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Degenerate four-wave mixing measurements, using the 35 ps pulses at 532 nm, have been employed to investigate the third-order nonlinear optical parameters of two chromium tricarbonyl complexes η 6-bonded to 3-Amino-9-ethylcarbazole (cas 132-32-1) at either the NH2-substituted aryl ring (1) or the unsubstituted ring (2) and their precursor 3-amino-9-ethylcarbazole (AECz). The second-order hyperpolarizability Y of the compounds 1 and 2 were found to be 42.9×10−31 and 35.9×10−31 esu, respectively, approximately one order of magnitude greater than AECz. The relation between the molecular structure and second-order hyperpolarizability of the compounds 1 and 2 was explored in detail based on the three-level model and the density functional theory (DFT) calculation. The theoretical results indicate that the spatial distribution of electron density has the profound role in the third-order nonlinear optical properties.
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