Programa de Pós-Graduação em Química, Universidade Federal do Sul e Sudeste do Pará, 68507-590, Marabá-PA, Brazil.
Universidade Federal do Maranhão, UFMA, Campus Balsas, 6500-000, Maranhão, Brazil.
Chemphyschem. 2023 Jun 15;24(12):e202300060. doi: 10.1002/cphc.202300060. Epub 2023 Apr 20.
The solute polarization due to solvent is a an electrostatic quantum effect that impacts diverse molecular properties, including the nonlinear optical response of a material. An iterative procedure that allows updating the solute charge distribution in the presence of the solvent is combined with a sequential Monte Carlo/Quantum Mechanics methodology and Density Functional Theory methods to evaluate the nonlinear optical (NLO) response using the hyper Rayleigh scattering (HRS) of a series of chromones recently identified in Chamaecrista diphylla, an herbaceous plant abundant throughout the Americas and used in folk medicine. From this study, it is determined that from gas to solvent environment, the systems acquire low refractive index (n) and an improvement of the first hyperpolarizability (β ), signaling potential NLO uses. It is shown that the octupolar contributions (β ) superate the dipolar ones (β ) and dominate the second-order optical response in both gas and liquid phases, which indicate nontrivial optical materials. Moreover, the solvent environment and structural changes in the periphery can tune significantly the dipolar/octupolar balance, showing a key to control the decoupling between these contributions.
溶剂引起的溶质极化是一种静电量子效应，它会影响多种分子性质，包括材料的非线性光学响应。一种迭代程序，允许在溶剂存在的情况下更新溶质电荷分布，与顺序蒙特卡罗/量子力学方法和密度泛函理论方法相结合，用于评估使用一系列在 Chamaecrista diphylla 中最近鉴定的查尔酮的超瑞利散射 (HRS) 的非线性光学 (NLO) 响应，Chamaecrista diphylla 是一种在整个美洲丰富的草本植物，并在民间医学中使用。从这项研究中可以确定，从气相到溶剂环境，这些系统具有低折射率 (n) 和第一超极化率 (β) 的提高，表明具有潜在的 NLO 用途。结果表明，八极贡献 (β) 超过偶极贡献 (β)，并且在气相和液相中主导二阶光学响应，这表明是具有重要意义的光学材料。此外，溶剂环境和外围结构的变化可以显著调节偶极/八极平衡，显示出控制这些贡献解耦的关键。
