“Towards Novel Multifunctional Pillared Nanostructures: Effective Intercalation of Adamantylamine in Graphene Oxide and Smectite Clays”. Spyrou K, Potsi G, Diamanti EK, Ke X, Serestatidou E, Verginadis II, Velalopoulou AP, Evangelou AM, Deligiannakis Y, Van Tendeloo G, Gournis D, Rudolf P;, Advanced functional materials 24, 5841 (2014). http://doi.org/10.1002/adfm.201400975
Abstract: Multifunctional pillared materials are synthesized by the intercalation of cage-shaped adamantylamine (ADMA) molecules into the interlayer space of graphite oxide (GO) and aluminosilicate clays. The physicochemical and structural properties of these hybrids, determined by X-ray diffraction (XRD), Fourier transform infrared (FTIR), Raman and X-ray photoemission (XPS) spectroscopies and transmission electron microscopy (TEM) show that they can serve as tunable hydrophobic/hydrophilic and stereospecific nanotemplates. Thus, in ADMA-pillared clay hybrids, the phyllomorphous clay provides a hydrophilic nanoenvironment where the local hydrophobicity is modulated by the presence of ADMA moieties. On the other hand, in the ADMA-GO hybrid, both the aromatic rings of GO sheets and the ADMA molecules define a hydrophobic nanoenvironment where sp(3)-oxo moieties (epoxy, hydroxyl and carboxyl groups), present on GO, modulate hydrophilicity. As test applications, these pillared nanostructures are capable of selective/stereospecific trapping of small chlorophenols or can act as cytotoxic agents.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 12.124
Times cited: 19
DOI: 10.1002/adfm.201400975
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“Direct determination of polarity, faceting, and core location in colloidal core/shell wurtzite semiconductor nanocrystals”. Bertoni G, Grillo V, Brescia R, Ke X, Bals S, Catellani A, Li H, Manna L, ACS nano 6, 6453 (2012). http://doi.org/10.1021/nn302085t
Abstract: The ability to determine the atomic arrangement and termination of various facets of surfactant-coated nanocrystals is of great importance for understanding their growth mechanism and their surface properties and represents a critical piece of information that can be coupled to other experimental techniques and to calculations. This is especially appealing in the study of nanocrystals that can be grown in strongly anisotropic shapes, for which the relative growth rates of various facets can be influenced under varying reaction conditions. Here we show that in two representative cases of rod-shaped nanocrystals in the wurtzite phase (CdSe(core)/CdS(shell) and ZnSe(core)/ZnS(shell) nanorods) the terminations of the polar facets can be resolved unambiguously by combining advanced electron microscopy techniques, such as aberration-corrected HRTEM with exit wave reconstruction or aberration-corrected HAADF-STEM. The [0001] and [000-1] polar directions of these rods, which grow preferentially along their c-axis, are revealed clearly, with one side consisting of the Cd (or Zn)-terminated (0001) facet and the other side with a pronounced faceting due to Cd (or Zn)-terminated {10-1-1} facets. The lateral faceting of the rods is instead dominated by three nonpolar {10-10} facets. The core buried in the nanostructure can be localized in both the exit wave phase and HAADF-STEM images.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 13.942
Times cited: 63
DOI: 10.1021/nn302085t
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“Knitting the catalytic pattern of artificial photosynthesis to a hybrid graphene nanotexture”. Quintana M, López AM, Rapino S, Toma FM, Iurlo M, Carraro M, Sartorel A, Maccato C, Ke X, Bittencourt C, Da Ros T, Van Tendeloo G, Marcaccio M, Paolucci F, Prato M, Bonchio M;, ACS nano 7, 811 (2013). http://doi.org/10.1021/nn305313q
Abstract: The artificial leaf project calls for new materials enabling multielectron catalysis with minimal overpotential, high turnover frequency, and long-term stability. Is graphene a better material than carbon nanotubes to enhance water oxidation catalysis for energy applications? Here we show that functionalized graphene with a tailored distribution of polycationic, quaternized, ammonium pendants provides an sp(2) carbon nanoplatform to anchor a totally inorganic tetraruthenate catalyst, mimicking the oxygen evolving center of natural PSII. The resulting hybrid material displays oxygen evolution at overpotential as low as 300 mV at neutral pH with negligible loss of performance after 4 h testing. This multilayer electroactive asset enhances the turnover frequency by 1 order of magnitude with respect to the isolated catalyst, and provides a definite up-grade of the carbon nanotube material, with a similar surface functionalization. Our innovation is based on a noninvasive, synthetic protocol for graphene functionalization that goes beyond the ill-defined oxidation-reduction methods, allowing a definite control of the surface properties.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 13.942
Times cited: 69
DOI: 10.1021/nn305313q
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“Light-induced selective deposition of Au nanoparticles on single-wall carbon nanotubes”. Quintana M, Ke X, Van Tendeloo G, Meneghetti M, Bittencourt C, Prato M, ACS nano 4, 6105 (2010). http://doi.org/10.1021/nn101183y
