Photon Correlation Spectroscopy of Luminescent Quantum Defects in Carbon Nanotubes
Photon Correlation Spectroscopy of Luminescent Quantum Defects in Carbon Nanotubes
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DOI：
10.1021/acs.nanolett.9b02553
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发表时间：
2019-10-01
期刊：
影响因子：
10.8
通讯作者：
Hoegele, Alexander
中科院分区：
文献类型：
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作者：
Nutz, Manuel;Zhang, Jiaxiang;Hoegele, Alexander
缺陷修饰的单壁碳纳米管在成像、传感和室温单光子源的开发方面显示出了快速增长的潜力。这种高度非经典发射统计的关键是缺陷局域激子的离散能谱。然而，缺陷组态的变化会产生不同的光谱带，这可能会影响实际器件中的单光子效率和纯度，在实验上，研究不同缺陷特定态之间的激子布居分布一直是具有挑战性的。在这里，我们对己基修饰的单壁碳纳米管进行了光子相关光谱，以揭示中性和带电激子群之间的动力学和竞争。通过在单管水平上的自相关测量，我们证明了缺陷特定激子和三子光致发光的非经典光子发射统计性质，并用互相关光谱确定了它们在光发射事件中的互斥性。此外，我们的研究揭示了粒子搁置时间尺度在10到100 ns之间的暗态的存在。这些新的见解将指导进一步开发用于量子光子学应用的化学定制的碳纳米管状态。
Defect-decorated single-wall carbon nanotubes have shown rapid growing potential for imaging, sensing, and the development of room-temperature single-photon sources. The key to the highly nonclassical emission statistics is the discrete energy spectrum of defect-localized excitons. However, variations in defect configurations give rise to distinct spectral bands that may compromise single-photon efficiency and purity in practical devices, and experimentally it has been challenging to study the exciton population distribution among the various defect-specific states. Here, we performed photon correlation spectroscopy on hexyl-decorated single-wall carbon nanotubes to unravel the dynamics and competition between neutral and charged exciton populations. With autocorrelation measurements at the single-tube level, we prove the nonclassical photon emission statistics of defect-specific exciton and trion photoluminescence and identify their mutual exclusiveness in photoemissive events with cross-correlation spectroscopy. Moreover, our study reveals the presence of a dark state with population-shelving time scales between 10 and 100 ns. These new insights will guide further development of chemically tailored carbon nanotube states for quantum photonics applications.