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Since the mid‐1980s, there has been a growth of interest in the search and development of molecular second‐order nonlinear optical (NLO) materials that possess various device applications. Beside the most traditional donor‐acceptor (“push‐pull”) organic chromophores (e.g. the stilbene family), chemists have increasingly extended their field of investigations to newer generations of organic molecules of greater complexity. In recent years, coordination complexes through their unique characteristics such as various redox and magnetic properties, in addition to their great diversity of geometries, have introduced a new dimension to the area. This review attempts to summarize the NLO capabilities of bis(salicylaldiminato)metal Schiff base complexes: (i) chromophores with enhanced hyperpolarizabilities (β) can be obtained by virtue of the coordinated metal center; (ii) the use of chiral substituents allows the engineering of the chromophores into various non‐centrosymmetric environments and efficiencies of about 10 times that of urea in second‐harmonic generation; (iii) the general trend observed for the high temperature stability in this family of chromophores, while combined with the large β×μ products, makes these systems interesting candidates for their incorporation into poled polymers with high glass transition temperatures (Tg); (iv) the possibility for β modulation induced by magnetic transition is also seen with respect to the concept of molecular switching.
Since the mid‐1980s, there has been a growth of interest in the search and development of molecular second‐order nonlinear optical (NLO) materials that possess various device applications. Beside the most traditional donor‐acceptor (“push‐pull”) organic chromophores (e.g. the stilbene family), chemists have increasingly extended their field of investigations to newer generations of organic molecules of greater complexity. In recent years, coordination complexes through their unique characteristics such as various redox and magnetic properties, in addition to their great diversity of geometries, have introduced a new dimension to the area. This review attempts to summarize the NLO capabilities of bis(salicylaldiminato)metal Schiff base complexes: (i) chromophores with enhanced hyperpolarizabilities (β) can be obtained by virtue of the coordinated metal center; (ii) the use of chiral substituents allows the engineering of the chromophores into various non‐centrosymmetric environments and efficiencies of about 10 times that of urea in second‐harmonic generation; (iii) the general trend observed for the high temperature stability in this family of chromophores, while combined with the large β×μ products, makes these systems interesting candidates for their incorporation into poled polymers with high glass transition temperatures (Tg); (iv) the possibility for β modulation induced by magnetic transition is also seen with respect to the concept of molecular switching.
The combination of electrical and nonlinear optical (NLO) properties in one material is described for the tetracyanoquinodimethane (TCNQ) radical ion paired with N‐methylstilbazolium‐based chromophores. One of the resulting hybrid materials has a conductivity of 2.3 × 10−3 Ω−1 cm−1 and a second‐harmonic generation efficiency 45 times that of urea. During the predicted transition from electronics to photonics, optoelectronics, which requires multiproperty materials such as those described here, will play an important role.
A remarkable feature of the spin-crossover process in several dinuclear iron(II) compounds is a plateau in the two-step transition curve. Up to now, it has not been possible to analyse the spin state of dinuclear pairs that constitute such a plateau, due to the relative high temperatures at which the transition takes place in complexes investigated so far. We solved this problem by experimentally studying a novel dinuclear spin-crossover compound [[Fe(phdia)(NCS)(2)](2)(phdia)] (phdia: 4,7-phenanthroline-5,6-diamine). We report here on the synthesis and characterisation of this system, which exhibits a two-step spin transition at T(c1)=108 K and T(c2)=80 K, displaying 2 K and 7 K wide thermal hysteresis loops in the upper and the lower steps, respectively. A plateau of approximately 20 K width centred at about 90 K, which corresponds to the 50 % of the spin conversion, separates the two transitions. The composition of the plateau was identified in metastable state after quenching to 4.2 K by means of Mössbauer spectroscopy in an external magnetic field. Such experiments revealed that the plateau consists mainly of [HS-LS] pairs (HS=high spin, LS=low spin) and confirmed the hypothesis that the spin conversion in dinuclear entities proceeds through [LS-LS]<-->[HS-LS]<-->[HS-HS] pairs. The results are discussed in terms of a thermodynamic model based on the regular solution theory adapted for dinuclear spin-crossover compounds.
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