Bekri Lahcène, Elhorri Abdelkader M, Hedidi Madani, Zouaoui-Rabah Mourad
Department of Chemistry, Faculty of Exact Sciences, Mustapha Stambouli, University of Mascara, Av. Cheikh El Khaldi, 29000, Mascara, Algeria.
Department of Chemistry, Faculty of Exact Sciences and Informatics, Hassiba BenBouali University, Chlef, Ouled Fares, P.O. Box 78C, 02180, Chlef, Algeria.
J Mol Model. 2023 Dec 13;30(1):8. doi: 10.1007/s00894-023-05801-3.
This work focuses on the study of six molecules composed of the TetraAmineLithium (TALi) and TetraAmineSodium (TANa) structures linked with the anions H, Li and Na. The NLO results obtained by these calculations showed significant values of static first hyperpolarizabilities (β) ranging from 8.74 * 10 to 691.99 * 10 esu. The two molecules TALi-Li and TALi-Na gave the highest values of static β equal to 563.20 and 691.99 * 10 esu respectively and static second hyperpolarizabilities (γ) of 680.02 and 779.05 * 10 esu. The highest dynamic first hyperpolarizabilities (β) values are around 1474080.00 * 10 esu and 6,145,080.00 * 10 esu at 720 nm lasers and which are attributed to the two molecules TANa-Li and TANa-Na respectively. Four molecules have push-pull behavior where the anions are donor groups, the Li-NH and Na-NH groups are acceptor groups and a bridge composed by the three remaining NH ligands. The maximum wavelengths (λ) in vacuum and in the presence of solvents for all molecules are in the range 240 to 870 nm.
The software used in this study is Gaussian 16. The optimizations of the molecules were calculated by B3LYP-D3/6-31 + + G(d,p). The static first hyperpolarizability (β) was calculated by different functionals: CAM-B3LYP, LC-wPBE, LC-BLYP, M11, wB97X, HSEh1PBE and M06-2X and the MP2 method, the basis-set used is 6-31 + + G(d,p). Other calculations of static β were carried out by the CAM-B3LYP functional combined with several basis-sets: 6-31G(d,p), 6-31 + + G(d,p), cc-pVDZ, AUG-cc- pVDZ, 6-311G(d,p), 6-311 + + G(d,p), cc-pVTZ and AUG-cc-pVTZ. The calculations of the first (β) and second (γ) hyperpolarizabilities in second harmonic generation (SHG) were calculated by CAM-B3LYP/6-31 + + G(d,p). The delocalization energies (E(2)) were determined by the NBO approach and calculated by the same functional and basis-set cited before. The solvation Gibbs energies (ΔG) were calculated using the implicit SMD model. Maximum wavelengths (λ) and oscillator strengths ([Formula: see text]) were calculated by TD-CAM-B3LYP/6-31 + + G(d,p) in the presence of the implicit CPCM model.
本研究聚焦于由四胺锂（TALi）和四胺钠（TANa）结构与阴离子H、Li和Na相连组成的六种分子。这些计算得到的非线性光学（NLO）结果显示，静态第一超极化率（β）的值显著，范围为8.74×10至691.99×10 esu。两种分子TALi-Li和TALi-Na的静态β值最高，分别等于563.20和691.99×10 esu，静态第二超极化率（γ）分别为680.02和779.05×10 esu。在720纳米激光下，最高动态第一超极化率（β）值分别约为1474080.00×10 esu和6145080.00×10 esu，分别归因于两种分子TANa-Li和TANa-Na。四个分子具有推拉行为，其中阴离子是供体基团，Li-NH和Na-NH基团是受体基团，由其余三个NH配体组成桥。所有分子在真空和有溶剂存在时的最大波长（λ）范围为240至870纳米。
本研究使用的软件是Gaussian 16。分子的优化通过B3LYP-D3/6-31++G(d,p)进行计算。静态第一超极化率（β）通过不同泛函计算：CAM-B3LYP、LC-wPBE、LC-BLYP、M11、wB97X、HSEh1PBE和M06-2X以及MP2方法，使用的基组是6-31++G(d,p)。静态β的其他计算通过CAM-B3LYP泛函与几种基组结合进行：6-31G(d,p)、6-31++G(d,p)、cc-pVDZ、AUG-cc-pVDZ、6-311G(d,p)、6-311++G(d,p)、cc-pVTZ和AUG-cc-pVTZ。二次谐波产生（SHG）中第一（β）和第二（γ）超极化率的计算通过CAM-B3LYP/6-31++G(d,p)进行。离域能（E(2)）通过NBO方法确定，并使用之前引用的相同泛函和基组进行计算。溶剂化吉布斯自由能（ΔG）使用隐式SMD模型计算。最大波长（λ）和振子强度（[公式：见原文]）在隐式CPCM模型存在下通过TD-CAM-B3LYP/6-31++G(d,p)计算。
