Pushing the frontiers of modeling excited electronic states and dynamics to accelerate materials engineering and design
Pushing the frontiers of modeling excited electronic states and dynamics to accelerate materials engineering and design
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DOI：
10.1016/j.commatsci.2019.01.004
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发表时间：
2019-04
影响因子：
3.3
通讯作者：
Kisung Kang;A. Kononov;Cheng-Wei Lee;J. Leveillee;Ethan P. Shapera;Xiao Zhang;A. Schleife
中科院分区：
文献类型：
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作者：
Kisung Kang;A. Kononov;Cheng-Wei Lee;J. Leveillee;Ethan P. Shapera;Xiao Zhang;A. Schleife
电子激发及其动力学通常是我们如何使用和探测材料的基础。虽然最近的实验进展使我们能够以前所未有的精度和时间分辨率这样做，但它们的解释依赖于坚实的理论理解。这可以通过基于多体微扰理论（MBPT）和含时密度泛函理论（TDDFT）的尖端的第一原理理论光谱学来提供。在这项工作中，我们回顾了我们最近的一些结果，作为电子结构方法如何导致有趣的洞察电子激发和深入理解现代材料的成功例子。在许多情况下，这些技术是准确的，甚至是预测性的，但它们依赖于近似计算是可行的。我们说明了需要进一步的理论理解，使用介质屏蔽作为MBPT和更快，更准确的数值积分器作为实时TDDFT的挑战的一个例子。最后，我们描述了如何将在线数据库纳入计算材料的研究激发电子态可以侧步骤的高计算成本的问题，以促进材料设计。
Electronic excitations and their dynamics are oftentimes at the foundation of how we use and probe materials. While recent experimental advances allow us to do so with unprecedented accuracy and time resolution, their interpretation relies on solid theoretical understanding. This can be provided by cutting-edge, first-principles theoretical-spectroscopy based on many-body perturbation theory (MBPT) and time-dependent density functional theory (TDDFT). In this work we review some of our recent results as successful examples for how electronic-structure methods lead to interesting insight into electronic excitations and deep understanding of modern materials. In many cases these techniques are accurate and even predictive, yet they rely on approximations to be computationally feasible. We illustrate the need for further theoretical understanding, using dielectric screening as an example in MBPT and faster, more accurate numerical integrators as a challenge for real-time TDDFT. Finally, we describe how incorporating online databases into computational materials research on excited electronic states can side-step the problem of high computational cost to facilitate materials design.