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中国物理学会期刊

双微球远程耦合实现激子及其复合体分离

Dual-Microsphere Remote Coupling Enabling Separation of Exciton and Complexes States

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  • 二维过渡金属硫族化合物单层材料中的激子及其复合体是研究低维多体物理的重要载体, 但其光致发光谱成分复杂且受缺陷态背景干扰, 难以分离鉴别. 本文提出一种“边缘激发-远程收集”的双介电微球远程耦合结构, 实现激子光谱筛选和鉴别. 一方面, 微球与金属界面模共同提供光学耦合选择性, 边缘激发可将可耦合的激子辐射近场分量定向转化为远程传播信号; 另一方面, 不同激子态在样品内具有不同的有效传播尺度, 远程收集保留可传播的激子能量贡献. 这种双重筛选机制有效抑制了宽谱背景, 并提高了特征谱线的可辨识度. 基于此, 我们在多组微球共振条件与多器件上重复测量, 观察到两个特征峰的能量锁定现象, 并以明激子为内标获得二者稳定的能量差统计(67.1±5.5 meV与87.6±5.8 meV); 结合路径互换、局部破损扰动与功率幂律分析, 建立无需外场的判据链, 区分两组成分在远程读出链路中的参与差异并给出了初步激子成分判断. 该方法为非理想样品条件下暗态相关发光的可重复读出与候选归属提供了实用谱学工具.

    Monolayer transition metal dichalcogenides host rich excitonic states, including bright excitons, dark excitons, charged complexes, and phonon-assisted sidebands, and therefore provide an important platform for studying low-dimensional excitonic many-body physics. However, in low-temperature photoluminescence measurements, weak excitonic features are often buried under broad defect-related emission, making reliable spectral separation and identification difficult. In this work, a low-temperature photoluminescence scheme based on dual-dielectric-microsphere remote coupling is developed to realize edge excitation and remote detection of excitonic emission in monolayer WSe2. Two fused-silica microspheres with diameters of about 6 μm and a separation of 10-20 μm are used as the excitation and detection terminals, respectively. By taking advantage of the difference in effective propagation length between localized defect emission and propagating excitonic channels, together with mode-selective near-field coupling at the interface, the proposed geometry suppresses broad background emission and enhances weak exciton-related spectral features without applying external-field modulation. Experimental results show that, compared with center excitation, edge excitation increases the photoluminescence intensity by about 2.35 times and enables more stable observation of characteristic narrow peaks under remote detection. Systematic measurements performed under different microsphere resonance conditions and on different device regions reveal two robust spectral components, denoted as A (~1.691 eV) and B (~1.668 eV), whose energies remain locked relative to the bright exciton. Statistical analysis gives stable energy offsets of 67.1±5.5 meV and 87.6±5.8 meV for A and B, respectively. Further evidence from path-interchange measurements, local-damage perturbation, and power-dependent photoluminescence shows that the two components exhibit clearly different behaviors in the remote detection process: component A is more robust in long-range readout and shows an approximately linear power dependence (α = 1.104), whereas component B is more sensitive to path variation and local damage and exhibits a sublinear power dependence (α = 0.826). These results indicate that component A is more likely associated with a dark-state-related excitonic complex with stronger interfacial coupling, while component B is more likely related to a phonon-assisted branch or replica of a dark-state-related excitation. The present method provides an effective optical approach for suppressing defect background, enhancing weak excitonic channels, and performing preliminary spectroscopic identification of dark-state-related emission and exciton complexes in nonideal two-dimensional semiconductors.

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