| 1. |
- Högberg, Hans, et al.
(författare)
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Reactive sputtering of CSx thin solid films using CS2 as precursor
- 2020
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Ingår i: Vacuum. - : PERGAMON-ELSEVIER SCIENCE LTD. - 0042-207X .- 1879-2715. ; 182
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Tidskriftsartikel (refereegranskat)abstract
- We deposit CSx thin solid films by reactive direct current magnetron sputtering of a C target in an argon plasma, using carbon disulfide (CS2) as a precursor to film growth. We investigate the influence of the partial pressure of the CS2 vapor introduced into the plasma on the composition, the chemical bonding structure, the structural, and the mechanical properties as determined by x-ray photoelectron spectroscopy (XPS), Raman spectroscopy, scanning electron microscopy (SEM), and nanoindentation for films deposited at 150 and 300 degrees C. The Raman and the XPS results indicate that S atoms are incorporated in mostly sp(2) bonded C network. These results agree with previous ab-initio theoretical findings obtained by modeling of the CSx compound by the Synthetic Growth Concept. The microstructure of the films as well as the results of their Raman characterization and the nano mechanical testing results all point out that with the increasing S content some spa bonding is admixed in the predominantly sp(2) bonded CSx network, leading to typical amorphous structure with short and interlocked graphene-like planes for S contents between 2% and 8%. We conclude that CSx thin solid films deposited by using CS2 as a precursor would be CSx films deposited at low temperature of similar to 150 degrees C and with an S content in the region of 6 at.% may be interesting candidates for applications as hard/elastic protective coatings.
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| 2. |
- Kakanakova-Gueorguieva, Anelia, et al.
(författare)
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MOCVD of AlN on epitaxial graphene at extreme temperatures
- 2021
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Ingår i: CrystEngComm. - : ROYAL SOC CHEMISTRY. - 1466-8033. ; 23:2, s. 385-390
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Tidskriftsartikel (refereegranskat)abstract
- The initial stages of metal organic chemical vapor deposition (MOCVD) of AlN on epitaxial graphene at temperatures in excess of 1200 degrees C have been rationalized. The use of epitaxial graphene, in conjunction with high deposition temperatures, can deliver on the realization of nanometer thin AlN whose material quality is characterized by the appearance of luminescent centers with narrow spectral emission at room temperature. It has been elaborated, based on our previous comprehensive ab initio molecular dynamics simulations, that the impact of graphene on AlN growth consists in the way it promotes dissociation of the trimethylaluminum, (CH3)(3)Al, precursor with subsequent formation of Al adatoms during the initial stages of the deposition process. The high deposition temperatures ensure adequate surface diffusion of the Al adatoms which is an essential factor in material quality enhancement. The role of graphene in intervening with the dissociation of another precursor, trimethylgallium, (CH3)(3)Ga, has accordingly been speculated by presenting a case of propagation of ultrathin GaN of semiconductor quality. A lower deposition temperature of 1100 degrees C in this case has better preserved the structural integrity of epitaxial graphene. Breakage and decomposition of the graphene layers has been deduced in the case of AlN deposition at temperatures in excess of 1200 degrees C.
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| 3. |
- Kakanakova-Gueorguieva, Anelia, et al.
(författare)
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Nanoscale phenomena ruling deposition and intercalation of AlN at the graphene/SiC interface
- 2020
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Ingår i: Nanoscale. - : ROYAL SOC CHEMISTRY. - 2040-3364 .- 2040-3372. ; 12:37, s. 19470-19476
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Tidskriftsartikel (refereegranskat)abstract
- The possibility for kinetic stabilization of prospective 2D AlN was explored by rationalizing metal organic chemical vapor deposition (MOCVD) processes of AlN on epitaxial graphene. From the wide range of temperatures which can be covered in the same MOCVD reactor, the deposition was performed at the selected temperatures of 700, 900, and 1240 degrees C. The characterization of the structures by atomic force microscopy, electron microscopy and Raman spectroscopy revealed a broad range of surface nucleation and intercalation phenomena. These phenomena included the abundant formation of nucleation sites on graphene, the fragmentation of the graphene layers which accelerated with the deposition temperature, the delivery of excess precursor-derived carbon adatoms to the surface, as well as intercalation of sub-layers of aluminum atoms at the graphene/SiC interface. The conceptual understanding of these nanoscale phenomena was supported by our previous comprehensiveab initiomolecular dynamics (AIMD) simulations of the surface reaction of trimethylaluminum, (CH3)(3)Al, precursor with graphene. A case of applying trimethylindium, (CH3)(3)In, precursor to epitaxial graphene was considered in a comparative way.
