Anomalously ultra-strong anti-Stokes photoluminescence in submicrometer-thick van der Waals layered semiconductor PbI2

IF 6.8 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Science China Materials Pub Date : 2025-03-12 DOI:10.1007/s40843-024-3272-5

Xiaofei Yue (, ), Qingqing Nie (, ), Jiajun Chen (, ), Shuwen Shen (, ), Jinkun Han (, ), Yabing Shan (, ), Wenxuan Wu (, ), Yuan Lin (, ), Xueting Zhou (, ), Ye Lu (, ), Laigui Hu (, ), Ran Liu (, ), Zhijun Qiu (, ), Chunxiao Cong (, )

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引用次数: 0

Abstract

Anti-Stokes photoluminescence (ASPL) in low-dimensional van der Waals (vdW) layered materials is becoming increasingly attractive for its potential in advanced applications such as optical cooling, sub-energy band detection and optoelectronic devices. While transition metal dichalcogenides (TMDCs), among the most studied vdW semiconductors for ASPL, exhibit a direct bandgap exclusively in their monolayer form. This characteristic results in a short light-matter interaction distance and thus low ASPL emission efficiency, which seriously impedes the advancement of ASPL in vdW layered materials. In contrast, transition metal halide lead iodide (PbI₂), a vdW semiconductor with a direct bandgap in a wide range of thicknesses (⩾3 layers) superior to TMDCs, has shown promise for ASPL. However, the reported ASPL emission efficiency of PbI₂ is notably low. Moreover, scant research has focused on the rich ASPL emission states in PbI₂, particularly concerning the assignment of these emission states. Here, through a designed thickness selection, we observed more detailed ASPL emissions in submicrometer-thick PbI₂ at room temperature, in addition to a series of previously unreported ASPL emission peaks that emerge at low temperatures. Importantly, the low-temperature ASPL of PbI₂ exhibits an approximate 1000-fold enhancement compared to that observed at room temperature. This significant enhancement is attributed to the transition from phonon-assisted one-photon absorption to two-step photon absorption induced by resonance absorption effect, as well as substantially reduced nonradiative decays at low temperatures. Our findings enhance the comprehensive understanding of ASPL in PbI₂, holding great significance for the development of ASPL applications.

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亚微米厚范德华层状半导体PbI2的异常超强反stokes光致发光

低维范德瓦尔斯（vdW）层状材料中的反斯托克斯光致发光（ASPL）因其在光学冷却、亚能带探测和光电子器件等先进应用中的潜力而越来越受到人们的关注。而过渡金属二硫族化合物（TMDCs）是研究最多的用于ASPL的vdW半导体，仅在其单层形式下表现出直接带隙。这一特性导致光-物质相互作用距离短，导致ASPL发射效率低，严重阻碍了vdW层状材料中ASPL的发展。相比之下，过渡金属卤化物碘化铅（PbI2），一种vdW半导体，具有宽范围厚度（大于或等于3层）的直接带隙，优于TMDCs，已经显示出ASPL的前景。然而，报道的PbI2的ASPL发射效率明显较低。此外，关于PbI2中丰富的ASPL发射态的研究很少，特别是关于这些发射态的分配。在这里，通过设计的厚度选择，我们在室温下观察到亚微米厚PbI2中更详细的ASPL发射，以及一系列以前未报道的低温下出现的ASPL发射峰。重要的是，与室温下相比，PbI2的低温ASPL表现出大约1000倍的增强。这种显著的增强归因于共振吸收效应诱导的声子辅助单光子吸收向两步光子吸收的转变，以及低温下非辐射衰变的大幅减少。我们的研究结果增强了对PbI2中ASPL的全面认识，对ASPL应用的发展具有重要意义。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Science China Materials Materials Science-General Materials Science

CiteScore

11.40

自引率

7.40%

发文量

949

期刊介绍： Science China Materials (SCM) is a globally peer-reviewed journal that covers all facets of materials science. It is supervised by the Chinese Academy of Sciences and co-sponsored by the Chinese Academy of Sciences and the National Natural Science Foundation of China. The journal is jointly published monthly in both printed and electronic forms by Science China Press and Springer. The aim of SCM is to encourage communication of high-quality, innovative research results at the cutting-edge interface of materials science with chemistry, physics, biology, and engineering. It focuses on breakthroughs from around the world and aims to become a world-leading academic journal for materials science.