Photoinduced Luminescence Blinking and Bleaching in Individual Single‐Walled Carbon Nanotubes

Georgi, Carsten; Hartmann, Nicolai F.; Gokus, Tobias; Green, Alexander A.; Hersam, Mark C.; Hartschuh, Achim

doi:10.1002/cphc.200800179

Cited by 36 publications

(60 citation statements)

References 36 publications

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“…4 High intensity illumination was found to induce blinking in surface tubes and attributed to the creation of defect states related to chemisorption of oxygen. 5,6 Stepwise blinking was found to occur for freely suspended nanotubes in oxygen ambient, but not in vacuum or in argon, and attributed to defect levels introduced by doping. 7 Capping layers were found to reduce blinking on surface nanotubes, presumably because they act as diffusion barriers.…”

Section: Resultsmentioning

confidence: 99%

Photoinduced Band Gap Shift and Deep Levels in Luminescent Carbon Nanotubes

Finnie

Jacques

2012

ACS Nano

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Individual air-suspended single-walled carbon nanotubes are imaged both spatially and spectrally in photoluminescence. At low excitation power, photoluminescence is bright and stable with high quantum efficiency; however, higher power initially causes a gradual red shift and then more severe changes. Blinking, the loss of quantum efficiency, and the appearance of new deep levels are all seen and can be explained by the introduction of defects. We propose that optical excitation induces molecular deposition onto the nanotube by optically induced van der Waals interactions, leading to physisorption and ultimately chemisorption which severely degrades the luminescence.KEYWORDS: single-walled carbon nanotube . photoluminescence . exciton . quantum efficiency . band gap shift . van der Waals interaction ARTICLE FINNIE AND LEFEBVRE

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Section: Resultsmentioning

confidence: 99%

Photoinduced Band Gap Shift and Deep Levels in Luminescent Carbon Nanotubes

Finnie

Jacques

2012

ACS Nano

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“…Fluorescence bleaching can be caused by protonation of adsorbed oxygen on the SWNT sidewall, the presence of an electron-accepting surfactant, or a photoinduced oxidation of the nanotube caused by chemisorption of initially adsorbed oxygen. 193 Protonation occurs at pH < 7, and could account for some small reduction in the observed fluorescence signal. 193 The presence of sulfate groups on SDS and SDBS make these surfactants slightly more electron-accepting than CAS, and so the former may be able to trap photoexcited charges from the nanotube.…”

Section: Discussionmentioning

confidence: 99%

“…193 Protonation occurs at pH < 7, and could account for some small reduction in the observed fluorescence signal. 193 The presence of sulfate groups on SDS and SDBS make these surfactants slightly more electron-accepting than CAS, and so the former may be able to trap photoexcited charges from the nanotube.…”

Section: Discussionmentioning

confidence: 99%

“…193 In general, the absence of fluctuations in fluorescence intensity at room temperature is attractive for applications in quantum optics that require a steady and uninterrupted source of single photons. Recent studies of fluorescence antibunching have confirmed that SWNTs are single-photon emitters at low temperatures.…”

Section: Discussionmentioning

confidence: 99%

“…193 Therefore, some chemisorption of oxygen likely occurs for all SWNT-surfactant systems upon excitation.…”

Section: Discussionmentioning

confidence: 99%

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Photophysics of Individual Single-Walled Carbon Nanotubes

2008

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Single-walled carbon nanotubes (SWNTs) are cylindrical graphitic molecules that have remained at the forefront of nanomaterials research since 1991, largely due to their exceptional and unusual mechanical, electrical, and optical properties. The motivation for understanding how nanotubes interact with light (i.e., SWNT photophysics) is both fundamental and applied. Individual nanotubes may someday be used as superior near-infrared fluorophores, biological tags and sensors, and components for ultrahigh-speed optical communications systems. Establishing an understanding of basic nanotube photophysics is intrinsically significant and should enable the rapid development of such innovations. Unlike conventional molecules, carbon nanotubes are synthesized as heterogeneous samples, composed of molecules with different diameters, chiralities, and lengths. Because a nanotube can be either metallic or semiconducting depending on its particular molecular structure, SWNT samples are also mixtures of conductors and semiconductors. Early progress in understanding the optical characteristics of SWNTs was limited because nanotubes aggregate when synthesized, causing a mixing of the energy states of different nanotube structures. Recently, significant improvements in sample preparation have made it possible to isolate individual nanotubes, enabling many advances in characterizing their optical properties. In this Account, single-molecule confocal microscopy and spectroscopy were implemented to study the fluorescence from individual nanotubes. Single-molecule measurements naturally circumvent the difficulties associated with SWNT sample inhomogeneities. Intrinsic SWNT photoluminescence has a simple narrow Lorentzian line shape and a polarization dependence, as expected for a one-dimensional system. Although the local environment heavily influences the optical transition wavelength and intensity, single nanotubes are exceptionally photostable. In fact, they have the unique characteristic that their single molecule fluorescence intensity remains constant over time; SWNTs do not “blink” or photobleach under ambient conditions. In addition, transient absorption spectroscopy was used to examine the relaxation dynamics of photoexcited nanotubes and to elucidate the nature of the SWNT excited state. For metallic SWNTs, very fast initial recovery times (300–500 fs) corresponded to excited-state relaxation. For semiconducting SWNTs, an additional slower decay component was observed (50–100 ps) that corresponded to electron–hole recombination. As the excitation intensity was increased, multiple electron–hole pairs were generated in the SWNT; however, these e−h pairs annihilated each other completely in under 3 ps. Studying the dynamics of this annihilation process revealed the lifetimes for one, two, and three e−h pairs, which further confirmed that the photoexcitation of SWNTs produces not free electrons but rather one-dimensional bound electron–hole pairs (i.e., excitons). In summary, nanotube photophysics is a rapidly developing area o...

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Photolithographic Patterning of Organic Color‐Centers

Huang

Powell

et al. 2020

Advanced Materials

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Organic color‐centers (OCCs) have emerged as promising single‐photon emitters for solid‐state quantum technologies, chemically specific sensing, and near‐infrared bioimaging. However, these quantum light sources are currently synthesized in bulk solution, lacking the spatial control required for on‐chip integration. The ability to pattern OCCs on solid substrates with high spatial precision and molecularly defined structure is essential to interface electronics and advance their quantum applications. Herein, a lithographic generation of OCCs on solid‐state semiconducting single‐walled carbon nanotube films at spatially defined locations is presented. By using light‐driven diazoether chemistry, it is possible to directly pattern p‐nitroaryl OCCs, which demonstrate chemically specific spectral signatures at programmed positions as confirmed by Raman mapping and hyperspectral photoluminescence imaging. This light‐driven technique enables the fabrication of OCC arrays on solid films that fluoresce in the shortwave infrared and presents an important step toward the direct writing of quantum emitters and other functionalities at the molecular level.

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Photoinduced Luminescence Blinking and Bleaching in Individual Single‐Walled Carbon Nanotubes

Cited by 36 publications

References 36 publications

Photoinduced Band Gap Shift and Deep Levels in Luminescent Carbon Nanotubes

Photoinduced Band Gap Shift and Deep Levels in Luminescent Carbon Nanotubes

Photophysics of Individual Single-Walled Carbon Nanotubes

Photolithographic Patterning of Organic Color‐Centers

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