The control of luminous radiation has extremely important implications for modern and future technologies as well as in medicine. In this Review, we detail chemical structures and their relevant photophysical features for various groups of materials, including organic dyes such as metalloporphyrins and metallophthalocyanines (and derivatives), other common organic materials, mixed metal complexes and clusters, fullerenes, dendrimeric nanocomposites, polymeric materials (organic and/or inorganic), inorganic semiconductors, and other nanoscopic materials, utilized or potentially useful for the realization of devices able to filter in a smart way an external radiation. The concept of smart is referred to the characteristic of those materials that are capable to filter the radiation in a dynamic way without the need of an ancillary system for the activation of the required transmission change. In particular, this Review gives emphasis to the nonlinear optical properties of photoactive materials for the functi...

Nonlinear Optical Materials for the Smart Filtering of Optical Radiation.

The current status of organic low-molecular weight and polymeric materials for third-order nonlinear optics is reviewed. The importance of organic materials lies in their promise of large nonlinear optical figure of merit, high optical damage thresholds, ultrafast optical responses, architectural flexibility, and ease of fabrication. Organic materials exhibiting interesting third-order nonlinear optical properties are discussed to illustrate the importance of structure–property correlations. Results on emerging organic materials that include liquids, dyes, fullerenes, charge-transfer complexes, π-conjugated polymers, dye-grafted polymers, organometallic compounds, composites, and liquid crystals are presented. Organic nonlinear optical materials seem promising for a wide range of applications and their potential for integrated optics should be further explored.

Organic Materials for Third‐Order Nonlinear Optics

Three novel coordination polymers [Pb(bbbm)2(NO3)2]n (bbbm = 1,1‘-(1,4-butanediyl)bis-1H-benzimidazole) 1, [Zn(bbbt)(NCS)2]n (bbbt = 1,1‘-(1,4-butanediyl)bis-1H-benzotriazole) 2, and [Zn(pbbt)(NCS)2]n (pbbt = 1,1‘-(1,3-propylene)bis-1H-benzotriazole) 3 were synthesized and structurally characterized. Polymer 1 exhibits a two-dimensional rhombohedral grid network structure, the dimensions of the grid are 14.274 × 14.274 A, and the diagonal-to-diagonal distances are 24.809 × 14.125 A. Polymer 2 possesses a concavo-convex chain structure different from those of the known one-dimensional polymers, which are linear chain, zigzag chain, helical chain, double-stranded chain, and ladder chain. Polymer 3 exhibits a one-dimensional zigzag chain structure, and these chains were packed as an ...ABAB... layered structure. The third-order nonlinear optical (NLO) properties of polymers 1, 2, and 3 were determined with a 7-ns pulsed laser at 532 nm. 1 shows strong third-order NLO absorptive and refractive properties, and...

Novel pb and zn coordination polymers: synthesis, molecular structures, and third-order nonlinear optical properties.

Experimental measurements of the frequency dependence of the isotropically averaged, molecular dc-induced second-harmonic susceptibility 〈γ(−2ω; ω, ω, 0)〉 and third-harmonic susceptibility 〈γ(−3ω; ω, ω, ω)〉 of conjugated linear-chain structures are in excellent agreement with the results of many-electron, multiple-excited-configuration-interaction calculations. For hexatriene, the N = 6 carbon site linear polyene chain, we demonstrate the first successful comparison, to our knowledge, between experiment and theory for the magnitude, sign, and dispersion of 〈γ(−2ω; ω, ω, 0)〉 and 〈γ(−3ω; ω, ω, ω)〉. These results provide experimental verification of the importance of electron-correlation effects in the third-order nonlinear-optical properties of conjugated structures. Measurements of 〈γ(−2ω; ω, ω, 0)〉 and 〈γ(−3ω; ω, ω, ω)〉 for β-carotene, the intermediate length, N = 22, conjugated chain, are also reported, and the frequency dependence is well described by a three-level model that is developed based on the results of the electron-correlation description of γijkl(−ω4; ω1, ω2, ω3) for shorter chains. Finally, through the detailed comparisons of 〈γ(−2ω; ω, ω, 0)〉 with 〈γ(−3ω; ω, ω, ω)〉 and of experiment with theory, as well as through examination of previously reported values of the macroscopic third-order susceptibility χ(3)(−ω4; ω1, ω2, ω3) of glasses by other nonlinear-optical techniques, it is demonstrated that the common reference standard for χ(3)(−ω4; ω1, ω2, ω3) of glass is inaccurate, and an improved value is recommended.

Dispersion measurements of electric-field-induced second-harmonic generation and third-harmonic generation in conjugated linear chains

Two-photon absorption of bis[4-(N,N-diphenylamino)phenylethynyl]arenes.

Cubic hyperpolarizability of a family of alkanes and substituted alkanes with a general formula CH3–(CH2)n−2CH2X (6 ≤ n ≤ 16 and X = H, Cl, Br, I) was measured by using third-harmonic generation at 1.064 μm. Using an additivity model and Onsager’s formulas for local-field factors, the cubic hyperpolarizabilities of the and –CH2X groups were determined, and the following values were obtained (in 10−37 esu): γCH2 = 6.6, γCH2X = 5.2 (X = H), 9.3 (X = Cl), 18.3 (X = Br), and 41.4 (X = I). For C–X bonds the corresponding values are γC–H = 2, γC–C = 1.2, γC–C = 7.7, γC–Br = 13.6, and γC–H = 30.6. A comparison of the above values with those found for other organic solvents shows the importance of molecular geometry in the additivity model.

Cubic hyperpolarizabilities and local electric field in alkanes and substituted alkanes

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Cubic hyperpolarizabilities and local electric field in alkanes and substituted alkanes