AI 中文总结
该研究通过数据挖掘结合DFT计算与非线性模型，预测有机晶体的太赫兹产生能力，筛选出性能优于现有材料的候选晶体，提出应采用综合方法评估单晶非线性光学性质。
AI 中文摘要
我们报告了利用DFT计算和数学模型，基于有机材料的晶体结构预测其非线性极化（P^{NL}）和非线性极化率系数（χ^{(2)}_{IJK}）的方法。我们将该计算方法应用于通过挖掘剑桥结构数据库得到的单组分晶体、共晶体和离子晶体。我们用已知太赫兹（THz）产生器的实验太赫兹产生效率验证这些计算结果，证明测量值与计算值一致。若干挖掘得到的结构显示出与最先进的THz产生晶体DAST、OH1和BNA相当或更大的P^{NL}值，表明其在非线性光学（NLO）应用中具有巨大潜力。重要的是，我们还将所得的非线性光学张量分量模型与常用的非线性简化模型进行了比较，表明该综合方法应成为评估单晶材料非线性光学性质的标准方法。
英文摘要
We report the use of DFT computation and mathematical models to predict the nonlinear dielectric polarization (P^{NL}) and nonlinear susceptibility coefficients (χ^{(2)}_{IJK}) of organic materials based on their crystal structures. We apply this computation approach on single-component crystals, co-crystals and ionic crystals found through data mining the Cambridge Structural Database. We verify these computational results with experimental terahertz (THz) generation efficiencies for known THz generators, demonstrating consistency between the measurements and the computed values. Several mined structures show similar or larger PNL values compared to state-of-the-art THz generation crystals DAST, OH1 and BNA, suggesting great potential for their use in nonlinear optical (NLO) applications. Importantly, we also compared the resulting model of nonlinear optical tensor components with commonly-used simplifications of nonlinearity, showing that the comprehensive approach should be the standard method to evaluate the nonlinear optical properties of single-crystalline materials.
Comments14 pages, 4 figures