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| 4. |
- Schmidt, Susann, et al.
(författare)
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CF(x) thin solid films deposited by high power impulse magnetron sputtering: Synthesis and characterization
- 2011
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Ingår i: Surface & Coatings Technology. - : Elsevier. - 0257-8972 .- 1879-3347. ; 206:4, s. 646-653
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Tidskriftsartikel (refereegranskat)abstract
- Fluorine containing amorphous carbon films (CF(x), 0.16 andlt;= x andlt;= 0.35) have been synthesized by reactive high power impulse magnetron sputtering (HiPIMS) in an Ar/CF(4) atmosphere. The fluorine content of the films was controlled by varying the CF(4) partial pressure from 0 mPa to 110 mPa at a constant deposition pressure of 400 mPa and a substrate temperature of 110 degrees C. The films were characterized regarding their composition, chemical bonding and microstructure as well as mechanical properties by applying elastic recoil detection analysis, X-ray photoelectron spectroscopy, Raman spectroscopy, transmission electron microscopy, and nanoindentation. First-principles calculations were carried out to predict and explain F-containing carbon thin film synthesis and properties. By geometry optimizations and cohesive energy calculations the relative stability of precursor species including C(2), F(2) and radicals, resulting from dissociation of CF4, were established. Furthermore, structural defects, arising from the incorporation of F atoms in a graphene-like network, were evaluated. All as-deposited CF(x) films are amorphous. Results from X-ray photoelectron spectroscopy and Raman spectroscopy indicate a graphitic nature of CF(x) films with x andlt;= 0.23 and a polymeric structure for films with x andgt;= 0.26. Nanoindentation reveals hardnesses between similar to 1 GPa and similar to 16 GPa and an elastic recovery of up to 98%.
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| 5. |
- Schmidt, Susann, et al.
(författare)
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Reactive high power impulse magnetron sputtering of CFx thin films in mixed Ar/C4F4 and Ar/C4F8 discharges
- 2013
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Ingår i: Thin Solid Films. - : Elsevier. - 0040-6090 .- 1879-2731. ; 542, s. 21-30
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Tidskriftsartikel (refereegranskat)abstract
- The reactive high power impulse magnetron sputtering processes of carbon in argon/tetrafluoromethane (CF4) and argon/octafluorocyclobutane (c-C4F8) have been characterized. Amorphous carbon fluoride (CFx) films were synthesized at deposition pressure and substrate temperature of 400 mPa and 110 degrees C, respectively. The CFx film composition was controlled in the range of 0.15 andlt; x andlt; 0.35 by varying the partial pressure of the F-containing gases from 0 mPa to 110 mPa. The reactive plasma was studied employing time averaged positive ion mass spectrometry and the resulting thin films were characterized regarding their composition, chemical bonding and microstructure as well as mechanical properties by elastic recoil detection analysis, X-ray photoelectron spectroscopy, transmission electron microscopy, nanoindentation, and water droplet contact angle measurements, respectively. The experimental results were compared to results obtained by first-principles calculations based on density functional theory. The modeling of the most abundant precursor fragment from the dissociation of CF4 and C4F8 provided their relative stability, abundance, and reactivity, thus permitting to evaluate the role of each precursor during film growth. Positive ion mass spectrometry of both fluorine plasmas shows an abundance of CF+, C+, CF2+, and CF3+ (in this order) as corroborated by first-principles calculations. Only CF3+ exceeded the Ar+ signal in a CF4 plasma. Two deposition regimes are found depending on the partial pressure of the fluorine-containing reactive gas, where films with fluorine contents below 24 at.% exhibit a graphitic nature, whereas a polymeric structure applies to films with fluorine contents exceeding 27 at.%. Moreover, abundant precursors in the plasma are correlated to the mechanical response of the different CFx thin films. The decreasing hardness with increasing fluorine content can be attributed to the abundance of CF3+ precursor species, weakening the carbon matrix.
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| 6. |
- Schmidt, Susann, et al.
