Revealing and Manipulating Hidden Fine-Structure Coherence of Bright Excitons in CsPbI3 Perovskite Quantum Dots.

IF 11.3 1区 化学 Q1 CHEMISTRY, PHYSICAL ACS Catalysis Pub Date : 2024-11-13 Epub Date: 2024-10-31 DOI:10.1021/acs.nanolett.4c04772
Kaimin Gao, Yuxuan Li, Yupeng Yang, Boyu Zhang, Meng Liu, Jingyi Zhu, Kaifeng Wu
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Abstract

Observation and understanding of fine-structure splitting of bright excitons in lead halide perovskite quantum dots (QDs) are crucial to their emerging applications in quantum light sources and exciton coherence manipulation. Recent studies demonstrate that ensemble-level polarization-resolved transient absorption spectroscopy can reveal the quantum beats arising from the coherence between two fine-structure levels. Here we report the observation of an extra fine-structure quantum coherence hidden in previous studies by using cryo-magnetic quantum beat spectroscopy. In ∼6 nm CsPbI3 QDs, two splitting energies of 0.25 and 1.20 meV were observed at 1.7 K, which gradually increased to 0.74 and 1.55 meV, respectively, when a longitudinal magnetic field up to 7 T was applied. The field dependence allowed us to extract two distinct nominal Landé g-factors corresponding to QDs with different orientations with respect to the external field.

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揭示和操纵 CsPbI3 包晶量子点中明亮激子的隐藏细微结构相干。
观察和了解卤化铅过氧化物量子点(QDs)中明亮激子的精细结构分裂,对于它们在量子光源和激子相干操纵方面的新兴应用至关重要。最近的研究表明,集合级偏振分辨瞬态吸收光谱可以揭示两个精细结构级之间的相干所产生的量子节拍。在此,我们报告了利用低温磁量子节拍光谱观测到的隐藏在以往研究中的额外精细结构量子相干性。在 ∼6 nm CsPbI3 QDs 中,我们观察到 1.7 K 时的两个分裂能量分别为 0.25 和 1.20 meV,当施加高达 7 T 的纵向磁场时,这两个分裂能量分别逐渐增加到 0.74 和 1.55 meV。根据磁场依赖性,我们可以提取出两个不同的标称朗德 g 因子,它们对应于相对于外部磁场具有不同取向的 QD。
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来源期刊
ACS Catalysis
ACS Catalysis CHEMISTRY, PHYSICAL-
CiteScore
20.80
自引率
6.20%
发文量
1253
审稿时长
1.5 months
期刊介绍: ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
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