Halogen bond-modulated solid-state reordering and symmetry breaking of azahelicenes

Abstract Spontaneous symmetry breaking predominately occurs during the aggregation of discrete molecules in solution. Herein, we report a unique solid-state symmetry breaking process of dynamically chiral aza[4]helicenes that emerged in vacuum-driven transformation of halogen bond-woven crystals. Du...

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Main Authors: Juncong Liang, Fuwei Gan, Guoli Zhang, Chengshuo Shen, Huibin Qiu
Format: Article
Language:English
Published: Nature Portfolio 2025-04-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-59222-2
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author Juncong Liang
Fuwei Gan
Guoli Zhang
Chengshuo Shen
Huibin Qiu
author_facet Juncong Liang
Fuwei Gan
Guoli Zhang
Chengshuo Shen
Huibin Qiu
author_sort Juncong Liang
collection DOAJ
description Abstract Spontaneous symmetry breaking predominately occurs during the aggregation of discrete molecules in solution. Herein, we report a unique solid-state symmetry breaking process of dynamically chiral aza[4]helicenes that emerged in vacuum-driven transformation of halogen bond-woven crystals. Due to the weak feature of the halogen bonding, the halides in the cocrystals can be completely removed under vacuum at an elevated temperature. Interestingly, the aza[4]helicene molecules released from the halogen bond network solely adopt one chiral conformation upon reordering and symmetry breaking instantly occurs in a solid state. The Cotton effects gradually increase with the extension of vacuum–heating treatment, indicating a unidirectional transformation of the chiral conformations and an amplification of symmetry breaking during the solid-state reorganization. Moreover, the use of aza[6]helicene as a chiral inducer further enables a precise manipulation for the absolute configuration of the solid-state symmetry breaking, paving a distinctive route to chiral organic materials from achiral/racemic precursors.
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spelling doaj-art-a3c3ae13fb434702b910143a5baefd3d2025-08-20T02:30:26ZengNature PortfolioNature Communications2041-17232025-04-0116111010.1038/s41467-025-59222-2Halogen bond-modulated solid-state reordering and symmetry breaking of azahelicenesJuncong Liang0Fuwei Gan1Guoli Zhang2Chengshuo Shen3Huibin Qiu4School of Chemistry and Chemical Engineering, State Key Laboratory of Synergistic Chem-Bio Synthesis, Frontiers Science Center for Transformative Molecules, Zhangjiang Institute for Advanced Study, State Key Laboratory of Micro-Nano Engineering Science, Shanghai Jiao Tong UniversitySchool of Chemistry and Chemical Engineering, State Key Laboratory of Synergistic Chem-Bio Synthesis, Frontiers Science Center for Transformative Molecules, Zhangjiang Institute for Advanced Study, State Key Laboratory of Micro-Nano Engineering Science, Shanghai Jiao Tong UniversitySchool of Chemistry and Chemical Engineering, State Key Laboratory of Synergistic Chem-Bio Synthesis, Frontiers Science Center for Transformative Molecules, Zhangjiang Institute for Advanced Study, State Key Laboratory of Micro-Nano Engineering Science, Shanghai Jiao Tong UniversitySchool of Chemistry and Chemical Engineering, Zhejiang Sci-Tech UniversitySchool of Chemistry and Chemical Engineering, State Key Laboratory of Synergistic Chem-Bio Synthesis, Frontiers Science Center for Transformative Molecules, Zhangjiang Institute for Advanced Study, State Key Laboratory of Micro-Nano Engineering Science, Shanghai Jiao Tong UniversityAbstract Spontaneous symmetry breaking predominately occurs during the aggregation of discrete molecules in solution. Herein, we report a unique solid-state symmetry breaking process of dynamically chiral aza[4]helicenes that emerged in vacuum-driven transformation of halogen bond-woven crystals. Due to the weak feature of the halogen bonding, the halides in the cocrystals can be completely removed under vacuum at an elevated temperature. Interestingly, the aza[4]helicene molecules released from the halogen bond network solely adopt one chiral conformation upon reordering and symmetry breaking instantly occurs in a solid state. The Cotton effects gradually increase with the extension of vacuum–heating treatment, indicating a unidirectional transformation of the chiral conformations and an amplification of symmetry breaking during the solid-state reorganization. Moreover, the use of aza[6]helicene as a chiral inducer further enables a precise manipulation for the absolute configuration of the solid-state symmetry breaking, paving a distinctive route to chiral organic materials from achiral/racemic precursors.https://doi.org/10.1038/s41467-025-59222-2
spellingShingle Juncong Liang
Fuwei Gan
Guoli Zhang
Chengshuo Shen
Huibin Qiu
Halogen bond-modulated solid-state reordering and symmetry breaking of azahelicenes
Nature Communications
title Halogen bond-modulated solid-state reordering and symmetry breaking of azahelicenes
title_full Halogen bond-modulated solid-state reordering and symmetry breaking of azahelicenes
title_fullStr Halogen bond-modulated solid-state reordering and symmetry breaking of azahelicenes
title_full_unstemmed Halogen bond-modulated solid-state reordering and symmetry breaking of azahelicenes
title_short Halogen bond-modulated solid-state reordering and symmetry breaking of azahelicenes
title_sort halogen bond modulated solid state reordering and symmetry breaking of azahelicenes
url https://doi.org/10.1038/s41467-025-59222-2
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AT fuweigan halogenbondmodulatedsolidstatereorderingandsymmetrybreakingofazahelicenes
AT guolizhang halogenbondmodulatedsolidstatereorderingandsymmetrybreakingofazahelicenes
AT chengshuoshen halogenbondmodulatedsolidstatereorderingandsymmetrybreakingofazahelicenes
AT huibinqiu halogenbondmodulatedsolidstatereorderingandsymmetrybreakingofazahelicenes