Abstract: Novel applications of single-walled carbon nanotubes (SWNT) rely on the development of new strategies to make them easier to handle without affecting their structural properties. In this work, we have selectively deposited Au nanoparticles (Au NP) on SWNT assisted by UV light irradiation. XPS analysis and UV-vis spectroscopy indicate that the deposition occurs at the defects generated after oxidation of the SWNT. By addition of n-dodecylthiol, the separation of oxidized tubes with Au NP (Au-ox-SWNT) from tubes devoid of Au NP (bare tubes, b-SWNT) was achieved. Raman and UV-vis-NIR spectra indicate that UV irradiation induces a faster nucleation of Au NP on metallic SWNT. This new technique can be useful for the preparation of nanohybrid composites with enhanced properties, as increased thermal stability, and to obtain purified SWNT.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 13.942
Times cited: 26
DOI: 10.1021/nn101183y
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“Measuring point defect density in individual carbon nanotubes using polarization-dependent X-ray microscopy”. Felten A, Gillon X, Gulas M, Pireaux J-J, Ke X, Van Tendeloo G, Bittencourt C, Najafi E, Hitchcock AP, ACS nano 4, 4431 (2010). http://doi.org/10.1021/nn1002248
Abstract: The presence of defects in carbon nanotubes strongly modifies their electrical, mechanical, and chemical properties. It was long thought undesirable, but recent experiments have shown that introduction of structural defects using ion or electron irradiation can lead to novel nanodevices. We demonstrate a method for detecting and quantifying point defect density in individual carbon nanotubes (CNTs) based on measuring the polarization dependence (linear dichroism) of the C 1s → π* transition at specific locations along individual CNTs with a scanning transmission X-ray microscope (STXM). We show that STXM can be used to probe defect density in individual CNTs with high spatial resolution. The quantitative relationship between ion dose, nanotube diameter, and defect density was explored by purposely irradiating selected sections of nanotubes with kiloelectronvolt (keV) Ga+ ions. Our results establish polarization-dependent X-ray microscopy as a new and very powerful characterization technique for carbon nanotubes and other anisotropic nanostructures.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 13.942
Times cited: 26
DOI: 10.1021/nn1002248
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“Surface-Facet-Dependent Phonon Deformation Potential in Individual Strained Topological Insulator Bi2Se3 Nanoribbons”. Yan Y, Zhou X, Jin H, Li C-Z, Ke X, Van Tendeloo G, Liu K, Yu D, Dressel M, Liao Z-M, ACS nano 9, 10244 (2015). http://doi.org/10.1021/acsnano.5b04057
Abstract: Strain is an important method to tune the properties of topological insulators. For example, compressive strain can induce superconductivity in Bi2Se3 bulk material. Topological insulator nanostructures are the superior candidates to utilize the unique surface states due to the large surface to volume ratio. Therefore, it is highly desirable to monitor the local strain effects in individual topological insulator nanostructures. Here, we report the systematical micro-Raman spectra of single strained Bi2Se3 nanoribbons with different thicknesses and different surface facets, where four optical modes are resolved in both Stokes and anti-Stokes Raman spectral lines. A striking anisotropy of the strain dependence is observed in the phonon frequency of strained Bi2Se3 nanoribbons grown along the ⟨112̅0⟩ direction. The frequencies of the in-plane Eg2 and out-of-plane A1g1 modes exhibit a nearly linear blue-shift against bending strain when the nanoribbon is bent along the ⟨112̅0⟩ direction with the curved {0001} surface. In this case, the phonon deformation potential of the Eg2 phonon for 100 nm-thick Bi2Se3 nanoribbon is up to 0.94 cm–1/%, which is twice of that in Bi2Se3 bulk material (0.52 cm–1/%). Our results may be valuable for the strain modulation of individual topological insulator nanostructures.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 13.942
Times cited: 14
DOI: 10.1021/acsnano.5b04057
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“Photovoltaic effect and evidence of carrier multiplication in graphene vertical homojunctions with asymmetrical metal contacts”. Chen JJ, Wang Q, Meng J, Ke X, Van Tendeloo G, Bie YQ, Liu J, Liu K, Liao ZM, Sun D, Yu D;, ACS nano 9, 8851 (2015). http://doi.org/10.1021/acsnano.5b02356
Abstract: Graphene exhibits exciting potentials for high-speed wideband photodetection and high quantum efficiency solar energy harvest because of its broad spectral absorption, fast photoelectric response, and potential carrier multiplication. Although photocurrent can be generated near a metalgraphene interface in lateral devices, the photoactive area is usually limited to a tiny one-dimensional line-like interface region. Here, we report photoelectric devices based on vertical graphene two-dimensional homojunction, which is fabricated via vertically stacking four graphene monolayers with asymmetric metal contacts. The devices show excellent photovoltaic output with excitation wavelength ranging from visible light to mid-infrared. The wavelength dependence of the internal quantum efficiency gives direct evidence of the carrier multiplication effect in graphene. The simple fabrication process, easy scale-up, large photoresponsive active area, and broadband response of the vertical graphene device are very promising for practical applications in optoelectronics and photovoltaics.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 13.942
