论文标题
纠缠电子驱动钴喹啉二聚体复合物中的非superexchange机制
Entangled Electrons Drive a non-Superexchange Mechanism in a Cobalt Quinoid Dimer Complex
论文作者
论文摘要
化学的一个中心主题是对驱动化学转化的机制的理解。有机金属化学中众所周知的高度引用的机制是甲壳度的机制，其中两个或多个金属中心上的未配对电子通过桥接配体的电子对相互作用。我们结合了新型的合成和计算，以表明这种相互作用实际上可能是通过基于两个金属中心的直接量子纠缠的超级缩减而发生的。具体而言，我们合成并实验表征了一种新型的钴二聚体复合物与苯甲喹啉桥桥配体，并使用大型活性空间使用变异的两电子降低密度矩阵方法研究其电子结构。结果吸引了无机机制与量子纠缠之间的新连接，从而为设计强烈相关的有机金属化合物开辟了新的可能性，这些化合物的磁性和自旋特性在超导体，储能，热电学，热电学和旋转方面都有应用。
A central theme in chemistry is the understanding of the mechanisms that drive chemical transformations. A well-known, highly cited mechanism in organometallic chemistry is the superexchange mechanism in which unpaired electrons on two or more metal centers interact through an electron pair of the bridging ligand. We use a combination of novel synthesis and computation to show that such interactions may in fact occur by a more direct mechanism than superexchange that is based on direct quantum entanglement of the two metal centers. Specifically, we synthesize and experimentally characterize a novel cobalt dimer complex with benzoquinoid bridging ligands and investigate its electronic structure with the variational two-electron reduced density matrix method using large active spaces. The result draws novel connections between inorganic mechanisms and quantum entanglement, thereby opening new possibilities for the design of strongly correlated organometallic compounds whose magnetic and spin properties have applications in superconductors, energy storage, thermoelectrics, and spintronics.
