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  1. Article ; Online: Variations in bile salt surfactant structure allow tuning of the sorting of single-wall carbon nanotubes by aqueous two-phase extraction.

    Avramenko, Marina / Defillet, Joeri / López Carrillo, Miguel Ángel / Martinati, Miles / Wenseleers, Wim / Cambré, Sofie

    Nanoscale

    2022  Volume 14, Issue 41, Page(s) 15484–15497

    Abstract: Being some of the most efficient agents to individually solubilize single-wall carbon nanotubes (SWCNTs), bile salt surfactants (BSS) represent the foundation for the surfactant-based structure sorting and spectroscopic characterization of SWCNTs. In ... ...

    Abstract Being some of the most efficient agents to individually solubilize single-wall carbon nanotubes (SWCNTs), bile salt surfactants (BSS) represent the foundation for the surfactant-based structure sorting and spectroscopic characterization of SWCNTs. In this work, we investigate three BSS in their ability to separate different SWCNT chiral structures by aqueous two-phase extraction (ATPE): sodium deoxycholate (DOC), sodium cholate (SC) and sodium chenodeoxycholate (CDOC). The small difference in their chemical structure (just one hydroxyl group) leads to significant differences in their stacking behavior on SWCNT walls with different diameter and chiral structure that, in turn, has direct consequences for the chiral sorting of SWCNTs using these BSS. By performing several series of systematic ATPE experiments, we reveal that, in general, the stacking of DOC and CDOC is more enantioselective than the stacking of SC on the SWCNT walls, while SC has a clear diameter preference for efficiently solubilizing the SWCNTs in comparison to DOC and CDOC. Moreover, combining sodium dodecylsulfate with SC allows for resolving the ATPE sorting transitions of empty and water-filled SWCNTs for a number of SWCNT chiralities. We also show that addition of SC to combinations of DOC and sodium dodecylbenzenesulfonate can enhance separations of particular chiralities.
    Language English
    Publishing date 2022-10-27
    Publishing country England
    Document type Journal Article
    ZDB-ID 2515664-0
    ISSN 2040-3372 ; 2040-3364
    ISSN (online) 2040-3372
    ISSN 2040-3364
    DOI 10.1039/d2nr03883h
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  2. Article: The role of the bile salt surfactant sodium deoxycholate in aqueous two-phase separation of single-wall carbon nanotubes revealed by systematic parameter variations

    Defillet, Joeri / Avramenko, Marina / Martinati, Miles / López Carrillo, Miguel Ángel / Van der Elst, Domien / Wenseleers, Wim / Cambré, Sofie

    Carbon. 2022 Aug. 15, v. 195

    2022  

    Abstract: Aqueous two-phase (ATP) extraction has been demonstrated as a fast, scalable, and effective separation technique to sort single-wall carbon nanotubes (SWCNTs) according to their diameter and chiral structure. The exact mechanism behind the chirality- ... ...

    Abstract Aqueous two-phase (ATP) extraction has been demonstrated as a fast, scalable, and effective separation technique to sort single-wall carbon nanotubes (SWCNTs) according to their diameter and chiral structure. The exact mechanism behind the chirality-dependent migration of SWCNTs between the two phases is however not completely understood, and depends on many parameters (e.g., choice of surfactants and their concentration, pH, temperature, …), making it difficult to optimize the multivariable parameter space. In this work, we present a systematic study of the choice and concentration of specific surfactants on the ATP sorting, by performing a series of single-step ATP separations in which each time only one parameter is systematically varied, while monitoring the structure-specific migration of every SWCNT chirality between both phases with detailed wavelength-dependent spectroscopy. These systematic studies reveal that the diameter-dependent stacking of a discrete number of sodium deoxycholate molecules fitting around the SWCNT circumference determines the separation order in the form of a periodically modulated pattern as a function of SWCNT diameter. Addition of cosurfactants can be used to compete with the bile salt surfactant to enhance the separation yields, but does not affect the sorting order. The results are afterwards directly applied to predict the parameters required to separate specific chiral structures in just two ATP steps.
    Keywords bile salts ; carbon ; carbon nanotubes ; deoxycholic acid ; optical isomerism ; pH ; spectroscopy ; surfactants ; temperature
    Language English
    Dates of publication 2022-0815
    Size p. 349-363.
    Publishing place Elsevier Ltd
    Document type Article
    ISSN 0008-6223
    DOI 10.1016/j.carbon.2022.03.071
    Database NAL-Catalogue (AGRICOLA)

