Two-Photon Absorption Activity of BOPHY Derivatives: Insights from Theory

• Published in: The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory Molecules, spectroscopy, kinetics, environment, & general theory, 2021-04, Vol.125 (12), p.2581-2587
• Main Authors: Petrusevich, Elizaveta F, Ośmiałowski, Borys, Zaleśny, Robert, Alam, Md. Mehboob
• Format: Article
• Language: English
• Subjects: A: Structure, Spectroscopy, and Reactivity of Molecules and Clusters
• ISSN: 1089-5639; 1520-5215
• DOI: 10.1021/acs.jpca.1c00756

We present a theoretical study of a two-photon absorption (2PA) process in dipolar and quadrupolar systems containing two BF2 units. For this purpose, we considered 13 systems studied by Ponce-Vargas et al. [ J. Phys. Chem. B 2017, 121, 10850−10858 ] and performed linear and quadratic response theory calculations based on the RI-CC2 method to obtain the 2PA parameters. Furthermore, using the recently developed generalized few-state model, we provided an in-depth view of the changes in 2PA properties in the molecules considered. Our results clearly indicate that suitable electron-donating group substitution to the core BF2 units results in a large red-shift of the two-photon absorption wavelength, thereby entering into the desired biological window. Furthermore, the corresponding 2PA strength also increases significantly (up to 30-fold). This makes the substituted systems a potential candidate for biological imaging.