论文标题
大而有界的：卡宾斯的自旋差距
Large yet bounded: Spin gap ranges in carbenes
论文作者
论文摘要
尽管它与化学相关，但尚未以系统的方式研究整个化学空间的游离碳烯的电子结构。我们探索了一个大型且系统的卡宾化学空间，该空间由以受控精度计算的单线和三重态型八千种不同和常见的卡宾支架组成（高阶的多等级理论水平）以及电子结构中经过验证的卡宾特征。源自具有强电子相关性的，发现单重毛间间隙的硬上限可在该化学空间中所有碳纤维类别的30 kcal/mol出现。我们还观察到许多Carbene类（分别$> $> $> $ 100和$ 60 kcal/mol）中的大型垂直和绝热的自旋差距，并且我们报告了组成，结构和电子自由度之间的新型关系。我们的QMSpin数据库包括$ \ $ \ $ 13'000 MRCI计算的数值结果，对随机选择的卡宾支架进行了计算。
Despite its relevance for chemistry, the electronic structure of free carbenes throughout chemical space has not yet been studied in a systematic manner. We explore a large and systematic carbene chemical space consisting of eight thousand diverse and common carbene scaffolds in their singlet and triplet state computed at controlled accuracy (higher order multireference level of theory) and with verified carbene character in the electronic structure. Originating in strong electron correlation, a hard upper limit for the singlet-triplet gap is found to emerge at around 30 kcal/mol for all the carbene classes in this chemical space. We also observe large vertical and adiabatic spin gap ranges within many carbene classes ($>$100 and $>$60 kcal/mol, respectively), and we report novel relationships between compositional, structural, and electronic degrees of freedom. Our QMspin data base includes numerical results for $\approx$13'000 MRCI calculations on randomly selected carbene scaffolds.
