1. |
- Lu, Jun, 1962-, et al.
(author)
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Tin+1Cn MXenes with fully saturated and thermally stable Cl terminations
- 2019
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In: Nanoscale Advances. - : Royal Society of Chemistry. - 2516-0230. ; 1:9, s. 3680-3685
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Journal article (peer-reviewed)abstract
- MXenes are a rapidly growing family of 2D materials that exhibit a highly versatile structure and composition, allowing for significant tuning of the materials properties. These properties are, however, ultimately limited by the surface terminations, which are typically a mixture of species, including F and O that are inherent to the MXene processing. Other and robust terminations are lacking. Here, we apply high-resolution scanning transmission electron microscopy (STEM), corresponding image simulations and first-principles calculations to investigate the surface terminations on MXenes synthesized from MAX phases through Lewis acidic melts. The results show that atomic Cl terminates the synthesized MXenes, with mere residual presence of other termination species. Furthermore, in situ STEM-electron energy loss spectroscopy (EELS) heating experiments show that the Cl terminations are stable up to 750 degrees C. Thus, we present an attractive new termination that widely expands the MXenes functionalization space and enables new applications.
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2. |
- Ding, Haoming, et al.
(author)
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Synthesis of MAX phases Nb2CuC and Ti2(Al0.1Cu0.9)N by A-site replacement reaction in molten salts
- 2019
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In: Materials Research Letters. - : Taylor & Francis. - 2166-3831. ; 7:12, s. 510-516
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Journal article (peer-reviewed)abstract
- New MAX phases Ti2(AlxCu1−x)N and Nb2CuC were synthesized by A-site replacement by reacting Ti2AlN and Nb2AlC, respectively, with CuCl2 or CuI molten salt. X-ray diffraction, scanning electron microscopy, and atomically resolved scanning transmission electron microscopy showed complete A-site replacement in Nb2AlC, which lead to the formation of Nb2CuC. However, the replacement of Al in Ti2AlN phase was only close to complete at Ti2(Al0.1Cu0.9)N. Density-functional theory calculations corroborated the structural stability of Nb2CuC and Ti2CuN phases. Moreover, the calculated cleavage energy in these Cu-containing MAX phases are weaker than in their Al-containing counterparts.The preparation of MAX phases Nb2CuC and Ti2(Al0.1Cu0.9)N were realized by A-site replacement in Ti2AlN and Nb2AlN, respectively.
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3. |
- Halim, Joseph, 1985-, et al.
(author)
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Synthesis of Two-Dimensional Nb1.33C (MXene) with Randomly Distributed Vacancies by Etching of the Quaternary Solid Solution (Nb2/3Sc1/3)2AlC MAX Phase
- 2018
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In: ACS Applied Nano Materials. - : American Chemical Society (ACS). - 2574-0970. ; 1:6, s. 2455-2460
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Journal article (peer-reviewed)abstract
- Introducing point defects in two-dimensional (2D) materials can alter or enhance their properties. Here, we demonstrate how etching a laminated (Nb2/3Sc1/3)2AlC MAX phase (solid solution) of both the Sc and Al atoms results in a 2D Nb1.33C material (MXene) with a large number of vacancies and vacancy clusters. This method is applicable to any quaternary, or higher, MAX phase, wherein one of the transition metals is more reactive than the other and could be of vital importance in applications such as catalysis and energy storage. We also report, for the first time, on the existence of solid solution (Nb2/3Sc1/3)3AlC2 and (Nb2/3Sc1/3)4AlC3 phases.
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4. |
- Hsiao, Ching-Lien, et al.
