Theoretical Photochemistry and Photophysics Group, Faculty of Chemistry, Wrocław University of Science and Technology, Wyb. Wyspiańskiego 27, Wrocław PL-50370, Poland.
Faculty of Chemistry, Nicolaus Copernicus University, Gagarina 7, Toruń PL-87100, Poland.
J Phys Chem A. 2021 Apr 1;125(12):2581-2587. doi: 10.1021/acs.jpca.1c00756. Epub 2021 Mar 23.
We present a theoretical study of a two-photon absorption (2PA) process in dipolar and quadrupolar systems containing two BF units. For this purpose, we considered 13 systems studied by Ponce-Vargas et al. [ 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 BF 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.
我们对包含两个 BF 单元的偶极子和四极子系统中的双光子吸收（2PA）过程进行了理论研究。为此，我们考虑了 Ponce-Vargas 等人研究的 13 个系统。[2017, 121, 10850-10858]，并基于 RI-CC2 方法进行了线性和二次响应理论计算，以获得 2PA 参数。此外，使用最近开发的广义少体模型，我们深入了解了所考虑分子中 2PA 性质的变化。我们的结果清楚地表明，适当的供电子基团取代 BF 单元的核心会导致双光子吸收波长的大幅红移，从而进入所需的生物窗口。此外，相应的 2PA 强度也显著增加（高达 30 倍）。这使得取代的系统成为生物成像的潜在候选者。
