Synergizing internal electric field and quantum-confined stark effect for customized carrier dynamics in two-dimensional heterostructures

IF 6.5 1区化学 Q2 CHEMISTRY, PHYSICAL Journal of Catalysis Pub Date : 2025-02-01 Epub Date: 2024-11-29 DOI:10.1016/j.jcat.2024.115877

Zhihua Zhang , Yingcai Fan , Xikui Ma , Juan Wang , Yiyi Guo , Yangyang Li , Mingwen Zhao

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Abstract

The customized transport of carriers within two-dimensional (2D) heterostructures (HSs) is instrumental in enhancing the electronic and optoelectronic functionalities. Internal electric field (IEF) has opened potential pathways for manipulating carrier migration behaviors, unlocking diverse applications such as photocatalysts, solar cells, photodetectors, and other photoelectrochemical (PEC) devices. While it is intuitively understood that the orientation of IEF governs the direction of carrier transport, there are notable discrepancies between theoretical predictions and experimental results concerning the dynamics of photogenerated carriers. In this work, based on several polar HSs with tunable IEF, we unveiled the role of IEF in the carrier dynamics within these HSs. Our findings show that IEF not only regulates the band alignment of the HSs but also manipulates the electron–phonon (e-ph) coupling. The synergistic interplay of IEF and the quantum-confined Stark effect determines the dynamics of photoexcited carriers, facilitating the transition between type-Ⅱ and Z-scheme. These insights offer prospective strategies for tailoring interlayer charge carrier migration pathways and the photocatalytic activity of HSs.

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二维异质结构中自定义载流子动力学的协同内电场和量子限制stark效应

二维（2D）异质结构（hs）中载流子的定制输运有助于增强电子和光电子功能。内部电场（IEF）为操纵载流子迁移行为开辟了潜在的途径，解锁了各种应用，如光催化剂、太阳能电池、光电探测器和其他光电化学（PEC）器件。虽然人们直观地理解，光生载流子的取向决定了载流子的输运方向，但关于光生载流子的动力学，理论预测和实验结果之间存在显著差异。在这项工作中，基于几个具有可调谐IEF的极性hs，我们揭示了IEF在这些hs中的载流子动力学中的作用。我们的研究结果表明，IEF不仅可以调节hs的波段对准，还可以操纵电子-声子（e-ph）耦合。IEF和量子受限Stark效应的协同相互作用决定了光激发载流子的动力学，促进了-Ⅱ型和z型之间的过渡。这些见解为调整层间电荷载流子迁移路径和HSs的光催化活性提供了前瞻性策略。

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来源期刊

Journal of Catalysis 工程技术-工程：化工

CiteScore

12.30

自引率

5.50%

发文量

447

审稿时长

31 days

期刊介绍： The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.