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Unraveling the structure–property relationship of novel thiophene and furan‐fused cyclopentadienyl chromophores for nonlinear optical applications
Journal of Computational Chemistry ( IF 3.4 ) Pub Date : 2024-07-23 , DOI: 10.1002/jcc.27467 Hejing Sun 1
Journal of Computational Chemistry ( IF 3.4 ) Pub Date : 2024-07-23 , DOI: 10.1002/jcc.27467 Hejing Sun 1
Affiliation
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Development of organic nonlinear optical materials has become progressively more important due to their emerging applications in new‐generation photonic devices. A novel series of chromophores based on innovative thiophene and furan‐fused cyclopentadienyl bridge with various powerful donor and acceptor moieties were designed and theoretically investigated for applications in nonlinear optics. To unravel the structure–property relationship between this new push‐pull conjugated systems and their nonlinear optical property, multiple methods, including density of states analysis, coupled perturbed Kohn–Sham (CPKS) method, sum‐over‐states (SOS) model, the two‐level model (TSM), hyperpolarizability density analysis, and the (hyper)polarizability contribution decomposition, were performed to comprehensively investigated the nonlinear optical and electronic properties of this new π‐system. Due to excellent charge transfer ability of new bridge and distinctive structure of donor and acceptor, the designed chromophores exhibit deep HOMO levels, low excitation energy, high dipole moment difference and large hyperpolarizability, indicating the appealing air‐stable property and remarkable electrooptic performance of them. Importantly, THQ‐CS‐A3 and PA‐CS‐A3 shows outstanding NLO response properties with β tot value of 6953.9 × 10−30 and 5066.0 × 10−30 esu in AN, respectively. The influence of the push‐pull strength, the heterocycle and the π‐conjugation of new bridge on the nonlinear optical properties of this novel powerful systems are clarified. This new series of chromophores exhibit remarkable electro‐optical Pockels and optical rectification effect. More interestingly, PA‐CS‐A3 and THQ‐CS‐A2 also show appealing SHG effect. This study will help people understand the nature of nonlinear optical properties of innovative heteroarene‐fused based cyclopentadienyl chromophores and offer guidance for the rational design of chromophores with outstanding electrooptic (EO) performance in the future.
中文翻译：
揭示用于非线性光学应用的新型噻吩和呋喃稠合环戊二烯基发色团的结构-性能关系
由于有机非线性光学材料在新一代光子器件中的新兴应用，其开发变得越来越重要。设计了一系列基于创新噻吩和呋喃稠合环戊二烯基桥的新型发色团，具有各种强大的供体和受体部分，并在理论上研究了其在非线性光学中的应用。为了揭示这种新型推挽共轭体系及其非线性光学性质之间的结构-性能关系，采用了多种方法，包括状态密度分析、耦合扰动 Kohn-Sham (CPKS) 方法、态求和 (SOS) 模型、进行了二能级模型（TSM）、超极化密度分析和（超）极化贡献分解，以全面研究这种新π系统的非线性光学和电子特性。由于新桥优异的电荷转移能力和独特的供体和受体结构，所设计的发色团表现出深HOMO能级、低激发能、高偶极矩差和大超极化率，表现出吸引人的空气稳定性和卓越的电光性能。重要的是，THQ-CS-A3 和 PA-CS-A3 显示出出色的 NLO 响应特性β总计值为 6953.9 × 10 −30和5066.0×10 −30分别在 AN 中的 esu。阐明了新桥的推拉强度、杂环和π共轭对这种新型强大系统的非线性光学性质的影响。这一系列新的发色团表现出显着的电光普克尔效应和光学整流效应。 更有趣的是，PA-CS-A3 和 THQ-CS-A2 也表现出吸引人的倍频效应。这项研究将帮助人们了解创新的杂芳烃稠合环戊二烯基发色团的非线性光学性质的本质，并为未来合理设计具有优异电光（EO）性能的发色团提供指导。
更新日期：2024-07-23
中文翻译：
揭示用于非线性光学应用的新型噻吩和呋喃稠合环戊二烯基发色团的结构-性能关系
由于有机非线性光学材料在新一代光子器件中的新兴应用，其开发变得越来越重要。设计了一系列基于创新噻吩和呋喃稠合环戊二烯基桥的新型发色团，具有各种强大的供体和受体部分，并在理论上研究了其在非线性光学中的应用。为了揭示这种新型推挽共轭体系及其非线性光学性质之间的结构-性能关系，采用了多种方法，包括状态密度分析、耦合扰动 Kohn-Sham (CPKS) 方法、态求和 (SOS) 模型、进行了二能级模型（TSM）、超极化密度分析和（超）极化贡献分解，以全面研究这种新π系统的非线性光学和电子特性。由于新桥优异的电荷转移能力和独特的供体和受体结构，所设计的发色团表现出深HOMO能级、低激发能、高偶极矩差和大超极化率，表现出吸引人的空气稳定性和卓越的电光性能。重要的是，THQ-CS-A3 和 PA-CS-A3 显示出出色的 NLO 响应特性β总计值为 6953.9 × 10 −30和5066.0×10 −30分别在 AN 中的 esu。阐明了新桥的推拉强度、杂环和π共轭对这种新型强大系统的非线性光学性质的影响。这一系列新的发色团表现出显着的电光普克尔效应和光学整流效应。 更有趣的是，PA-CS-A3 和 THQ-CS-A2 也表现出吸引人的倍频效应。这项研究将帮助人们了解创新的杂芳烃稠合环戊二烯基发色团的非线性光学性质的本质，并为未来合理设计具有优异电光（EO）性能的发色团提供指导。
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