Expanding the range of computational quantum chemistry: actinide molecular science and solid-state chemistry

我的研究计划福尔斯属于计算和量子化学的一般领域。1998年诺贝尔化学奖授予W。科恩和已故的J. Pople，这两个领域的杰出先驱。在这个框架内，我的研究的主要长期目标有两个：首先，计算量子化学已经达到了一个地步，它可以被化学家用作解决某些问题的几个标准的“黑箱”方法之一。例如，对于小分子和中等分子的有机化学来说就是这种情况。然而，在其他领域还没有达到同样的成熟程度。因此，我的第一个目标是将计算量子化学方法发展成为有价值和可靠的研究工具，用于尚未充分发挥其潜力的领域。一个这样的领域涉及扩展系统（固体、表面等）的建模，在那里，我的团队将开发广泛的新量子化学方法，用于模拟核磁共振（NMR）和电子自旋共振（ESR）参数。另一个领域包括元素周期表中最重的部分，锕系元素的化学。这些因素对研究人员提出了独特的挑战。在这里，我将建立在一系列现有的本地和国际合作，以开发新的方法（主要是关于相对论效应），并应用和测试在这方面尚未使用的方法。作为第二个主要研究目标，我的目标是发展对锕系元素化学的坚实理解（铀、镎、钚等），以便尽可能避免用放射性材料进行困难和危险的实验。在这一领域，这可以被描述为“理论锕系元素分子科学”，我将专注于模拟分子在水溶液中，以及选择性萃取剂和相关的配合物。这些系统与受污染场地的核废物问题有关（例如，加拿大北部的铀矿尾矿）。

My research program falls into the general area of computational and quantum chemistry. The growing relevance of this field has been recognized with the 1998 Nobel Prize in Chemistry that has been awarded to W. Kohn and the late J. Pople, two outstanding pioneers of the field. Within this framework, the principal, long-term goals of my research are twofold.First, computational quantum chemistry has reached a point where it can be used by chemists as one of several standard, "black-box" approaches for solving certain problems. This is the case for instance for organic chemistry of small and medium-sized molecules. Yet, the same kind of maturity has not been reached in other areas. My first goal, then, is to develop computational quantum chemistry methods into valuable and reliable research tools for areas where they have not yet reached their full potential. One such area concerns modeling of extended systems (solids, surfaces, etc.), where my group will develop extensive new quantum-chemical methods for the simulation of nuclear magnetic resonance (NMR) and electron spin resonance (ESR) parameters. Another area comprises the chemistry of the heaviest parts of the periodic table, the actinide elements. These elements present unique challenges to the researcher. Here, I will build on a range of existing local and international collaborations to develop new methods (chiefly concerning relativistic effects) and to apply and test methods that have not been used in this connection.As the second principal research goal, I aim at developing a solid understanding of the chemistry of the actinide elements (uranium, neptunium, plutonium, among others) from theory and computations alone, so as to avoid difficult and dangerous experiments with radioactive materials as much as possible. In this field, which can be described as "theoretical actinide molecular science", I will focus on modelling molecules in aqueous solution as well as selective extraction agents and related complexes. These are systems that are relevant to the nuclear waste problem at contaminated sites (for instance, uranium mine tailings in Canada's North).