量子旋转隧穿的涌现复杂性。

IF 12.5 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES
Science Advances Pub Date : 2025-02-07 Epub Date: 2025-02-05 DOI:10.1126/sciadv.ads0503
Yilin Guo, Chen Yang, Xinmiao Xie, Yanwei Li, Kendall N Houk, Xuefeng Guo
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引用次数: 0

摘要

构象异构决定了材料的性能和生物分子的活性。然而,在单分子水平上对构象异构化进行完整的动力学研究仍然是一个巨大的挑战。在这项工作中,我们以单事件分辨率对共价嵌入石墨烯电极中的单个芳香链的全旋转动力学进行实时原位电监测。我们发现苯环在低温下的旋转动力学过程是由量子旋转隧穿主导的,而不是准自由旋转过程。证明了单个芳香分子中不同分子内旋转的新出现的复杂性,包括由非弹性电子隧道驱动的具有多、单和半圆延迟的交替单向旋转,这在以前没有在宏观水平上得到充分考虑。这项工作在宏观和微观世界之间建立了一座桥梁,提高了我们对结构-活性关系的理解,有可能为普通材料带来不同的功能。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Emergent complexity of quantum rotation tunneling.

Conformational isomerism determines the performance of materials and the activity of biomolecules. However, a complete dynamic study of conformational isomerization is still a formidable challenge at the single-molecule level. In this work, we present real-time in situ electrical monitoring of the full rotation dynamics of a single aromatic chain covalently embedded in graphene electrodes with single-event resolution. We reveal that the dynamic process of phenyl ring rotations at low temperature is dominated by quantum rotation tunneling rather than the quasi-free rotation process. The emergent complexity of different intramolecular rotations in a single aromatic molecule is demonstrated, including the alternating unidirectional rotation with multi-, single-, and half-circle delays driven by inelastic electron tunneling, which has not been previously adequately considered at the macroscopic level. This work builds a bridge between macroscopic and microscopic worlds and improves our understanding of structure-activity relationships, potentially bringing different functions to ordinary materials.

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来源期刊
Science Advances
Science Advances 综合性期刊-综合性期刊
CiteScore
21.40
自引率
1.50%
发文量
1937
审稿时长
29 weeks
期刊介绍: Science Advances, an open-access journal by AAAS, publishes impactful research in diverse scientific areas. It aims for fair, fast, and expert peer review, providing freely accessible research to readers. Led by distinguished scientists, the journal supports AAAS's mission by extending Science magazine's capacity to identify and promote significant advances. Evolving digital publishing technologies play a crucial role in advancing AAAS's global mission for science communication and benefitting humankind.
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