Sagir Muhammad, Mushtaq Kalsoom, Khalid Muhammad, Khan Mashal, Tahir Muhammad Bilal, Braga Ataualpa A C
Institute of Chemical and Environmental Engineering, Khwaja Fareed University of Engineering & Information Technology Rahim Yar Khan 64200 Pakistan.
Institute of Chemistry, Khwaja Fareed University of Engineering & Information Technology Rahim Yar Khan 64200 Pakistan.
RSC Adv. 2023 Nov 1;13(45):31855-31872. doi: 10.1039/d3ra04580c. eCollection 2023 Oct 26.
In the current study, seven non-fullerene compounds abbreviated as ATTD2-ATTD8 were designed through structural tailoring and their nonlinear optical (NLO) properties were reported. The objective of this study was to explore the potential for newly configured D-π-A type non-fullerene-based compounds. Quantum chemical methods were adopted and revealed the molecules as highly efficient materials with favorable NLO characteristics for use in optoelectronic devices. The M06 functional along with the 6-311G(d,p) basis set in chloroform solvent were utilized for the natural bonding orbital (NBO) analysis, absorption spectra and computational assessments of frontier molecular orbitals (FMOs), global reactivity descriptors (GRPs), transition density matrix (TDM) and nonlinear optical properties (NLO) for ATTR1 and ATTD2-ATTD8. The HOMO-LUMO energy gap was significantly reduced in all the designed moieties compared to the reference compound in the following decreasing order: ATTR1 > ATTD8 > ATTD4 > ATTD5 > ATTD2 > ATTD7 > ATTD6 > ATTD3. All of the designed molecules (ATTD2-ATTD8) showed good NLO response. Global reactivity parameters were found to be closely associated with the band gap between the HOMO and LUMO orbitals, and the compound with the smallest energy gap, ATTD3, exhibited a lower hardness value of 1.754 eV and higher softness value of 0.570 eV with outstanding NLO response. For the reference compound and ATTD2-ATTD8 derivatives, attributes like dipole moment (), average polarizability 〈〉, first hyperpolarizability (), and second hyperpolarizability were calculated. Out of all the derivatives, ATTD3 revealed the highest amplitude with a of 8.23 × 10 esu, which was consistent with the reduced band gap (1.754 eV) and suggested it was the best possibility for NLO materials in the future.
在当前研究中，通过结构剪裁设计了七种缩写为ATTD2 - ATTD8的非富勒烯化合物，并报道了它们的非线性光学（NLO）性质。本研究的目的是探索新构型的D - π - A型非富勒烯基化合物的潜力。采用量子化学方法，结果表明这些分子是用于光电器件的具有良好NLO特性的高效材料。在氯仿溶剂中，使用M06泛函以及6 - 311G(d,p)基组对ATTR1和ATTD2 - ATTD8进行自然键轨道（NBO）分析、吸收光谱以及前沿分子轨道（FMO）、全局反应性描述符（GRP）、跃迁密度矩阵（TDM）和非线性光学性质（NLO）的计算评估。与参考化合物相比，所有设计的部分的最高占据分子轨道（HOMO）-最低未占据分子轨道（LUMO）能隙均显著降低，顺序如下：ATTR1 > ATTD8 > ATTD4 > ATTD5 > ATTD2 > ATTD7 > ATTD6 > ATTD3。所有设计的分子（ATTD2 - ATTD8）均表现出良好的NLO响应。发现全局反应性参数与HOMO和LUMO轨道之间的带隙密切相关，能隙最小的化合物ATTD3表现出较低的硬度值1.754 eV和较高的软度值0.570 eV，具有出色的NLO响应。对于参考化合物和ATTD2 - ATTD8衍生物，计算了偶极矩（）、平均极化率〈〉、第一超极化率（）和第二超极化率等属性。在所有衍生物中，ATTD3的振幅最高，为8.23×10 esu，这与降低的带隙（1.754 eV）一致，表明它是未来NLO材料的最佳选择。
