Accurate Energetics Across the Periodic Table

北得克萨斯大学的Angela Wilson获得了理论和计算化学计划颁发的奖项，该计划旨在开发计算主要基团和过渡金属物种热力学性质的方法，以接近化学精度，即在1千卡/摩尔或更少。这些方法正在应用于对环境可持续性有影响的问题，包括五个组成部分：(1)正在开发基于相关协调复合方法(CCCA)的多参考复合方法；(2)CCCA复合方法正在通过轨道定域化和基组截断等方法扩展到更大的化学体系；(3)正在改进针对过渡金属物种的当前一代CCCA；(4)正在开发适用于更多不同化学环境的QM/QM和QM/MM混合技术；(5)通过过渡金属(如Ni、Pd、Pt)催化剂对木素键模型的断裂进行了前四种方法的研究。计算化学中长期存在的挑战之一是获得化学上精确的能量学，这项工作正在对此产生影响。复合模型方法已经开发出来，以允许考虑更大的分子，Wilson和她的团队通过开发关联一致复合方法或CCCA方法做出了贡献，该方法可以应用于过渡金属，这是计算化学领域中出了名的困难的一组元素。这项工作通过将其应用于对环境具有重要意义的系统，以及通过大量学生参与UNT的工作，产生了广泛的影响。

Angela Wilson of the University of North Texas is supported by an award from the Theoretical and Computational Chemistry program for research to develop methods for the calculation of thermodynamic properties of main group and transition metal species to near chemical accuracy, i.e. to within one kcal/mol or less. The approaches are being applied to problems that have implications for environmental sustainability and has five components: (1) A multireference composite method based on the correlation consistent Composite Approach (ccCA) is being developed; (2) The ccCA composite approach is being extended to larger chemical systems via methods such as orbital localization and basis set truncation; (3) The current generation of ccCA for transition metal species is being improved; (4) Hybrid QM/QM and QM/MM techniques that are applicable to more diverse chemical environments are being developed; (5) The scission of lignin linkage models via a transition metal (e.g., Ni, Pd, Pt) catalyst is being investigated using the first four methodological developments.One of the long-standing challenges in computational chemistry is in achieving chemically accurate energetics and this work is having an impact on that. Composite model approaches have been developed to allow the consideration of larger molecules and Wilson and her group have contributed through the development of the correlation consistent Composite Approach, or ccCA method, which can be applied to transition metals, a notoriously difficult group of elements in the computational chemistry field. The work is having a broad impact through its applications in systems that are important for environmental reasons as well as through the large number of students involved in the work at UNT.