(author)
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Curved-Lattice Epitaxial Growth of InxAl1-xN Nanospirals with Tailored Chirality
- 2015
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In: Nano letters (Print). - : American Chemical Society (ACS). - 1530-6984 .- 1530-6992. ; 15:1, s. 294-300
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Journal article (peer-reviewed)abstract
- Chirality, tailored by external morphology and internal composition, has been realized by controlled curved-lattice epitaxial growth (CLEG) of uniform coatings of single-crystalline InxAl1-xN nanospirals. The nanospirals are formed by sequentially stacking segments of curved nanorods on top of each other, where each segment is incrementally rotated around the spiral axis. By controlling the growth rate, segment length, rotation direction, and incremental rotation angle, spirals are tailored to predetermined handedness, pitch, and height. The curved morphology of the segments is a result of a lateral compositional gradient across the segments while maintaining a preferred crystallographic growth direction, implying a lateral gradient in optical properties as well. Left- and right-handed nanospirals, tailored with 5 periods of 200 nm pitch, as confirmed by scanning electron microscopy, exhibit uniform spiral diameters of ~80 nm (local segment diameters of ~60 nm) with tapered hexagonal tips. High resolution electron microscopy, in combination with nanoprobe energy dispersive X-ray spectroscopy and valence electron energy loss spectroscopy, show that individual nanospirals consist of an In-rich core with ~15 nm-diameter hexagonal cross-section, comprised of curved basal planes. The core is surrounded by an Al-rich shell with a thickness asymmetry spiraling along the core. The ensemble nanospirals, across the 1 cm2 wafers, show high in-plane ordering with respect to shape, crystalline orientation, and direction of compositional gradient. Mueller matrix spectroscopic ellipsometry shows that the tailored chirality is manifested in the polarization state of light reflected off the CLEG nanospiral-coated wafers. In that, the polarization state is shown to be dependent on the handedness of the nanospirals and the wavelength of the incident light in the ultraviolet-visible region.
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5. |
- Palisaitis, Justinas, 1983-, et al.
(author)
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On the Structural Stability of MXene and the Role of Transition Metal Adatoms
- 2018
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In: Nanoscale. - : Royal Society of Chemistry. - 2040-3364 .- 2040-3372. ; 10:23, s. 10850-10855
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Journal article (peer-reviewed)abstract
- In the present communication, the atomic structure and coordination of surface adsorbed species on Nb2C MXene is investigated over time. In particular, the influence of the Nb adatoms on the structural stability and oxidation behavior of the MXene is addressed. This investigation is based on plan-view geometry observations of single Nb2C MXene sheets by a combination of atomic-resolution scanning transmission electron microscopy (STEM), electron energy loss spectroscopy (EELS) and STEM image simulations.
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6. |
- Dobrovolskiy, Alexander, et al.
(author)
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Effects of Polytypism on Optical Properties and Band Structure ofIndividual Ga(N)P Nanowires from Correlative Spatially Resolved Structural and Optical Studies
- 2015
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In: Nano letters (Print). - : American Chemical Society (ACS). - 1530-6984 .- 1530-6992. ; 15:6, s. 4052-4058
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Journal article (peer-reviewed)abstract
- III-V semiconductor nanowires (NWs) have gained significant interest as building blocks in novel nanoscale devices. The one-dimensional (1D) nanostructure architecture allows one to extend band structure engineering beyond quantum confinement effects by utilizing formation of different crystal phases that are thermodynamically unfavorable in bulk materials. It is therefore of crucial importance to understand the influence of variations in the NWs crystal structure on their fundamental physical properties. In this work we investigate effects of structural polytypism on the optical properties of gallium phosphide and GaP/GaNP core/shell NW structures by a correlative investigation on the structural and optical properties of individual NWs. The former is monitored by transmission electron microscopy, whereas the latter is studied via cathodoluminescence (CL) mapping. It is found that structural defects, such as rotational twins in zinc blende (ZB) GaNP, have detrimental effects on light emission intensity at low temperatures by promoting nonradiative recombination processes. On the other hand, formation of the wurtzite (WZ) phase does not notably affect the CL intensity neither in GaP nor in the GaNP alloy. This suggests that zone folding in WZ GaP does not enhance its radiative efficiency, consistent with theoretical predictions. We also show that the change in the lattice structure have negligible effects on the bandgap energies of the GaNP alloys, at least within the range of the investigated nitrogen compositions of <2%. Both WZ and ZB GaNP are found to have a significantly higher efficiency of radiative recombination as compared with that in parental GaP, promising for potential applications of GaNP NWs as efficient nanoscale light emitters within the desirable amber-red spectral range.
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7. |
- Filippov, Stanislav, et al.