(författare)
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Reactive High Power Impulse Magnetron Sputtering of CFx Thin Films in Mixed Ar/CF4 and Ar/C4F8 Discharges
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Annan publikation (övrigt vetenskapligt/konstnärligt)abstract
- The reactive high power impulse magnetron sputtering (HiPIMS) processes of C in Ar/tetrafluoromethane CF4 and Ar/octafluorocyclobutane (c-C4F8) have been characterized. Amorphous carbon fluoride (CFx) films were synthesized at deposition pressure and substrate temperature of 400 mPa and 110 oC, respectively. The CFx film composition was controlled in the range of 0.15 < x < 0.35 by varying the partial pressure of the F-containing gases from 0 mPa to 110 mPa. The reactive plasma was studied employing time averaged positive ion mass spectrometry and the resulting thin films were characterized regarding their composition, chemical bonding and microstructure as well as mechanical properties by elastic recoil detection analysis, X-ray photoelectron spectroscopy, transmission electron microscopy, nanoindentation, and water droplet contact angle measurements, respectively. The experimental results were compared to results obtained by first-principles calculations based on density functional theory.The modeling of the most abundant precursor fragment from the dissociation of CF4 and C4F8 provided their relative stability, abundance, and reactivity, thus permitting to evaluate the role of each precursor during film growth. Positive ion mass spectrometry of both F plasmas show an abundance of CF+, C+, CF⁺₂, and CF⁺₃ (in this order) as corroborated by first-principles calculations. Only CF⁺₃ exceeded the Ar+ signal in a CF4 plasma. Two deposition regimes are found depending on the partial pressure of the F-containing reactive gas, where films with fluorine contents below 24 at% exhibit a graphitic nature, whereas a polymeric structure applies to films with fluorine contents exceeding 27 at%. Moreover, abundant precursors in the plasma are correlated to the mechanical response of the different CFx thin films. The decreasing hardness with increasing F content can be attributed to the abundance of CF⁺₃ precursor species, weakening the C matrix.
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| 7. |
- Alves Machado Filho, Manoel, et al.
(författare)
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Self-Induced Core–Shell InAlN Nanorods: Formation and Stability Unraveled by Ab Initio Simulations
- 2023
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Ingår i: ACS Nanoscience Au. - : American Chemical Society (ACS). - 2694-2496. ; 3:1, s. 84-93
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Tidskriftsartikel (refereegranskat)abstract
- By addressing precursor prevalence and energetics using the DFT-based synthetic growth concept (SGC), the formation mechanism of self-induced InAlN core–shell nanorods (NRs) synthesized by reactive magnetron sputter epitaxy (MSE) is explored. The characteristics of In- and Al-containing precursor species are evaluated considering the thermal conditions at a typical NR growth temperature of around 700 °C. The cohesive and dissociation energies of In-containing precursors are consistently lower than those of their Al-containing counterparts, indicating that In-containing precursors are more weakly bonded and more prone to dissociation. Therefore, In-containing species are expected to exhibit lower abundance in the NR growth environment. At increased growth temperatures, the depletion of In-based precursors is even more pronounced. A distinctive imbalance in the incorporation of Al- and In-containing precursor species (namely, AlN/AlN+, AlN2/AlN2+, Al2N2/Al2N2+, and Al2/Al2+ vs InN/InN+, InN2/InN2+, In2N2/In2N2+, and In2/In2+) is found at the growing edge of the NR side surfaces, which correlates well with the experimentally obtained core–shell structure as well as with the distinctive In-rich core and vice versa for the Al-rich shell. The performed modeling indicates that the formation of the core–shell structure is substantially driven by the precursors’ abundance and their preferential bonding onto the growing edge of the nanoclusters/islands initiated by phase separation from the beginning of the NR growth. The cohesive energies and the band gaps of the NRs show decreasing trends with an increment in the In concentration of the NRs’ core and with an increment in the overall thickness (diameter) of the NRs. These results reveal the energy and electronic reasons behind the limited growth (up to ∼25% of In atoms of all metal atoms, i.e., InxAl1–xN, x ∼ 0.25) in the NR core and may be qualitatively perceived as a limiting factor for the thickness of the grown NRs (typically <50 nm).
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| 8. |
- Bairagi, Samiran, et al.
