LAUSR

Abstract In the current work a new third-order nonlinear optical organic single crystal of (2 E )-3-(4-Methylphenyl)-1-(3-nitrophenyl) prop-2-en-1-one ( ML3NC ) has been grown with well-defined morphology using the slow evaporation solution growth technique. X-ray diffraction technique was used to confirm the crystal system. The presence of functional groups in the molecular structure was identified by robust FT-IR and FT-Raman spectra by experimental and theoretical analysis. The ultraviolet-visible-near infrared and photoluminescence studies shows that the grown crystals possess excellent transparency window and green emission band (∼560 nm) confirms their use in green OLEDs. The third-order nonlinear and optical limiting studies have been performed using femtosecond (fs) Z-scan technique. The third-order nonlinear optical susceptibility ( χ (3) ), second-order hyperpolarizability (γ), nonlinear refractive index ( n 2 ) and limiting threshold values are found to be 4.03 × 10 −12  esu, 14.2 × 10 −32  esu, −4.33 × 10 −14  cm 2 /W and 2.41 mJ/cm 2 , respectively. Furthermore, the quantum chemical studies were carried out to achieve the ground state molecular geometry and correlate with experimental results. The experimental value of absorption wavelength (λ abs  = 328 nm) is found to be in excellent accord with the theoretical value (λ abs  = 328 nm) at TD-DFT/B3LYP/6-31G* level of theory. To understand the static and dynamic NLO behavior, the polarizability (α) and second hyperpolarizability (γ) values were determined using TD-HF method. The computed second hyperpolarizability γ(-3ω; ω,ω,ω) at 800 nm wavelength was found to be 0.499 × 10 −32  esu which is in good agreement with experimental value at the same wavelength. These results confirms the applied nature of title molecule in optoelectronic and nonlinear optical devices.