First theoretical framework of di-substituted donor moieties of triphenylamine and carbazole for NLO properties: quantum paradigms of interactive molecular computation

The dependence of polarisability (α) and hyperpolarisability (β) on donor strength has been systematically studied by employing density functional theory method on triphenylamine (TPA) and carbazole (CZ) based compounds. The electronic structures, absorption spectra and non-linear optical (NLO) response were calculated by using quantum chemical methods. All the calculations were performed in gas phase in presence of solvent. The results reveal that the polarizability (α) and hyperpolarizability (β) significantly increased by the addition of second donor moiety. Similarly, the oscillator strength and light harvesting efficiency were also increased, while absorption wavelength was red-shifted by the addition of second donor moiety. These results indicate that the di-substituted donor is an effective way to improve NLO response. The TPA dyes possess a large second-order non-linear response and this is primarily because of the strong donor-π-acceptor conjugation that is ascribed to the excited state intramolecular charge transfer. These theoretical frameworks of carbon architecture might be advantageous to design other organic charge-transfer compounds.