Interlayer Slipping Facilitating Manipulation of Electronic Properties of Few‐Layer Two‐Dimensional Conjugated Polymers

ABSTRACT Two‐dimensional conjugated polymers (2DCPs) have received great interest in smart devices due to their unique physical properties associated with flexibility, nanosized thickness, and correlated quantum size effect. Control of interlayer interactions of multilayer 2DCPs is crucial for modul...

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Main Authors: Yang Li, Pu Wang, Yongshuai Wang, Dan Liu, Qingbin Li, Jichen Dong, Yunqi Liu, Wenping Hu, Huanli Dong
Format: Article
Language:English
Published: Wiley 2025-06-01
Series:SmartMat
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Online Access:https://doi.org/10.1002/smm2.70019
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author Yang Li
Pu Wang
Yongshuai Wang
Dan Liu
Qingbin Li
Jichen Dong
Yunqi Liu
Wenping Hu
Huanli Dong
author_facet Yang Li
Pu Wang
Yongshuai Wang
Dan Liu
Qingbin Li
Jichen Dong
Yunqi Liu
Wenping Hu
Huanli Dong
author_sort Yang Li
collection DOAJ
description ABSTRACT Two‐dimensional conjugated polymers (2DCPs) have received great interest in smart devices due to their unique physical properties associated with flexibility, nanosized thickness, and correlated quantum size effect. Control of interlayer interactions of multilayer 2DCPs is crucial for modulating the confinement of charge carriers, heat, and photons to give remarkable properties because of the breaking of symmetry. However, to date, it is unclear how the multilayers of 2DCPs affect their physical properties. In this article, we for the first time perform a density functional theory calculation for the interlayer slipping effect on in‐plane electronic properties of few‐layer 2DCPs. Based on five homopolymers formed by C─C bonds with various stacking configurations beyond the inclined and serrated ones, results show that a moderate electric field causes the valence (conduction) band of few‐layer 2DCPs to exhibit distinctive electrical characteristics which are dominated by the outermost two layers on hole (electron) enriched side. Analysis based on recombined molecular orbitals reveals that band properties are sensitive to the interlayer offsets when they result from the interference among multiple orbitals from each building block. This result provides a new guideline for manipulating charge transfer and spintronic properties of few‐layer 2DCPs through an electric field to advance their various applications.
format Article
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institution OA Journals
issn 2688-819X
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publishDate 2025-06-01
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spelling doaj-art-c8cd04b695954f16bb2541df8039ca952025-08-20T02:35:05ZengWileySmartMat2688-819X2025-06-0163n/an/a10.1002/smm2.70019Interlayer Slipping Facilitating Manipulation of Electronic Properties of Few‐Layer Two‐Dimensional Conjugated PolymersYang Li0Pu Wang1Yongshuai Wang2Dan Liu3Qingbin Li4Jichen Dong5Yunqi Liu6Wenping Hu7Huanli Dong8College of Science Shenyang University Shenyang ChinaBeijing National Laboratory for Molecular Science, Key Laboratory of Organic Solids, Institute of Chemistry Chinese Academy of Sciences Beijing ChinaBeijing National Laboratory for Molecular Science, Key Laboratory of Organic Solids, Institute of Chemistry Chinese Academy of Sciences Beijing ChinaBeijing National Laboratory for Molecular Science, Key Laboratory of Organic Solids, Institute of Chemistry Chinese Academy of Sciences Beijing ChinaBeijing National Laboratory for Molecular Science, Key Laboratory of Organic Solids, Institute of Chemistry Chinese Academy of Sciences Beijing ChinaBeijing National Laboratory for Molecular Science, Key Laboratory of Organic Solids, Institute of Chemistry Chinese Academy of Sciences Beijing ChinaBeijing National Laboratory for Molecular Science, Key Laboratory of Organic Solids, Institute of Chemistry Chinese Academy of Sciences Beijing ChinaTianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science Tianjin University and Collaborative Innovation Center of Chemical Science and Engineering Tianjin ChinaBeijing National Laboratory for Molecular Science, Key Laboratory of Organic Solids, Institute of Chemistry Chinese Academy of Sciences Beijing ChinaABSTRACT Two‐dimensional conjugated polymers (2DCPs) have received great interest in smart devices due to their unique physical properties associated with flexibility, nanosized thickness, and correlated quantum size effect. Control of interlayer interactions of multilayer 2DCPs is crucial for modulating the confinement of charge carriers, heat, and photons to give remarkable properties because of the breaking of symmetry. However, to date, it is unclear how the multilayers of 2DCPs affect their physical properties. In this article, we for the first time perform a density functional theory calculation for the interlayer slipping effect on in‐plane electronic properties of few‐layer 2DCPs. Based on five homopolymers formed by C─C bonds with various stacking configurations beyond the inclined and serrated ones, results show that a moderate electric field causes the valence (conduction) band of few‐layer 2DCPs to exhibit distinctive electrical characteristics which are dominated by the outermost two layers on hole (electron) enriched side. Analysis based on recombined molecular orbitals reveals that band properties are sensitive to the interlayer offsets when they result from the interference among multiple orbitals from each building block. This result provides a new guideline for manipulating charge transfer and spintronic properties of few‐layer 2DCPs through an electric field to advance their various applications.https://doi.org/10.1002/smm2.70019density functional theoryinterferenceinterlayer interactionstwo‐dimensional conjugated polymers
spellingShingle Yang Li
Pu Wang
Yongshuai Wang
Dan Liu
Qingbin Li
Jichen Dong
Yunqi Liu
Wenping Hu
Huanli Dong
Interlayer Slipping Facilitating Manipulation of Electronic Properties of Few‐Layer Two‐Dimensional Conjugated Polymers
SmartMat
density functional theory
interference
interlayer interactions
two‐dimensional conjugated polymers
title Interlayer Slipping Facilitating Manipulation of Electronic Properties of Few‐Layer Two‐Dimensional Conjugated Polymers
title_full Interlayer Slipping Facilitating Manipulation of Electronic Properties of Few‐Layer Two‐Dimensional Conjugated Polymers
title_fullStr Interlayer Slipping Facilitating Manipulation of Electronic Properties of Few‐Layer Two‐Dimensional Conjugated Polymers
title_full_unstemmed Interlayer Slipping Facilitating Manipulation of Electronic Properties of Few‐Layer Two‐Dimensional Conjugated Polymers
title_short Interlayer Slipping Facilitating Manipulation of Electronic Properties of Few‐Layer Two‐Dimensional Conjugated Polymers
title_sort interlayer slipping facilitating manipulation of electronic properties of few layer two dimensional conjugated polymers
topic density functional theory
interference
interlayer interactions
two‐dimensional conjugated polymers
url https://doi.org/10.1002/smm2.70019
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