Organometallic compounds are receiving attention as potential second-order and third-order nonlinear optical (NLO) materials.[' -71 Experimental and theoretical studies on hyperpolarizabilities indicate that molecules with large transition dipole moments and small energy gaps are, in general, likely candidates for NLO materials.[*] Thus, as part of our on going program to develop new chromophores, we sought to design organometallic compounds with these properties. Many organometallic complexes exhibit metal to ligand charge transfer (MLCT) bands. However, these bands often exhibit only moderate extinction coefficients in the range of 1000 -20000 M -cm-' which may be limited by relatively weak coupling between the metal and the ligand."' We believe organometallic compounds could be useful in nonlinear optics[*] if the electronic coupling between the transition metal and the organic fragment can be optimized, thereby resulting in stronger optical transitions.
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