(author)
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Strongly polarized quantum-dot-like light emitters embedded in GaAs/GaNAs core/shell nanowires
- 2016
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In: Nanoscale. - : Royal Society of Chemistry. - 2040-3364 .- 2040-3372. ; 8:35, s. 15939-15947
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Journal article (peer-reviewed)abstract
- Recent developments in fabrication techniques and extensive investigations of the physical properties of III-V semiconductor nanowires (NWs), such as GaAs NWs, have demonstrated their potential for a multitude of advanced electronic and photonics applications. Alloying of GaAs with nitrogen can further enhance the performance and extend the device functionality via intentional defects and heterostructure engineering in GaNAs and GaAs/GaNAs coaxial NWs. In this work, it is shown that incorporation of nitrogen in GaAs NWs leads to formation of three-dimensional confining potentials caused by short-range fluctuations in the nitrogen composition, which are superimposed on long-range alloy disorder. The resulting localized states exhibit a quantum-dot like electronic structure, forming optically active states in the GaNAs shell. By directly correlating the structural and optical properties of individual NWs, it is also shown that formation of the localized states is efficient in pure zinc-blende wires and is further facilitated by structural polymorphism. The light emission from these localized states is found to be spectrally narrow (similar to 50-130 mu eV) and is highly polarized (up to 100%) with the preferable polarization direction orthogonal to the NW axis, suggesting a preferential orientation of the localization potential. These properties of self-assembled nano-emitters embedded in the GaNAs-based nanowire structures may be attractive for potential optoelectronic applications.
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8. |
- Folkenant, Matilda, et al.
(author)
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Structure and properties of Cr–C/Ag films deposited by magnetron sputtering
- 2015
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In: Surface & Coatings Technology. - : Elsevier. - 0257-8972 .- 1879-3347. ; 281, s. 184-192
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Journal article (peer-reviewed)abstract
- Cr–C/Ag thin films with 0–14 at.% Ag have been deposited by magnetron sputtering from elemental targets. The samples were analyzed by X-ray diffraction, transmission electron microscopy, X-ray photoelectron spectroscopy (XPS) and scanning electron microscopy (SEM) to study their structure and chemical bonding. A complex nanocomposite structure consisting of three phases; nanocrystalline Ag, amorphous CrCx and amorphous carbon is reported. The carbon content in the amorphous carbide phase was determined to be 32–33 at.% C, independent of Ag content. Furthermore, SEM and XPS results showed higher amounts of Ag on the surface compared to the bulk. The hardness and Young's modulus were reduced from 12 to 8 GPa and from 270 to 170 GPa, respectively, with increasing Ag content. The contact resistance was found to decrease with Ag addition, with the most Ag rich sample approaching the values of an Ag reference sample. Initial tribological tests gave friction coefficients in the range of 0.3 to 0.5, with no clear trends. Annealing tests show that the material is stable after annealing at 500 °C for 1 h, but not after annealing at 800 °C for 1 h. In combination, these results suggest that sputtered Cr–C/Ag films could be potentially applicable for electric contact applications.
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9. |
- Karlsson, Linda, et al.
(author)
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Residue reduction and intersurface interaction on single graphene sheets
- 2016
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In: Carbon. - : Pergamon Press. - 0008-6223 .- 1873-3891. ; 100, s. 345-350
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Journal article (peer-reviewed)abstract
- Large regions of pristine graphene are essential to applications which rely on the ideal graphene properties. Common methods for transferring chemical vapour deposition grown graphene to suitable substrates leaves metal oxide particles and poly(methyl methacrylate) (PMMA) residues on opposing surfaces, which degrade the properties. A common method to reduce the residues include annealing in vacuum or in argon, however, residues remain on the graphene sheet. The present investigation reports on the metal oxide particle ripening and PMMA decomposition on a single graphene sheet during in-situ annealing up to 1300 degrees C in a transmission electron microscope. It is shown that the PMMA residues are increasingly reduced at elevated temperatures although the reduction is strongly correlated to the metal oxide particle coverage on the opposing graphene surface. This is shown to occur as a consequence of an electrostatic interaction between the residues and that this prevents the establishment of large clean areas. (C) 2016 Elsevier Ltd. All rights reserved.
