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单分子电致发光中自旋三重态介导的上转换和交叉行为。

Spin-Triplet-Mediated Up-Conversion and Crossover Behavior in Single-Molecule Electroluminescence.

作者信息

Chen Gong, Luo Yang, Gao Hongying, Jiang Jun, Yu Yunjie, Zhang Li, Zhang Yang, Li Xiaoguang, Zhang Zhenyu, Dong Zhenchao

机构信息

International Center for Quantum Design of Functional Materials (ICQD), Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230026, China.

School of Physics and Engineering, Zhengzhou University, Zhengzhou, Henan 450052, China.

出版信息

Phys Rev Lett. 2019 May 3;122(17):177401. doi: 10.1103/PhysRevLett.122.177401.

Abstract

Scanning-tunneling-microscope-induced light emission serves as a powerful approach in revealing and manipulating the optical properties of molecular species, intermolecular energy transfer, and plasmon-molecule coupling. Earlier studies have established the existence of molecular up-conversion electroluminescence in diverse situations, but the underlying microscopic mechanisms are still under active debate, dominated by intermolecular triplet-triplet annihilation and plasmonic pumping. Here we report on the experimental realization of up-conversion electroluminescence from a prototypical single phthalocyanine molecule, allowing us to unambiguously rule out mechanisms based on intermolecular coupling and also offering unprecedented opportunities to elucidate much richer characteristics unforeseen in previous studies. In particular, the bias-dependent emission intensity displays three distinct regions with different nonlinear current dependences, which can be attributed to crossover behavior caused by the interplay between inelastic electron scattering and carrier-injection processes. We also develop a microscopic description to capture the essential physics involved in up-conversion electroluminescence mediated by a proper intermediate spin-triplet state.

摘要

扫描隧道显微镜诱导发光是揭示和操纵分子物种的光学性质、分子间能量转移以及等离子体-分子耦合的有力方法。早期研究已证实分子上转换电致发光在多种情况下的存在,但其潜在的微观机制仍在激烈争论中,主要争议点在于分子间三重态-三重态湮灭和等离子体泵浦。在此,我们报告了从典型的单个酞菁分子实现上转换电致发光的实验,这使我们能够明确排除基于分子间耦合的机制,还为阐明先前研究中未预见的更丰富特性提供了前所未有的机会。特别是,偏压依赖的发射强度显示出具有不同非线性电流依赖性的三个不同区域,这可归因于非弹性电子散射与载流子注入过程之间相互作用引起的交叉行为。我们还开发了一种微观描述,以捕捉由适当的中间自旋三重态介导的上转换电致发光所涉及的基本物理过程。

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