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  3. Article: Electronic structure of confined carbyne from joint wavelength-dependent resonant Raman spectroscopy and density functional theory investigations

    Martinati, Miles / Wenseleers, Wim / Shi, Lei / Pratik, Saied Md / Rohringer, Philip / Cui, Weili / Pichler, Thomas / Coropceanu, Veaceslav / Brédas, Jean-Luc / Cambré, Sofie

    Carbon. 2022 Apr. 15, v. 189

    2022  

    Abstract: Carbyne, i.e. an infinitely long linear carbon chain (LCC), has been at the focus of a lot of research for quite a while, yet its optical, electronic, and vibrational properties have only recently started to become accessible experimentally thanks to its ...

    Abstract Carbyne, i.e. an infinitely long linear carbon chain (LCC), has been at the focus of a lot of research for quite a while, yet its optical, electronic, and vibrational properties have only recently started to become accessible experimentally thanks to its synthesis inside carbon nanotubes (CNTs). While the role of the host CNT in determining the optical gap of the LCCs has been studied previously, little is known about the excited states of such ultralong LCCs. In this work, we employ the selectivity of wavelength-dependent resonant Raman spectroscopy to investigate the excited states of ultralong LCCs encapsulated inside double-walled CNTs. In addition to the optical gap, the Raman resonance profile shows three additional resonances. Corroborated with DFT calculations on LCCs with up to 100 carbon atoms, we assign these resonances to a vibronic series of a different electronic state. Indeed, the calculations predict the existence of two optically allowed electronic states separated by an energy of 0.14–0.22 eV in the limit of an infinite chain, in agreement with the experimental results. Furthermore, among these two states, the one with highest energy is also characterized by the largest electron-vibration couplings, which explains the corresponding vibronic series of overtones.
    Keywords Raman spectroscopy ; carbon ; carbon nanotubes ; density functional theory ; energy
    Language English
    Dates of publication 2022-0415
    Size p. 276-283.
    Publishing place Elsevier Ltd
    Document type Article
    ISSN 0008-6223
    DOI 10.1016/j.carbon.2021.12.059
    Database NAL-Catalogue (AGRICOLA)

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  4. Article: Well-defined sub-nanometer graphene ribbons synthesized inside carbon nanotubes

    Kuzmany, Hans / Shi, Lei / Martinati, Miles / Cambré, Sofie / Wenseleers, Wim / Kürti, Jenő / Koltai, János / Kukucska, Gergő / Cao, Kecheng / Kaiser, Ute / Saito, Takeshi / Pichler, Thomas

    Carbon. 2021 Jan., v. 171

    2021  

    Abstract: Graphene nanoribbons with sub-nanometer widths are extremely interesting for nanoscale electronics and devices as they combine the unusual transport properties of graphene with the opening of a band gap due to quantum confinement in the lateral dimension. ...

    Abstract Graphene nanoribbons with sub-nanometer widths are extremely interesting for nanoscale electronics and devices as they combine the unusual transport properties of graphene with the opening of a band gap due to quantum confinement in the lateral dimension. Strong research efforts are presently paid to grow such nanoribbons. Here we show the synthesis of 6- and 7-armchair graphene nanoribbons, with widths of 0.61 and 0.74 nm, and excitonic gaps of 1.83 and 2.18 eV, by high-temperature vacuum annealing of ferrocene molecules inside single-walled carbon nanotubes. The growth of the so-obtained graphene nanoribbons is evidenced from atomic resolution electron microscopy, while their well-defined structure is identified by a combination of an extensive wavelength-dependent Raman scattering characterization and quantum-chemical calculations. These findings enable a facile and scalable approach leading to the controlled growth and detailed analysis of well-defined sub-nanometer graphene nanoribbons.
    Keywords carbon nanotubes ; electron microscopy ; electronics ; ferrocenes ; graphene
    Language English
    Dates of publication 2021-01
    Size p. 221-229.
    Publishing place Elsevier Ltd
    Document type Article
    Note NAL-AP-2-clean
    ISSN 0008-6223
    DOI 10.1016/j.carbon.2020.08.065
    Database NAL-Catalogue (AGRICOLA)

