A fundamental understanding of the inherent electronic and magnetic properties of open-shell diradicaloids is essential so that these properties can be modified to create molecules that meet the potential needs of industry. However, there have been very few attempts to date to systematically accomplish this in diradicaloid compounds. Here, we present the synthetic, spectroscopic, and computational investigation of a series of molecules based on the diindeno[1,2-b:1′,2′-g]anthracene framework. Calculations suggest that by altering the transfer integral term, t_ab, we are able to manipulate the diradical character and, thus, ΔE_ST within this series of molecules. Experimentally determined values by superconducting quantum interference device (SQUID) magnetometry show that we can effectively “tune” ΔE_ST of the five derivatives within a narrow 1.6 kcal mol⁻¹ range.

对开壳双自由基的内在电子和磁性质有基本的了解是必不可少的，因此可以修改这些性质以创建满足工业潜在需求的分子。然而，迄今为止，很少有人尝试在双基类化合物中系统地完成这一任务。在这里，我们介绍了基于二茚并[1,2- b：1'，2'- g ]蒽骨架的一系列分子的合成，光谱学和计算研究。计算表明，通过更改传递积分项t _ab，我们能够操纵双自由基特征，从而操纵ΔE _ST在这一系列分子中。通过超导量子干涉仪（SQUID）磁力测定法得出的实验值表明，我们可以在1.6 kcal mol ^-1狭窄范围内有效地“调谐”这五个衍生物的ΔE _ST。