Times cited: 11
DOI: 10.1021/acsnano.5b02356
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“Study of the interface between rhodium and carbon nanotubes”. Suarez-Martinez I, Ewels CP, Ke X, Van Tendeloo G, Thiess S, Drube W, Felten A, Pireaux J-J, Ghijsen J, Bittencourt C, ACS nano 4, 1680 (2010). http://doi.org/10.1021/nn9015955
Abstract: X-ray photoelectron spectroscopy at 3.5 keV photon energy, in combination with high-resolution transmission electron microscopy, is used to follow the formation of the interface between rhodium and carbon nanotubes. Rh nucleates at defect sites, whether initially present or induced by oxygen-plasma treatment. More uniform Rh cluster dispersion is observed on plasma-treated CNTs. Experimental results are compared to DFT calculations of small Rh clusters on pristine and defective graphene. While Rh interacts as strongly with the carbon as Ti, it is less sensitive to the presence of oxygen, suggesting it as a good candidate for nanotube contacts.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 13.942
Times cited: 26
DOI: 10.1021/nn9015955
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“Tailoring ZnSe-CdSe colloidal quantum dots via cation exchange : from core/shell to alloy nanocrystals”. Groeneveld E, Witteman L, Lefferts M, Ke X, Bals S, Van Tendeloo G, de Mello Donega C, ACS nano 7, 7913 (2013). http://doi.org/10.1021/nn402931y
Abstract: We report a study of Zn2+ by Cd2+ cation exchange (CE) in colloidal ZnSe nanocrystals (NCs). Our results reveal that CE in ZnSe NCs is a thermally activated isotropic process. The CE efficiency (i.e., fraction of Cd2+ ions originally in solution, Cdsol, that is incorporated in the ZnSe NC) increases with temperature and depends also on the Cdsol/ZnSe ratio. Interestingly, the reaction temperature can be used as a sensitive parameter to tailor both the composition and the elemental distribution profile of the product (Zn,Cd)Se NCs. At 150 °C ZnSe/CdSe core/shell hetero-NCs (HNCs) are obtained, while higher temperatures (200 and 220 °C) produce (Zn1xCdx)Se gradient alloy NCs, with increasingly smoother gradients as the temperature increases, until homogeneous alloy NCs are obtained at T ≥ 240 °C. Remarkably, sequential heating (150 °C followed by 220 °C) leads to ZnSe/CdSe core/shell HNCs with thicker shells, rather than (Zn1xCdx)Se gradient alloy NCs. Thermal treatment at 250 °C converts the ZnSe/CdSe core/shell HNCs into (Zn1xCdx)Se homogeneous alloy NCs, while preserving the NC shape. A mechanism for the cation exchange in ZnSe NCs is proposed, in which fast CE takes place at the NC surface, and is followed by relatively slower thermally activated solid-state cation diffusion, which is mediated by Frenkel defects. The findings presented here demonstrate that cation exchange in colloidal ZnSe NCs provides a very sensitive tool to tailor the nature and localization regime of the electron and hole wave functions and the optoelectronic properties of colloidal ZnSeCdSe NCs.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 13.942
Times cited: 153
DOI: 10.1021/nn402931y
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“Electronic Coupling between Graphene and Topological Insulator Induced Anomalous Magnetotransport Properties”. Zhang L, Lin B-C, Wu Y-F, Wu H, Huang T-W, Chang C-R, Ke X, Kurttepeli M, Tendeloo GV, Xu J, Yu D, Liao Z-M, ACS nano 11, 6277 (2017). http://doi.org/10.1021/acsnano.7b02494
Abstract: It has been theoretically proposed that the spin textures of surface states in a topological insulator can be directly transferred to graphene by means of the proximity effect, which is very important for realizing the two-dimensional topological insulator based on graphene. Here we report the anomalous magnetotransport properties of graphene-topological insulator Bi2Se3 heterojunctions, which are sensitive to the electronic coupling between graphene and the topological surface state. The coupling between the p_z orbitals of graphene and the p orbitals of the surface states on the Bi2Se3 bottom surface can be enhanced by applying a perpendicular negative magnetic field, resulting in a giant negative magnetoresistance at the Dirac point up to about -91%. Obvious resistances dip in the transfer curve at the Dirac point is also observed in the hybrid devices, which is consistent with theoretical predictions of the distorted Dirac bands with nontrivial spin textures inherited from the Bi2Se3 surface states.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 13.942
Times cited: 12
DOI: 10.1021/acsnano.7b02494
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Ke X (2010) From top-down to bottom-up : from carbon nanotubes to nanodevices. Antwerpen
Keywords: Doctoral thesis; Electron microscopy for materials research (EMAT)
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