Theoretical prediction of topological states in two-dimensional halogen-bonded organic frameworks (XOFs)†

IF 2.9 3区化学 Q3 CHEMISTRY, PHYSICAL

Physical Chemistry Chemical Physics Pub Date : 2025-07-16 DOI:10.1039/D5CP02195B

Yixuan Gao, Yiyang Yin and Lizhi Zhang

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引用次数: 0

Abstract

The rapid development of two-dimensional (2D) crystalline porous frameworks, such as covalent organic frameworks (COFs), metal–organic frameworks (MOFs), and hydrogen-bonded organic frameworks (HOFs), have opened avenues for exploring exotic topological quantum states. However, experimental validation of these theoretical predictions remains rare. Here, we investigate the topological and magnetic properties of newly synthesized halogen-bonded organic frameworks (XOFs) (X. G. Bai, et al., Angew. Chem., Int. Ed., 2024, 63, e202408428), X-TPyB and X-TPEB (X = I, Br), through systematic first-principles calculations. Our results reveal that these frameworks exhibit half-metallic Kagome band structures near the Fermi level, with nontrivial edge states within spin–orbit coupling (SOC)-induced gaps confirming their topological nature. Notably, Br-substituted frameworks (Br-TPEB) demonstrate enhanced ferromagnetic exchange interactions and higher Curie temperatures (∼100 K) compared to I-based analogs, as validated by Monte Carlo simulations. This work opens up a new pathway for investigating topological states in XOFs and introduces a novel class of candidate materials for developing topological quantum devices.

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二维卤素键合有机骨架（XOFs）拓扑态的理论预测

共价有机框架（COFs）、金属有机框架（MOFs）和氢键有机框架（HOFs）等二维（2D）晶体多孔框架的快速发展，为探索奇异拓扑量子态开辟了途径。然而，这些理论预测的实验验证仍然很少。本文研究了新合成的卤素键合有机骨架（XOFs）的拓扑结构和磁性能。化学。Int。编辑。2024,63,e202408428)， X- tpyb和X- tpeb (X = I, Br)，通过系统第一性原理计算。我们的研究结果表明，这些框架在费米能级附近表现出半金属的Kagome带结构，在自旋轨道耦合（SOC）诱导的间隙内具有非平凡边缘态，证实了它们的拓扑性质。值得注意的是，与基于i的类似物相比，br取代框架（Br-TPEB）表现出增强的铁磁交换相互作用和更高的居里温度（~100 K），这一点得到了蒙特卡罗模拟的验证。这项工作为研究XOFs的拓扑态开辟了一条新的途径，并为开发拓扑量子器件引入了一类新的候选材料。

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来源期刊

Physical Chemistry Chemical Physics 化学-物理：原子、分子和化学物理

CiteScore

5.50

自引率

9.10%

发文量

2675

审稿时长

2.0 months

期刊介绍： Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.