinear material under 532 nm continuous wave laser. The optical limiting study reveals that AC exhibit a strong limiting behavior with action beginning from 0.8 KW/cm 2 , and seems to be promising optical limiting candidates for future optoelectronic applications. Through B3LYP/6-311G++d,p level of theory Density Functional Theory (DFT), Global Reactivity, Natural Bond Orbital (NBO), and Natural Population were calculated and investigated. Delocalization and hyperconjugation interactions, intramolecular charge transfers, and stabilization energies were discovered using NBO and NPA. The comprehensive studies of Hirshfeld surface (HS) and fingerprint plots (FP) calculations were done in order to evaluate the nature of intermolecular interactions in the compounds. The inclusion of a strong donor and the π-conjugated system improved charge transfer, chemical stability, and optoelectronic properties of the anthracene-heterocyclic chalcone derivatives. As a result, the present work realizes the potential of designed derivatives that can be used in NLO applications.

Nonlinear Optical Behavior Due to Charge Transfer within Selected Heterocyclic Anthracenyl Chalcones under Continuous Wave Laser Excitation