Designing a Propellane‐based Nonlinear Optically Active System Absorbing in Three Different Wavelength Regions

Abstract

The aim of this work is to demonstrate the possibility of using propellane in designing a molecule that can absorb in three different wavelength regions and their nonlinear optical (NLO) activity can be fine-tuned by varying the three wings. We considered 22 tailor-made propellane derivatives consisting of phenyl, naphthyl, and biphenyl wings for this purpose. Using the state-of-the-art linear and quadratic response methods within TD-DFT and RI-CC2 theories and a suitable generalized few-state model that quantifies the effect of orientation of different transition moments on NLO properties, we discussed how and why the linear and nonlinear optical activity of propellane vary when the three wings are assembled successively to construct a full-propellane.

Why does the orientation of azulene affect the two-photon activity of a porphyrinoid–azulene system?

“…The OPA 64–66 profiles of the first five excited singlet states of azulene, five PP systems, and the 18 porphyrinoid–azulene systems calculated at the RICC2/cc-pVDZ level of theory are presented in Fig. 2–7.…”