Solution-phase synthesis of Clar’s goblet and elucidation of its spin properties

IF 19.2 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nature chemistry Pub Date : 2025-03-17 DOI:10.1038/s41557-025-01776-1

Tianyu Jiao, Cong-Hui Wu, Yu-Shuang Zhang, Xiaohe Miao, Shaofei Wu, Shang-Da Jiang, Jishan Wu

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Abstract

In the traditional view, spin pairing occurs between two electrons in a chemical bond where the bonding interaction compensates for the penalty of electrostatic repulsion. It is a mystery whether spin pairing can occur between two non-bonded electrons within a molecular entity. Unveiling this type of spin entanglement (that is, pairing between two spatially segregated spins) at the molecular scale is a long-standing challenge. Clar’s goblet, proposed by Erich Clar in 1972, provides an ideal platform to verify this unusual property. Here we report the solution-phase synthesis of Clar’s goblet and experimental elucidation of its spin properties. Magnetic studies reveal that the two spins are spatially segregated with an average distance of 8.7 Å and antiferromagnetically coupled in the ground state with an ΔE_S–T of −0.29 kcal mol⁻¹. Our results provide insight into the spin entanglement in Clar’s goblet and may inspire the design of correlated molecular spins for quantum information technologies.

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克拉氏杯的固相合成及其自旋性质的研究

传统观点认为，自旋配对发生在化学键中的两个电子之间，化学键的相互作用弥补了静电排斥的惩罚。自旋配对是否会发生在分子实体中两个非键合电子之间，这是一个谜。在分子尺度上揭示这种类型的自旋纠缠（即两个空间隔离的自旋之间的配对）是一个长期存在的挑战。Erich Clar 于 1972 年提出的 Clar's goblet 为验证这种不寻常的特性提供了一个理想的平台。在此，我们报告了克拉尔高脚杯的溶液相合成及其自旋特性的实验阐释。磁学研究表明，两个自旋在空间上是分离的，平均距离为 8.7 Å，在基态下是反铁磁耦合的，ΔES-T 为 -0.29 kcal mol-1。我们的研究结果使人们对克拉尔高脚杯中的自旋纠缠有了更深入的了解，并可能对量子信息技术中相关分子自旋的设计有所启发。

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来源期刊

Nature chemistry 化学-化学综合

CiteScore

29.60

自引率

1.40%

发文量

226

审稿时长

1.7 months

期刊介绍： Nature Chemistry is a monthly journal that publishes groundbreaking and significant research in all areas of chemistry. It covers traditional subjects such as analytical, inorganic, organic, and physical chemistry, as well as a wide range of other topics including catalysis, computational and theoretical chemistry, and environmental chemistry. The journal also features interdisciplinary research at the interface of chemistry with biology, materials science, nanotechnology, and physics. Manuscripts detailing such multidisciplinary work are encouraged, as long as the central theme pertains to chemistry. Aside from primary research, Nature Chemistry publishes review articles, news and views, research highlights from other journals, commentaries, book reviews, correspondence, and analysis of the broader chemical landscape. It also addresses crucial issues related to education, funding, policy, intellectual property, and the societal impact of chemistry. Nature Chemistry is dedicated to ensuring the highest standards of original research through a fair and rigorous review process. It offers authors maximum visibility for their papers, access to a broad readership, exceptional copy editing and production standards, rapid publication, and independence from academic societies and other vested interests. Overall, Nature Chemistry aims to be the authoritative voice of the global chemical community.