量子性质流形自动采样的元自洽学：分子双自由基景观的探索
Metadynamics for Automatic Sampling of Quantum Property Manifolds: Exploration of Molecular Biradicality Landscapes
摘要：
我们提出了一个一般的扩展的元adaptics允许自动采样的量子性质流形（ASQPM）引起的功能景观，类似于在玻恩-奥本海默近似的框架中的势能面。为此，我们采用广义电子集体变量进行偏置的分子动力学模拟的量子化学方法，探索所需的属性流形的框架。我们说明了我们的方法的“biradicity景观”的例子，我们通过引入自然轨道占用数（NOONs）作为电子集体变量驱动的动态探索。我们证明了该方法的适用性上的模拟\textit{p} -二甲苯和[8]轮烯允许自动提取的双自由基的几何形状。在[8]轮烯的情况下，ASQPM代谢导致预测可以通过合适的化学取代来稳定的双自由基支架，导致设计表现出双自由基功能的新型功能分子。
英文摘要：
We present a general extension of the metadynamics allowing for an automatic sampling of quantum property manifolds (ASQPM) giving rise to functional landscapes that are analogous to the potential energy surfaces in the frame of the Born-Oppenheimer approximation. For this purpose, we employ generalized electronic collective variables to carry out biased molecular dynamics simulations in the framework of quantum chemical methods that explore the desired property manifold. We illustrate our method on the example of the "biradicality landscapes", which we explore by introducing the natural orbital occupation numbers (NOONs) as the electronic collective variable driving the dynamics. We demonstrate the applicability of the method on the simulation of \textit{p}-xylylene and [8]annulene allowing to automatically extract the biradical geometries. In the case of [8]annulene the ASQPM metadynamics leads to the prediction of biradical scaffolds that can be stabilized by a suitable chemical substitution, leading to the design of novel functional molecules exhibiting biradical functionality.
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