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  • 1.
    Alvi, Sajid
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Jarzabek, Dariusz M.
    Department of Mechanics of Materials (ZMM), Institute of Fundamental Technological Research, Polish Academy of Sciences, 02-106 Warsaw, Poland.
    Gilzad Kohan, Mojtaba
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Hedman, Daniel
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Jenczyk, Piotr
    Department of Mechanics of Materials (ZMM), Institute of Fundamental Technological Research, Polish Academy of Sciences, 02-106 Warsaw, Poland.
    Natile, Marta Maria
    CNR—Institute of Condensed Matter Chemistry and Technologies for Energy (ICMATE), I-16149 Genoa, Italy. Department of Chemical Sciences, University of Padova, 35131 Padova, Italy.
    Vomiero, Alberto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Akhtar, Farid
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Synthesis and Mechanical Characterization of a CuMoTaWV High-Entropy Film by Magnetron Sputtering2020In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 12, no 18, p. 21070-21079Article in journal (Refereed)
    Abstract [en]

    Development of high-entropy alloy (HEA) films is a promising and cost-effective way to incorporate these materials of superior properties in harsh environments. In this work, a refractory high-entropy alloy (RHEA) film of equimolar CuMoTaWV was deposited on silicon and 304 stainless-steel substrates using DC-magnetron sputtering. A sputtering target was developed by partial sintering of an equimolar powder mixture of Cu, Mo, Ta, W, and V using spark plasma sintering. The target was used to sputter a nanocrystalline RHEA film with a thickness of ∼900 nm and an average grain size of 18 nm. X-ray diffraction of the film revealed a body-centered cubic solid solution with preferred orientation in the (110) directional plane. The nanocrystalline nature of the RHEA film resulted in a hardness of 19 ± 2.3 GPa and an elastic modulus of 259 ± 19.2 GPa. A high compressive strength of 10 ± 0.8 GPa was obtained in nanopillar compression due to solid solution hardening and grain boundary strengthening. The adhesion between the RHEA film and 304 stainless-steel substrates was increased on annealing. For the wear test against the E52100 alloy steel (Grade 25, 700–880 HV) at 1 N load, the RHEA film showed an average coefficient of friction (COF) and wear rate of 0.25 (RT) and 1.5 (300 °C), and 6.4 × 10–6 mm3/N m (RT) and 2.5 × 10–5 mm3/N m (300 °C), respectively. The COF was found to be 2 times lower at RT and wear rate 102 times lower at RT and 300 °C than those of 304 stainless steel. This study may lead to the processing of high-entropy alloy films for large-scale industrial applications.

  • 2.
    Alvi, Sajid
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science. Department of Physics, Chalmers University of Technology, SE‐412 96 Göteborg, Sweden.
    Milczarek, Michal
    Department of Mechanics of Materials (ZMM), Institute of Fundamental Technological Research, Polish Academy of Sciences, 02-106 Warsaw, Poland.
    Jarzabek, Dariusz M.
    Department of Mechanics of Materials (ZMM), Institute of Fundamental Technological Research, Polish Academy of Sciences, 02-106 Warsaw, Poland.
    Hedman, Daniel
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science. Research Center for Computational Design of Advanced Functional Materials, National Institute of Advanced Industrial Science and Technology (AIST), Central 2, 1‐1‐1 Umezono, Tsukuba, Ibaraki, 305‐8568 Japan; Center for Multidimensional Carbon Materials, Institute for Basic Science (IBS), Ulsan, 44919 Republic of Korea.
    Gilzad Kohan, Mojtaba
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Levintant-Zayonts, Neonila
    Department of Mechanics of Materials (ZMM), Institute of Fundamental Technological Research, Polish Academy of Sciences, 02-106 Warsaw, Poland.
    Vomiero, Alberto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science. Department of Molecular Sciences and Nanosystems, Ca' Foscari University of Venice, Via Torino 155, 30172 Mestre Venezia, Italy.
    Akhtar, Farid
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Enhanced mechanical, thermal and electrical properties of high‐entropy HfMoNbTaTiVWZr thin film metallic glass and its nitrides2022In: Advanced Engineering Materials, ISSN 1438-1656, E-ISSN 1527-2648, Vol. 24, no 9, article id 2101626Article in journal (Refereed)
    Abstract [en]

