{"title":"Emergent complexity of quantum rotation tunneling.","authors":"Yilin Guo, Chen Yang, Xinmiao Xie, Yanwei Li, Kendall N Houk, Xuefeng Guo","doi":"10.1126/sciadv.ads0503","DOIUrl":null,"url":null,"abstract":"<p><p>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.</p>","PeriodicalId":21609,"journal":{"name":"Science Advances","volume":"11 6","pages":"eads0503"},"PeriodicalIF":11.7000,"publicationDate":"2025-02-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11797527/pdf/","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Science Advances","FirstCategoryId":"103","ListUrlMain":"https://doi.org/10.1126/sciadv.ads0503","RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2025/2/5 0:00:00","PubModel":"Epub","JCR":"Q1","JCRName":"MULTIDISCIPLINARY SCIENCES","Score":null,"Total":0}
引用次数: 0
Abstract
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.
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.