Accurate Energetics Across the Periodic Table

北德克萨斯大学的Angela Wilson获得了理论和计算化学项目的奖励，该项目的研究开发了计算主族和过渡金属物种热力学性质的方法，接近化学精度，即在1千卡/摩尔或更低的范围内。这些方法正在应用于对环境可持续性有影响的问题，并有五个组成部分：（1）正在开发基于相关一致合成方法的多参比合成方法;（2）通过轨道定位和基组截断等方法，将相关一致合成方法扩展到更大的化学体系;（3）正在改进过渡金属物种的当前一代相关一致合成方法;（4）正在开发适用于更多样化化学环境的混合QM/QM和QM/MM技术;（5）通过过渡金属（例如，Ni，Pd，Pt）催化剂的研究。计算化学长期面临的挑战之一是实现化学精确的能量学，这项工作正在产生影响。 复合模型方法已经被开发出来，可以考虑更大的分子，威尔逊和她的团队通过开发相关性一致的复合方法或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众所周知的困难元素。 这项工作通过其在对环境原因很重要的系统中的应用以及通过参与UNT工作的大量学生产生了广泛的影响。

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.