Athmani Hamza, Direm Amani, Osório Francisco A P, Valverde Clodoaldo
Laboratory of Structures, Properties and Interatomic Interactions LASPI2A, Faculty of Sciences and Technology, Abbes Laghrour University, 40.000, Khenchela, Algeria.
Department of Matter Sciences, Faculty of Sciences and Technology, Abbes Laghrour University, 40.000, Khenchela, Algeria.
J Mol Model. 2024 Jul 24;30(8):280. doi: 10.1007/s00894-024-06077-x.
In this study, we detail the synthesis and crystallographic characterization of an unprecedented structure, specifically hypoxanthinium chloride monohydrate ((I) hereafter), which crystallizes in the monoclinic P2/c space group. A comparative analysis was conducted with four related hypoxanthinium salts: hypoxanthinium bromide monohydrate (II), 9-methylhypoxanthinium chloride monohydrate (III), hypoxanthinium nitrate monohydrate (IV), and hypoxanthinium perchlorate monohydrate (V). This analysis has focused mainly on their crystal packing, hydrogen-bonding networks, and non-classical intermolecular interactions, as elucidated by comprehensive Hirshfeld surface and topological analyses. Theoretical investigation of the nonlinear optical (NLO) properties of the hypoxanthinium derivatives (I-V) was performed using the Density Functional Theory (DFT).
The crystalline environment was simulated using the iterative Supermolecule method (SM), and the static and dynamics linear refractive index, linear polarizability, second-order hyperpolarizability, and the third-order nonlinear susceptibility at the DFT/CAM-B3LYP/6-311++G(d,p) level were computed. The results for the macroscopic third-order nonlinear susceptibility of (II) was found to equal . By replacing the bromine atom in (II) with a chlorine atom as in (III), the value will be multiplied by 2.16, and therefore these results are large enough to suggest the potential application of these crystals as NLO materials.
在本研究中，我们详细阐述了一种前所未有的结构——一水合次黄嘌呤氯化物（以下简称（I））的合成及晶体学表征，其结晶于单斜P2/c空间群。对四种相关的次黄嘌呤盐进行了对比分析：一水合次黄嘌呤溴化物（II）、一水合9 - 甲基次黄嘌呤氯化物（III）、一水合次黄嘌呤硝酸盐（IV）和一水合次黄嘌呤高氯酸盐（V）。通过全面的 Hirshfeld 表面和拓扑分析阐明，该分析主要聚焦于它们的晶体堆积、氢键网络和非经典分子间相互作用。使用密度泛函理论（DFT）对次黄嘌呤衍生物（I - V）的非线性光学（NLO）性质进行了理论研究。
使用迭代超分子方法（SM）模拟晶体环境，并在DFT/CAM - B3LYP/6 - 311++G(d,p)水平计算静态和动态线性折射率、线性极化率、二阶超极化率以及三阶非线性极化率。发现（II）的宏观三阶非线性极化率结果等于 。如（III）中那样用氯原子取代（II）中的溴原子， 值将乘以2.16，因此这些结果足以表明这些晶体作为 NLO 材料的潜在应用。
