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钙钛矿纳米晶超晶格中激子的环境辅助量子输运

Environment-assisted quantum transport of excitons in perovskite nanocrystal superlattices.

作者信息

Blach Daria D, Lumsargis-Roth Victoria A, Chuang Chern, Clark Daniel E, Deng Shibin, Williams Olivia F, Li Christina W, Cao Jianshu, Huang Libai

机构信息

Department of Chemistry, Purdue University, West Lafayette, IN, USA.

Department of Chemistry and Biochemistry, University of Nevada, Las Vegas, NV, USA.

出版信息

Nat Commun. 2025 Feb 2;16(1):1270. doi: 10.1038/s41467-024-55812-8.

Abstract

Transport of energy carriers in solid-state materials is determined by their wavefunctions and interactions with the environment. While quantum transport theory has predicted distinct transport in the intermediate coupling regime resulting from the intricate interplay between coherent wave-like and incoherent particle-like mechanisms, these predictions are awaiting experimental evidence. Here we demonstrate quantum transport signatures in perovskite nanocrystal superlattices by imaging exciton propagation with high spatial and temporal resolutions over 7-298 K. At 7 K, coherent propagation of the excitons dominates, with transient ballistic motion within a coherence length of up to 40 nanocrystal sites. The interference of the wave-like motion leads to Anderson Localization in the long-time limit. As temperature increases, a peak in the long-time diffusion constant is observed at a temperature where static disorder and dephasing are balanced, which substantiates evidence for environment-assisted quantum transport. Our results connect theoretical predictions and experiments using a stochastic Anderson localization model, highlighting perovskite nanocrystals as promising building blocks for quantum materials.

摘要

固态材料中能量载体的传输由其波函数以及与环境的相互作用决定。虽然量子传输理论预测,由于相干波状机制和非相干粒子状机制之间的复杂相互作用,在中间耦合区域会出现独特的传输现象,但这些预测仍有待实验验证。在此,我们通过在7至298 K的温度范围内以高空间和时间分辨率对激子传播进行成像,展示了钙钛矿纳米晶体超晶格中的量子传输特征。在7 K时,激子的相干传播占主导,在长达40个纳米晶体位点的相干长度内存在瞬态弹道运动。波状运动的干涉在长时间极限下导致安德森局域化。随着温度升高,在静态无序和退相达到平衡的温度下,观察到长时间扩散常数出现峰值,这为环境辅助量子传输提供了证据。我们的结果使用随机安德森局域化模型将理论预测与实验联系起来,突出了钙钛矿纳米晶体作为量子材料有前景的构建单元。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b203/11788439/0cccc5f1c0e5/41467_2024_55812_Fig1_HTML.jpg

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