    The inception of high-entropy alloy promises to push the boundaries for new alloy design with unprecedented properties. This work reports entropy stabilisation of an octonary refractory, HfMoNbTaTiVWZr, high-entropy thin film metallic glass, and derived nitride films. The thin film metallic glass exhibited exceptional ductility of ≈60% strain without fracture and compression strength of 3 GPa in micro-compression, due to the presence of high density and strength of bonds. The thin film metallic glass shows thermal stability up to 750 °C and resistance to Ar-ion irradiation. Nitriding during film deposition of HfMoNbTaTiVWZr thin film of strong nitride forming refractory elements results in deposition of nanocrystalline nitride films with compressive strength, hardness, and thermal stability of up to 10 GPa, 18.7 GPa, and 950 °C, respectively. The high amount of lattice distortion in the nitride films leads to its insulating behaviour with electrical conductivity as low as 200 S cm−1 in the as-deposited film. The design and exceptional properties of the thin film metallic glass and derived nitride films may open up new avenues of development of bulk metallic glasses and the application of refractory-based high entropy thin films in structural and functional applications.

  • 3.
    Dobryden, Illia
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Steponavičiu̅tė, Medeina
    Institute of Chemistry, Vilnius University, LT-03225 Vilnius, Lithuania.
    Hedman, Daniel
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science. Center for Multidimensional Carbon Materials, Institute for Basic Science (IBS), Ulsan 44919, Republic of Korea.
    Klimkevičius, Vaidas
    Institute of Chemistry, Vilnius University, LT-03225 Vilnius, Lithuania.
    Makuška, Ričardas
    Institute of Chemistry, Vilnius University, LT-03225 Vilnius, Lithuania.
    Dėdinaitė, Andra
    KTH Royal Institute of Technology, School of Engineering Sciences in Chemistry, Biotechnology and Health, Engineering Pedagogics, SE-100 44 Stockholm, Sweden; RISE Research Institutes of Sweden, Division of Bioscience and Materials, SE-114 86 Stockholm, Sweden.
    Liu, Xiaoyan
    School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi’an 710062, China.
    Corkery, Robert W.
    KTH Royal Institute of Technology, School of Engineering Sciences in Chemistry, Biotechnology and Health, Department of Chemistry, Division of Surface and Corrosion Science, SE-100 44 Stockholm, Sweden.
    Claesson, Per Martin
    KTH Royal Institute of Technology, School of Engineering Sciences in Chemistry, Biotechnology and Health, Department of Chemistry, Division of Surface and Corrosion Science, SE-100 44 Stockholm, Sweden.
    Local Wear of Catechol-Containing Diblock Copolymer Layers: Wear Volume, Stick–Slip, and Nanomechanical Changes2021In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 125, no 38, p. 21277-21292Article in journal (Refereed)
    Abstract [en]

    Polymers containing catechol groups have gained a large interest, as they mimic an essential feature of mussel adhesive proteins that allow strong binding to a large variety of surfaces under water. This feature has made this class of polymers interesting for surface modification purposes, as layer functionalities can be introduced by a simple adsorption process, where the catechol groups should provide a strong anchoring to the surface. In this work, we utilize an AFM-based method to evaluate the wear resistance of such polymer layers in water and compare it with that offered by electrostatically driven adsorption. We pay particular attention to two block copolymer systems where the anchoring group in one case is an uncharged catechol-containing block and in the other case a positively charged and catechol-containing block. The wear resistance is evaluated in terms of wear volume, and here, we compare with data for similar copolymers with statistical distribution of the catechol groups. Monitoring of nanomechanical properties provides an alternative way of illustrating the effect of wear, and we use modeling to show that the stiffness, as probed by an AFM tip, of the soft layer residing on a hard substrate increases as the thickness of the layer decreases. The stick–slip characteristics are also evaluated.