(författare)
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Formation of quaternary Zn(AlxGa1−x)2O4 epilayers driven by thermally induced interdiffusion between spinel ZnGa2O4 epilayer and Al2O3 substrate
- 2023
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Ingår i: Materials Today Advances. - : Elsevier. - 2590-0498. ; 20
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Tidskriftsartikel (refereegranskat)abstract
- Zinc aluminogallate, Zn(AlxGa1−x)2O4 (ZAGO), a single-phase spinel structure, offers considerable potential for high-performance electronic devices due to its expansive compositional miscibility range between aluminum (Al) and gallium (Ga). Direct growth of high-quality ZAGO epilayers however remains problematic due to the high volatility of zinc (Zn). This work highlights a novel synthesis process for high-quality epitaxial quaternary ZAGO thin films on sapphire substrates, achieved through thermal annealing of a ZnGa2O4 (ZGO) epilayer on sapphire in an ambient air setting. In-situ annealing x-ray diffraction measurements show that the incorporation of Al in the ZGO epilayer commenced at 850 °C. The Al content (x) in ZAGO epilayer gradually increased up to around 0.45 as the annealing temperature was raised to 1100 °C, which was confirmed by transmission electron microscopy (TEM) and energy dispersive x-ray spectroscopy. X-ray rocking curve measurement revealed a small full width at half maximum value of 0.72 °, indicating the crystal quality preservation of the ZAGO epilayer with a high Al content. However, an epitaxial intermediate �–(AlxGa1−x)2O3 layer (� - AGO) was formed between the ZAGO and sapphire substrate. This is believed to be a consequence of the interdiffusion of Al and Ga between the ZGO thin film and sapphire substrate. Using density functional theory, the substitution cost of Ga in sapphire was determined to be about 0.5 eV lower than substitution cost of Al in ZGO. Motivated by this energetically favorable substitution, a formation mechanism of the ZAGO and AGO layers was proposed. Spectroscopic ellipsometry studies revealed an increase in total thickness of the film from 105.07 nm (ZGO) to 147.97 nm (ZAGO/AGO) after annealing to 1100 °C, which were corroborated using TEM. Furthermore, an observed increase in the direct (indirect) optical bandgap from 5.06 eV (4.7 eV) to 5.72 eV (5.45 eV) with an increasing Al content in the ZAGO layer further underpins the formation of a quaternary ZAGO alloy with a tunable composition.
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| 9. |
- Bakoglidis, Konstantinos, et al.
(författare)
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Self-Healing in Carbon Nitride Evidenced As Material Inflation and Superlubric Behavior
- 2018
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Ingår i: ACS Applied Materials and Interfaces. - : AMER CHEMICAL SOC. - 1944-8244 .- 1944-8252. ; 10:19, s. 16238-16243
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Tidskriftsartikel (refereegranskat)abstract
- All known materials wear under extended mechanical contacting. Superlubricity may present solutions, but is an expressed mystery in C-based materials. We report negative wear of carbon nitride films; a wear-less condition with mechanically induced material inflation at the nanoscale and friction coefficient approaching ultralow values (0.06). Superlubricity in carbon nitride is expressed as C-N bond breaking for reduced coupling between graphitic-like sheets and eventual N-2 desorption. The transforming surface layer acts as a solid lubricant, whereas the film bulk retains its high elasticity. The present findings offer new means for materials design at the atomic level, and for property optimization in wear-critical applications like magnetic reading devices or nanomachines.
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| 10. |
- Batista dos Santos, Renato, et al.
(författare)
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Electric-Field Control of Spin-Polarization and Semiconductor-to-Metal Transition in Carbon-Atom-Chain Devices
- 2017
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Ingår i: The Journal of Physical Chemistry C. - : AMER CHEMICAL SOC. - 1932-7447 .- 1932-7455. ; 121:46, s. 26125-26132
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Tidskriftsartikel (refereegranskat)abstract
- We propose hybrid molecular systems containing small carbon atomic chains interconnected by graphene-like flakes, theoretically predicted as true energy minima, as low-dimensional structures that may be useful in electronic devices at the limit of the atomic miniaturization. The effects of an external electric field applied along the direction of the carbon chains indicate that it is possible to control energy gap and spin polarization with sufficiently high strength, within the limit of the structural restoring of the systems. In this sense, by applying electric fields with magnitudes in the 1-5 V/nm range, we obtain semiconductor-to-metallic transitions for all odd-numbered carbon-chain systems proposed here. Furthermore, high-spin-to-low-spin transitions are determined for these systems as a function of the electric-field magnitude. In the case of the even-numbered carbon-chain systems, the overall electric field effect is pushing electron density near the Fermi level, leading to a gapless or metallic regime at 3.0 V/nm. An electric-field control of the spin-polarization of these latter systems is only achieved by doping the extremities of the graphene-like terminations with sulfur atoms. This finding, however, is beneficial for applications of these systems in spin controlled carbon-based devices connected by gold electrodes, even in the presence of a weak spin-orbit coupling.
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