| 1. |
- Aidas, Kestutis, et al.
(författare)
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The Dalton quantum chemistry program system
- 2014
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Ingår i: WIREs Computational Molecular Science. - : Wiley. - 1759-0876 .- 1759-0884. ; 4:3, s. 269-284
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Tidskriftsartikel (refereegranskat)abstract
- Dalton is a powerful general-purpose program system for the study of molecular electronic structure at the Hartree-Fock, Kohn-Sham, multiconfigurational self-consistent-field, MOller-Plesset, configuration-interaction, and coupled-cluster levels of theory. Apart from the total energy, a wide variety of molecular properties may be calculated using these electronic-structure models. Molecular gradients and Hessians are available for geometry optimizations, molecular dynamics, and vibrational studies, whereas magnetic resonance and optical activity can be studied in a gauge-origin-invariant manner. Frequency-dependent molecular properties can be calculated using linear, quadratic, and cubic response theory. A large number of singlet and triplet perturbation operators are available for the study of one-, two-, and three-photon processes. Environmental effects may be included using various dielectric-medium and quantum-mechanics/molecular-mechanics models. Large molecules may be studied using linear-scaling and massively parallel algorithms. Dalton is distributed at no cost from for a number of UNIX platforms.
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| 2. |
- Aquilante, Francesco, et al.
(författare)
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Cholesky decomposition techniques in electronic structure theory
- 2011
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Ingår i: Linear-Scaling Techniques in Computational Chemistry and Physics. - Dordrecht : Springer. - 9789048128525 ; , s. 301-304
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Bokkapitel (övrigt vetenskapligt/konstnärligt)abstract
- We review recently developed methods to efficiently utilize the Cholesky decomposition technique in electronic structure calculations. The review starts with a brief introduction to the basics of the Cholesky decomposition technique. Subsequently, examples of applications of the technique to ab inito procedures are presented. The technique is demonstrated to be a special type of a resolution-of-identity or density-fitting scheme. This is followed by explicit examples of the Cholesky techniques used in orbital localization, computation of the exchange contributionto the Fock matrix, in MP2, gradient calculations, and so-called method specific Cholesky decomposition. Subsequently, examples of calibration of the method with respect to computed total energies, excitation energies, and auxiliary basis set pruning are presented. In particular, it is demonstrated that the Cholesky method is an unbiased method to derive auxiliary basis sets. Furthermore, details of the implementational considerations are put forward and examples from a parallel Cholesky decomposition scheme is presented. Finally, an outlook and perspectives are presented, followed by a summary and conclusions section. We are of the opinion that the Cholesky decomposition method is a technique that has been overlooked for too long. We have just recently started to understand how to efficiently incorporate the method in existing ab initio programs. The full potential of the Cholesky technique has not yet been fully explored.
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| 5. |
- Böör, Katalin, et al.
(författare)
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On the growth kinetics, texture, microstructure, and mechanical properties of tungsten carbonitride deposited by chemical vapor deposition
- 2022
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Ingår i: Journal of Vacuum Science & Technology. A. Vacuum, Surfaces, and Films. - : American Institute of Physics (AIP). - 0734-2101 .- 1520-8559. ; 40:5
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Tidskriftsartikel (refereegranskat)abstract
- Tungsten carbonitride [W(C,N)] was deposited on cemented carbide substrates by chemical vapor deposition (CVD) in a hot-wall reactor using tungsten hexafluoride (WF6), acetonitrile (CH3CN), and hydrogen (H-2) as precursors. Tungsten carbides and nitrides with a hexagonal 6-WC type structure are generally difficult to obtain by CVD. Here, it was found that the combination of WF6 and CH3CN precursors enabled the deposition of W(C,N) coatings with a delta-WC type structure and columnar grains. A process window as a function of the deposition temperature and precursor partial pressures was determined to establish the conditions for the deposition of such coatings. Scanning electron microscopy, x-ray diffraction, electron backscatter diffraction, and elastic recoil detection analysis were used for the investigation of the coating thickness, microstructure, texture, and composition. From the investigation of the kinetics, it was concluded that the growth was mainly controlled by surface kinetics with an apparent activation energy of 77 kJ/mol, yielding an excellent step coverage. The partial reaction orders of the reactants together with their influence on the microstructure and coating composition was further used to gain a deeper understanding of the growth mechanism. Within the process window, the microstructure and the texture of the W(C,N) coatings could be tailored by the process parameters, enabling microstructural engineering with tuning of the mechanical properties of the W(C,N) coatings. The nanoindentation hardness (36.6-45.7 GPa) and elastic modulus (564-761 GPa) were found to be closely related to the microstructure.
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| 6. |
- Fondell, Mattis, 1984-, et al.