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  5. Book ; Online: The role of the bile salt surfactant sodium deoxycholate in aqueous two-phase separation of single-wall carbon nanotubes revealed by systematic parameter variations

    Defillet, Joeri / Avramenko, Marina / Martinati, Miles / Carillo, Miguel Ángel López / Van der Elst, Domien / Wenseleers, Wim / Cambré, Sofie

    2022  

    Abstract: Aqueous two-phase (ATP) extraction has been demonstrated as a fast, scalable, and effective separation technique to sort single-wall carbon nanotubes (SWCNTs) according to their diameter and chiral structure. The exact mechanism behind the chirality- ... ...

    Abstract Aqueous two-phase (ATP) extraction has been demonstrated as a fast, scalable, and effective separation technique to sort single-wall carbon nanotubes (SWCNTs) according to their diameter and chiral structure. The exact mechanism behind the chirality-dependent migration of SWCNTs between the two phases is however not completely understood, and depends on many parameters (e.g., choice of surfactants and their concentration, pH, temperature, .), making it difficult to optimize the multivariable parameter space. In this work, we present a systematic study of the choice and concentration of specific surfactants on the ATP sorting, by performing a series of single-step ATP separations in which each time only one parameter is systematically varied, while monitoring the structure-specific migration of every SWCNT chirality between both phases with detailed wavelength-dependent spectroscopy. These systematic studies reveal that the diameter-dependent stacking of a discrete number of sodium deoxycholate molecules fitting around the SWCNT circumference determines the separation order in the form of a periodically modulated pattern as a function of SWCNT diameter. Addition of cosurfactants can be used to compete with the bile salt surfactant to enhance the separation yields, but does not affect the sorting order. The results are afterwards directly applied to predict the parameters required to separate specific chiral structures in just two ATP steps.
    Keywords Condensed Matter - Mesoscale and Nanoscale Physics ; Physics - Optics
    Subject code 612
    Publishing date 2022-04-18
    Publishing country us
    Document type Book ; Online
    Database BASE - Bielefeld Academic Search Engine (life sciences selection)

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  6. Book ; Online: Well-defined sub-nanometer graphene ribbons synthesized inside carbon nanotubes

    Kuzmany, Hans / Shi, Lei / Martinati, Miles / Cambré, Sofie / Wenseleers, Wim / Kürti, Jenő / Koltai, János / Kukucska, Gergő / Cao, Kecheng / Kaiser, Ute / Saito, Takeshi / Pichler, Thomas

    2020  

    Abstract: Graphene nanoribbons with sub-nanometer widths are extremely interesting for nanoscale electronics and devices as they combine the unusual transport properties of graphene with the opening of a band gap due to quantum confinement in the lateral dimension. ...

    Abstract Graphene nanoribbons with sub-nanometer widths are extremely interesting for nanoscale electronics and devices as they combine the unusual transport properties of graphene with the opening of a band gap due to quantum confinement in the lateral dimension. Strong research efforts are presently paid to grow such nanoribbons. Here we show the synthesis of 6- and 7-armchair graphene nanoribbons, with widths of 0.61 and 0.74 nm, and excitonic gaps of 1.83 and 2.18 eV, by high-temperature vacuum annealing of ferrocene molecules inside single-walled carbon nanotubes. The encapsulation of the so-obtained graphene nanoribbons is proved by atomic resolution electron microscopy, while their assignment is provided by a combination of an extensive wavelength-dependent Raman scattering characterization and quantum-chemical calculations. These findings enable a facile and scalable approach leading to the controlled growth and detailed analysis of well-defined sub-nanometer graphene nanoribbons.

    Comment: 35 pages, 4 figures
    Keywords Condensed Matter - Materials Science
    Subject code 541
    Publishing date 2020-06-23
    Publishing country us
    Document type Book ; Online
    Database BASE - Bielefeld Academic Search Engine (life sciences selection)

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