“…The variety of chemical substitutions provided by organic chemistry guided by empirical as well as more elaborate theoretical models has allowed for the targeted tailoring of optimized crystals towards quadratic nonlinear optics Zyss & Chemla, 1987). Molecular nonlinear evaluations from the EFISH experiment (Levine & Bethea, 1974;Oudar & Le Person, 1975, 1976Ledoux & Zyss, 1982), related by an oriented gas model, have been very useful for selective development of such crystals. Besides purely crystallographic structural considerations, the spectral adequacy of crystals has also been discussed, in view of applications, in terms of a 'transparencyefficiency' trade-off based on both molecular (Zyss, 1991a) and excitonic considerations (Zyss, Ledoux, Bertault & Toupet, 1991;Pierre, Baldeck, Block, Georges, Trommsdorf & Zyss, 1991).…”