Pressure-controlled free exciton and self-trapped exciton emission in quasi-one-dimensional hybrid lead bromides.

IF 15.7 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES
Bin Xu, Yawen Li, Peibin Hong, Peijie Zhang, Jiang Han, Zewen Xiao, Zewei Quan
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Abstract

Hybrid metal halides represent a novel type of semiconductor light emitters with intriguing excitonic emission properties, including free exciton emission and self-trapped exciton emission. Achieving precise control over these two excitonic emissions in hybrid metal halides is highly desired yet remains challenging. Here, the complete transformation from intrinsically broadband self-trapped exciton emission to distinctively sharp free exciton emission in a quasi-one-dimensional hybrid metal halide (C2H10N2)8[Pb4Br18]·6Br with a ribbon width of n = 4, is successfully achieved based on high-pressure method. During compression, pressure-induced phonon hardening continuously reduces exciton-phonon coupling, therefore suppressing excitonic localization and quenching the original self-trapped exciton emission. Notably, further compression triggers excitonic delocalization to induce intense free exciton emission, accompanied with reduced carrier effective masses and improved charge distribution. Controlled high-pressure investigations indicate that the ribbon width of n > 2 is necessary to realize excitonic delocalization and generate free exciton emissions in similar quasi-one-dimensional hybrid metal halides. This work presents an important photophysical process of excitonic transitions from self-trapped exciton emission to free exciton emission in quasi-one-dimensional hybrid metal halides without chemical regulation, promoting the rational synthesis of hybrid metal halides with desired excitonic emissions.

Abstract Image

准一维混合溴化铅中受压力控制的自由激子和自俘获激子发射。
混合金属卤化物是一种新型的半导体发光体,具有引人入胜的激子发射特性,包括自由激子发射和自阱激子发射。在混合金属卤化物中实现对这两种激子发射的精确控制是人们的强烈愿望,但仍然具有挑战性。在这里,基于高压方法,我们成功地在带宽为 n = 4 的准一维混合金属卤化物 (C2H10N2)8[Pb4Br18]-6Br 中实现了从固有宽带自俘获激子发射到独特尖锐的自由激子发射的完全转变。在压缩过程中,压力诱导的声子硬化会不断降低激子-声子耦合,从而抑制激子定位并淬灭原有的自俘获激子发射。值得注意的是,进一步压缩会引发激子去局域化,从而诱发强烈的自由激子发射,同时降低载流子有效质量并改善电荷分布。受控高压研究表明,在类似的准一维杂化金属卤化物中,n > 2 的带状宽度是实现激子去局域化和产生自由激子发射的必要条件。这项工作展示了准一维杂化金属卤化物中从自俘获激子发射到自由激子发射的重要光物理转变过程,无需化学调控,促进了具有所需激子发射的杂化金属卤化物的合理合成。
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来源期刊
Nature Communications
Nature Communications Biological Science Disciplines-
CiteScore
24.90
自引率
2.40%
发文量
6928
审稿时长
3.7 months
期刊介绍: Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.
文献相关原料
公司名称
产品信息
阿拉丁
Lead bromide (PbBr2)
阿拉丁
Ethylenediamine monohydrate
阿拉丁
Hydrogen bromide
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