In the emerging two-dimensional organic–inorganic hybrid perovskites, the electronic structures and carrier behaviors are strongly impacted by intrinsic electron–phonon interactions, which have received inadequate attention. In this study, we report an intriguing phenomenon of negative carrier diffusion induced by electron–phonon coupling in (2T)₂PbI₄. Theoretical calculations reveal that the electron–phonon coupling drives the band alignment in (2T)₂PbI₄ to alternate between type I and type II heterostructures. As a consequence, photoexcited holes undergo transitions between the organic ligands and inorganic layers, resulting in abnormal carrier transport behavior compared to other two-dimensional hybrid perovskites. These findings provide valuable insights into the role of electron–phonon coupling in shaping the band alignments and carrier behaviors in two-dimensional hybrid perovskites. They also open up exciting avenues for designing and fabricating functional semiconductor heterostructures with tailored properties.

中文翻译：

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用于定制二维杂化钙钛矿中电子-声子耦合的有机配体工程


在新兴的二维有机-无机杂化钙钛矿中，电子结构和载流子行为受到本征电子-声子相互作用的强烈影响，但这一点尚未引起足够的重视。在这项研究中，我们报告了 (2T) ₂ PbI ₄ 中电子-声子耦合引起的负载流子扩散的有趣现象。理论计算表明，电子声子耦合驱动(2T) ₂ PbI ₄ 中的能带排列在I型和II型异质结构之间交替。因此，光生空穴在有机配体和无机层之间发生转变，导致与其他二维杂化钙钛矿相比异常的载流子传输行为。这些发现为了解电子-声子耦合在塑造二维杂化钙钛矿中的能带排列和载流子行为中的作用提供了有价值的见解。它们还为设计和制造具有定制特性的功能半导体异质结构开辟了令人兴奋的途径。