Chen Ruisi, Guo Xintao, Zhang Bo, Liu Ying, Liu Jun
AVIC Manufacturing Technology Institute, Beijing 100024, China.
State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China.
Materials (Basel). 2024 Dec 20;17(24):6240. doi: 10.3390/ma17246240.
By combining molecular dynamics (MD) simulations and density functional theory (DFT), the influence of dye structure on the optical modulation properties of negative-mode guest-host liquid crystal (GHLC) systems was systematically investigated. Firstly, the reliability of the simulation method was validated by comparing the performance parameters of the GHLC system obtained from simulations with those from experimental results. Subsequently, a series of guest dye molecules, along with their mixtures with negative dielectric anisotropy mesogens, were designed and analyzed. This exploration focused on how variations in dye terminal chain lengths, substitution positions, and substituent group properties affect dye molecular geometry, dye alignment within the host, transition dipole orientation, absorption spectra, and electronic excitation properties. Our findings suggest that dye molecules with a flexible terminal chain substitution of five carbon atoms, positioned at the 2 and 6 locations on the anthraquinone core, exhibit higher order parameters, favorable for enhancing dichroic performance. Moreover, introducing different α-substituents further influences the dye orientation and electronic behavior within the host. These results highlight that structural modifications of anthraquinone-based dyes allow for the design of high-dichroic-ratio materials with customized absorption properties. Overall, our results provide a beneficial understanding of the structure-property relation in GHLC systems, offering valuable guidance for designing high-performance dye molecules and advanced optoelectronic materials in future research.
通过结合分子动力学(MD)模拟和密度泛函理论(DFT),系统地研究了染料结构对负模式客体-主体液晶(GHLC)系统光学调制特性的影响。首先,通过将模拟得到的GHLC系统性能参数与实验结果进行比较,验证了模拟方法的可靠性。随后,设计并分析了一系列客体染料分子及其与负介电各向异性液晶元的混合物。该探索聚焦于染料末端链长度、取代位置和取代基性质的变化如何影响染料分子几何形状、主体内染料排列、跃迁偶极取向、吸收光谱和电子激发特性。我们的研究结果表明,在蒽醌核心的2和6位置具有五个碳原子的柔性末端链取代的染料分子表现出更高的序参数,有利于增强二向色性性能。此外,引入不同的α-取代基进一步影响主体内染料的取向和电子行为。这些结果突出表明,基于蒽醌的染料的结构修饰允许设计具有定制吸收特性的高双折射比材料。总体而言,我们的结果为GHLC系统中的结构-性能关系提供了有益的理解,为未来研究中设计高性能染料分子和先进光电子材料提供了有价值的指导。