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10. |
- Petruhins, Andrejs, 1987-
(author)
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Synthesis and characterization of magnetic nanolaminated carbides
- 2018
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Doctoral thesis (other academic/artistic)abstract
- MAX phases are a group of nanolaminated ternary carbides and nitrides, with a composition expressed by the general formula Mn+1AXn (? = 1 − 3), where M is a transition metal, A is an A-group element, and X is carbon and/or nitrogen. MAX phases have attracted interest due to their unique combination of metallic and ceramic properties, related to their inherently laminated structure of a transition metal carbide (Mn+1Xn) layer interleaved by an A-group metal layer.This Thesis explores synthesis and characterization of magnetic MAX phases, where the A-group element is gallium (Ga). Due to the low melting point of Ga (T = 30 °C), conventional thin film synthesis methods become challenging, as the material is in liquid form at typical process temperatures. Development of existing methods has therefore been investigated, for reliable/reproducible synthesis routes, including sputtering from a liquid target, and resulting high quality material. Routes for minimizing trial-and-error procedures during optimization of thin film synthesis have also been studied, allowing faster identification of optimal deposition conditions and a simplified transfer of essential deposition parameters between different deposition systems.A large part of this Thesis is devoted towards synthesis of MAX phase thin films in the Cr-Mn-Ga-C system. First, through process development, thin films of Cr2GaC were deposited by magnetron sputtering. The films were epitaxial, however with small amount of impurity phase Cr3Ga, as confirmed by X-ray diffraction (XRD) measurements. The film structure was confirmed by scanning transmission electron microscopy (STEM) and the composition by energy dispersive X-ray spectroscopy (EDX) inside the TEM.Inspired by predictive ab initio calculations, the new MAX phase Mn2GaC was successfully synthesized in thin film form by magnetron sputtering. Structural parameters and magnetic properties were analysed. The material was found to have two magnetic transitions in the temperature range 3 K to 750 K, with a first order transition at around 214 K, going from non-collinear antiferromagnetic state at lower temperature to an antiferromagnetic state at higher temperature. The Neél temperature was determined to be 507 K, changing from an antiferromagnetic to a paramagnetic state. Above 800 K, Mn2GaC decomposes. Furthermore, magnetostrictive, magnetoresistive and magnetocaloric properties of the material were iv determined, among which a drastic change in lattice parameters upon the first magnetic transition was observed. This may be of interest for magnetocaloric applications.Synthesis of both Cr2GaC and Mn2GaC in thin film form opens the possibility to tune the magnetic properties through a solid solution on the transition metal site, by alloying the aforementioned Cr2GaC with Mn, realizing (Cr1-xMnx)2GaC. From a compound target with a Cr:Mn ratio of 1:1, thin films of (Cr0.5Mn0.5)2GaC were synthesized, confirmed by TEM-EDX. Optimized structure was obtained by deposition on MgO substrates at a deposition temperature of 600 ºC. The thin films were phase pure and of high structural quality, allowing magnetic measurements. Using vibrating sample magnetometry (VSM), it was found that (Cr0.5Mn0.5)2GaC has a ferromagnetic component in the temperature range from 30 K to 300 K, with the measured magnetic moment at high field decreasing by increasing temperature. The remanent moment and coercive field is small, 0.036 μB, and 12 mT at 30 K, respectively. Using ferromagnetic resonance spectroscopy, it was also found that the material has pure spin magnetism, as indicated by the determined spectroscopic splitting factor g = 2.00 and a negligible magnetocrystalline anisotropy energy.Fuelled by the recent discoveries of in-plane chemically ordered quaternary MAX phases, so called i-MAX phases, and guided by ab initio calculations, new members within this family, based on Cr and Mn, were synthesized by pressureless sintering methods, realizing (Cr2/3Sc1/3)2GaC and (Mn2/3Sc1/3)2GaC. Their structural properties were determined. Through these phases, the Mn content is the highest obtained in a bulk MAX phase to date.This work has further developed synthesis processes for sputtering from liquid material, for an optimized route to achieve thin films of controlled composition and a high structural quality. Furthermore, through this work, Mn has been added as a new element in the family of MAX phase elements. It has also been shown, that alloying with different content of Mn gives rise to varying magnetic properties in MAX phases. As a result of this Thesis, it is expected that the MAX phase family can be further expanded, with more members of new compositions and new properties.
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