Ubiquity of Exciton Localization in Cryogenic Carbon Nanotubes

Hofmann, Matthias; Noé, Jonathan; Kneer, Alexander; Crochet, Jared; Högele, Alexander

doi:10.1021/acs.nanolett.5b04901

Cited by 25 publications

(27 citation statements)

References 52 publications

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“…It is noteworthy that the segmentation of the E 11 emission (highlighted in blue) at 4 K originates from random localizations of excitons in long polymer-wrapped SWNTs or from other extrinsic defects introduced during initial processing. They are also present in SWNTs that were not specifically functionalized [39][40][41] . An integrated spectrum of 62 spots closely resembles the ensemble spectrum of a thin film at room temperature (Supplementary Fig.…”

Section: Resultsmentioning

confidence: 99%

Synthetic control over the binding configuration of luminescent sp3-defects in single-walled carbon nanotubes

et al. 2021

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The controlled functionalization of single-walled carbon nanotubes with luminescent sp3-defects has created the potential to employ them as quantum-light sources in the near-infrared. For that, it is crucial to control their spectral diversity. The emission wavelength is determined by the binding configuration of the defects rather than the molecular structure of the attached groups. However, current functionalization methods produce a variety of binding configurations and thus emission wavelengths. We introduce a simple reaction protocol for the creation of only one type of luminescent defect in polymer-sorted (6,5) nanotubes, which is more red-shifted and exhibits longer photoluminescence lifetimes than the commonly obtained binding configurations. We demonstrate single-photon emission at room temperature and expand this functionalization to other polymer-wrapped nanotubes with emission further in the near-infrared. As the selectivity of the reaction with various aniline derivatives depends on the presence of an organic base we propose nucleophilic addition as the reaction mechanism.

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Section: Resultsmentioning

confidence: 99%

Synthetic control over the binding configuration of luminescent sp3-defects in single-walled carbon nanotubes

et al. 2021

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“…One of the many exciting properties of semiconducting SWCNTs is their potential for single-photon emission due to exciton localization even without any intentional functionalization and in seemingly homogeneous environments. [105,106] Early experiments had demonstrated photon antibunching (i.e., vanishing probability of the emission of more than one photon per excitation) in nanotubes at cryogenic temperatures [107] and thus introduced them as strong contenders for single-photon emitters in secure quantum communication and even quantum computing. [108] Carbon nanotubes are particularly attractive for these applications for several reasons.…”

Section: Single-photon Emittersmentioning

confidence: 99%

Luminescent Defects in Single‐Walled Carbon Nanotubes for Applications

Zaumseil

2021

Advanced Optical Materials

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most applications, only semiconducting nanotubes and ideally only one (n,m) species (monochiral) are desired. This technological need has pushed the search for more controlled and selective growth of SWCNTs [5,6] and even more importantly fueled the development of post-growth purification and sorting of the different nanotube types and chiralities. Various, quite different techniques, such as gelchromatography, [7][8][9] aqueous two-phase separation (ATPE), [10][11][12] and selective polymer-wrapping, [13][14][15][16][17] now make it possible to produce and work with sufficiently large amounts of not only purely semiconducting nanotubes of a certain diameter range but also monochiral nanotubes and even enantiomerically pure samples. [18,19] This high degree of purification and hence the availability of nanotubes as a material with reproducible properties has been critical for applications in electronics [20,21] and energy conversion, [22,23] as well as imaging [24,25] and sensing [26,27] based on the near-infrared photoluminescence (PL) of SWCNTs and its modulation. However, an important paradigm shift occurred when it became clear that defects in the sp 2 carbon lattice of nanotubes are not always detrimental to the photoluminescence yield, but can indeed lead to new electronic states with highly interesting and useful optical properties. [28][29][30] These specific defects, which are variably named sp 3 defects, luminescent defects, organic color centers or quantum defects [31][32][33][34][35] have been at the heart of many recent studies on carbon nanotubes and promise a wide range of potential applications from single-photon emission to in vivo super-resolution imaging. This review will briefly introduce the underlying photo physics and properties of these defects, peruse recent progress in their controlled creation and discuss the various potential applications in detail.Semiconducting single-walled carbon nanotubes show extraordinary electronic and optical properties, such as high charge carrier mobilities and diameter-dependent near-infrared photoluminescence. The introduction of sp 3 defects in the carbon lattice of these nanotubes creates new electronic states that result in even further red-shifted photoluminescence with longer lifetimes and higher photoluminescence yield. These luminescent defects or organic color centers can be tuned chemically by controlling the precise binding configuration and the electrostatic properties of the attached substituents. This review covers the basic photophysics of luminescent sp 3 defects, synthetic methods for their controlled formation and discusses their application as near-infrared single-photon emitters at room temperature, in electroluminescent devices, as versatile optical sensors, and as fluorophores for bioimaging and potential super-resolution microscopy.

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“…When lower energy states are populated with a certain number of excitons, the subsequent excitons must then occupy higher energy states due to the Pauli principle26. In CNTs, the quasi-1D electronic structure differs from QDs in that excitons are mobile along the tube direction and thereby a new multiexciton ground state could be created at higher energy27. However, if somehow the exciton path is blocked, then the exciton is localized and lower dimensional effects such as state filling become important.…”

Section: Resultsmentioning

confidence: 99%

Quantum dot-like excitonic behavior in individual single walled-carbon nanotubes

Wang

Alexander-Webber

Jia

et al. 2016

Sci Rep

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Semiconducting single-walled carbon nanotubes are one-dimensional materials with great prospects for applications such as optoelectronic and quantum information devices. Yet, their optical performance is hindered by low fluorescent yield. Highly mobile excitons interacting with quenching sites are attributed to be one of the main non-radiative decay mechanisms that shortens the exciton lifetime. In this paper we report on time-integrated photoluminescence measurements on individual polymer wrapped semiconducting carbon nanotubes. An ultra narrow linewidth we observed demonstrates intrinsic exciton dynamics. Furthermore, we identify a state filling effect in individual carbon nanotubes at cryogenic temperatures as previously observed in quantum dots. We propose that each of the CNTs is segmented into a chain of zero-dimensional states confined by a varying local potential along the CNT, determined by local environmental factors such as the amount of polymer wrapping. Spectral diffusion is also observed, which is consistent with the tunneling of excitons between these confined states.

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Ubiquity of Exciton Localization in Cryogenic Carbon Nanotubes

Cited by 25 publications

References 52 publications

Synthetic control over the binding configuration of luminescent sp3-defects in single-walled carbon nanotubes

Synthetic control over the binding configuration of luminescent sp3-defects in single-walled carbon nanotubes

Luminescent Defects in Single‐Walled Carbon Nanotubes for Applications

Quantum dot-like excitonic behavior in individual single walled-carbon nanotubes

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