Journal
NANO LETTERS
Volume 19, Issue 10, Pages 7078-7084Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.9b02553
Keywords
Carbon nanotubes; covalent quantum defects; photoluminescence spectroscopy; photon correlation spectroscopy; single photon emission statistics; bunching; antibunching; localized excitons; localized trions
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Funding
- European Research Council [336749, 772195]
- Volkswagen Foundation
- Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under German Excellence Initiative via the Nanosystems Initiative Munich (NIM)
- Center for NanoScience (CeNS)
- LMUinnovativ
- National Science Foundation [PHY-1839165, CHE-1507974]
- Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany's Excellence Strategy [EXC-2111-390814868]
- European Research Council (ERC) [336749, 772195] Funding Source: European Research Council (ERC)
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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.
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