(författare)
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Phase control of iron oxides grown in nano-scale cauliflower structures: hematite, maghemite and magnetite
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Annan publikation (övrigt vetenskapligt/konstnärligt)abstract
- We demonstrate that iron oxide in the form of hematite, suitable as absorber in photoelectrochemical cells, can be produced by pulsed chemical vapour deposition. By choosing carbon monoxide or nitrogen as carrier gases in the process the phase and granularity of the grown material can be controlled. The choice of carrier gas a ect the decomposition rate of iron pentacarbonyl used as iron precursor. The iron oxide phase is also dependent on the chosen substrate, here fluorine doped tin oxide and crystalline silicon have been used. Regardless of the substrate nitrogen yields hematite, whereas carbon monoxide gives magnetite on Si and maghemite on fluorine doped tin oxide. A combination of Raman spectroscopy, X-ray di raction, and hard X-ray photoelectron spectroscopy were used for characterization of the crystalline phase and chemical composition in the films. Scanning electron microscopy were used to visualise the deposited films’ nano-structure reminiscent of a cauliflower.
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| 7. |
- Fondell, Mattis, et al.
(författare)
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Phase control of iron oxides grown in nano-scale structures on FTO and Si(100) : Hematite, maghemite and magnetite
- 2015
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Ingår i: Vacuum. - : Elsevier BV. - 0042-207X .- 1879-2715. ; 117, s. 85-90
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Tidskriftsartikel (refereegranskat)abstract
- We demonstrate that iron oxide in the form of hematite, suitable as absorption material in photo-electrochemical cells, can be produced by pulsed chemical vapour deposition. By choosing carbon monoxide or nitrogen as carrier gases in the process the phase and granularity of the grown material can be controlled. The choice of carrier gas affect the decomposition rate of iron pentacarbonyl used as iron precursor. The iron oxide phase is also dependent on the chosen substrate, here fluorine doped tin oxide and crystalline silicon have been used. Regardless of the substrate nitrogen yields hematite, whereas carbon monoxide gives, magnetite on Si and maghemite on fluorine doped tin oxide. A combination of Raman spectroscopy, X-ray diffraction, and hard X-ray photoelectron spectroscopy were used for characterization of the crystalline phase and chemical composition in the films. Scanning electron microscopy were used to visualise the deposited films' nano-structure.
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| 8. |
- Fondell, Mattis, 1984-, et al.
(författare)
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Temperature Induced Diffusion of Sn and Si in Hematite and Implications for Photocatalytic Water Splitting Applications
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Annan publikation (övrigt vetenskapligt/konstnärligt)abstract
- The performance of Hematite (α-Fe2O3) for the water oxidation step in solar hydrogen production is dependent upon annealing of the material. In this study, these effects are investigated in terms of temperature induced diffusion of Sn and Si from the substrate into thin films of hematite by using hard X-ray photoelectron spectroscopy (HAXPES). Here, HAXPES is used for the first time to characterize a buried interface between a conducting substrate and a nanostructured thin film overlayer by diffusion upon annealing. This process is prototypical for the large class of photoelectrochemical devices that uses indium and fluorine doped tin oxide as substrates where the device is subsequently annealed. Indeed, we observe that: diffusion of Sn and Si is significant, already at 550 °C; the photocatalytic efficiency of the hematite films increased, from low values to 0.23 mA/cm2; annealing in air preserves the hematite phase, while annealing in vacuum induces a phase transition into magnetite, which impairs the photocatalytic performance. The increase in efficiency is explained in terms of an improvement of the quantum efficiency of the oxygen evolution reaction accompanied by a slight improvement in charge carrier transport.
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| 10. |
- von Fieandt, Linus, et al.
(författare)
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Chemical vapor deposition of TiN on transition metal substrates
- 2018
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Ingår i: Surface and Coatings Technology. - : Elsevier BV. - 0257-8972 .- 1879-3347. ; 334, s. 373-383
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Tidskriftsartikel (refereegranskat)abstract
- The growth of chemical vapor deposited TiN from a reaction gas mixture of TiCl 4 , N 2 and H 2 was investigated on three different transition metal substrates: Fe, Co and Ni at deposition temperatures ranging from 850 °C to 950 °C. The interactions between the substrate metals and the gas phase were investigated using thermodynamic calculations. The TiN coatings were characterized by scanning electron microscopy, scanning transmission electron microscopy, X-ray diffraction, energy dispersive X-ray spectroscopy and transmission Kikuchi diffraction. Chemical vapor deposition (CVD) of TiN on Co substrates resulted in dense, columnar coatings of single phase TiN. The activation energy for TiN deposition on Co was determined to be 90 kJ/mol. CVD of TiN on Fe substrates caused severe substrate corrosion by the formation of gaseous FeCl x . Due to the substrate corrosion, the activation energy could not be determined. Furthermore, it was found that CVD of TiN on Ni substrates produced a phase mixture of TiN and Ni 3 Ti. Formation of Ni 3 Ti could be minimized by decreasing the H 2 partial pressure and increasing the N 2 partial pressure. Deposition on Ni yielded two different activation energies, 40 kJ/mol in the temperature interval 850 °C to 900 °C and 165 kJ/mol in the interval 900 °C to 950 °C. This is an indication of two different types of process control, which were identified as Ni diffusion into the growing film and a gas phase processes. The results of the present study showed that CVD of TiN on a cemented carbide using Fe and Ni in the binder phase, must be optimized in order to avoid corrosion or unwanted phases. Methods to achieve this are presented in this paper.
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