  • 4.
    Feltrin, Ana Carolina
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Hedman, Daniel
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Akhtar, Farid
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Thermal properties and high-temperature ablation of high-entropy (Ti0.25V0.25Zr0.25Hf0.25)B2 coating on graphite substrateIn: Article in journal (Refereed)
  • 5.
    Feltrin, Ana Carolina
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Hedman, Daniel
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science. Center for Multidimensional Carbon Materials, Institute for Basic Science (IBS), Ulsan 44919, Republic of Korea.
    Akhtar, Farid
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Transformation of metastable dual-phase (Ti0.25V0.25Zr0.25Hf0.25)B2 to stable high-entropy single-phase boride by thermal annealing2021In: Applied Physics Letters, ISSN 0003-6951, E-ISSN 1077-3118, Vol. 119, no 16, article id 161905Article in journal (Refereed)
    Abstract [en]

    Transition metal borides have a unique combination of high melting point and high chemical stability and are suitable for high temperature applications (>2000 °C). A metastable dual-phase boride (Ti0.25V0.25Zr0.25Hf0.25)B2 with distinct two hexagonal phases and with an intermediate entropy formation ability of 87.9 (eV/atom)−1 as calculated via the density functional theory (DFT) was consolidated by pulsed current sintering. Thermal annealing of the sintered dual-phase boride at 1500 °C promoted the diffusion of metallic elements between the two boride phases leading to chemical homogenization and resulted in the stabilization of a single-phase high-entropy boride. Scanning electron microscopy, in situ high temperature x-ray diffraction, and simultaneous thermal analysis of the as-sintered and annealed high-entropy borides showed the homogenization of a dual-phase to a single-phase. The experimentally obtained single-phase structure was verified by DFT calculations using special quasirandom structures, which were further used for theoretical investigations of lattice distortions and mechanical properties. Experimentally measured mechanical properties of the single-phase boride showed improved mechanical properties with a hardness of 33.2 ± 2.1 GPa, an elastic modulus of 466.0 ± 5.9 GPa, and a fracture toughness of 4.1 ± 0.6 MPa m1/2.

  • 6.
    Hedman, Daniel
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    A Theoretical Study: The Connection between Stability of Single-Walled Carbon Nanotubes and Observed Products2017Licentiate thesis, comprehensive summary (Other academic)
    Abstract [en]

    Over the past 20 years’ researchers have tried to utilize the remarkable properties of single-walled carbon nanotubes (SWCNTs) to create new high-tech materials and devices, such as strong light-weight composites, efficient electrical wires and super-fast transistors. But the mass production of these materials and devices are still hampered by the poor uniformity of the produced SWCNTs. These are hollow cylindrical tubes of carbon where the atomic structure of the tube wall consists of just a single atomic layer of carbon atoms arranged in a hexagonal grid. For a SWCNT the orientation of the hexagonal grid making up the tube wall is what determines its properties, this orientation is known as the chirality of a SWCNT. As an example, tubes with certain chiralities will be electrically conductive while others having different chiralities will be semiconducting.

    Today’s large scale methods for producing SWCNTs, commonly known as growth of SWCNTs, gives products with a large spread of different chiralities. A mixture of chiralities will give products with a mixture of different properties. This is one of the major problems holding back the use of SWCNTs in future materials and devices. The ultimate goal is to achieve growth where the resulting product is uniform, meaning that all of the SWCNTs have the same chirality, a process termed chirality-specific growth. To achieve chirality-specific growth of SWCNTs requires us to obtain a better fundamental understanding about how they grow, both from an experimental and a theoretical point of view.

    This work focuses on theoretical studies of SWCNT properties and how they relate to the growth process, thereby giving us vital new information about how SWCNTs grow and taking us ever closer to achieving the ultimate goal of chirality-specific growth. In this thesis, an introduction to the field is given and the current state of the art experiments focusing on chirality-specific growth of SWCNTs are presented. A brief review of the current theoretical works and computer simulations related to growth of SWCNTs is also presented. The results presented in this thesis are obtained using first principle density functional theory. The first study shows a correlation between the stability of SWCNT-fragments and the observed products from experiments. Calculations confirm that in 84% of the investigated cases the chirality of experimental products matches the chirality of the most stable SWCNT-fragments (within 0.2 eV). Further theoretical calculations also reveal a previously unknown link between the stability of SWCNT-fragments and their length. The calculations show that at specific SWCNT-fragment lengths the most stable chirality changes. Thus, introducing the concept of a switching length for SWCNT stability. How these new results link to the existing understanding of SWCNT growth is discussed at the end of the thesis.

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  • 7.
    Hedman, Daniel
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Linking Stability of Single-Walled Carbon Nanotubes with Growth Products2017Conference paper (Other academic)
    Abstract [en]

    Many of the envisioned products and technologies using single-walled carbon nanotubes (SWCNTs) are only possible with a uniform product. Thus, control over the chirality during catalytical chemical vapor deposition (CCVD) growth of SWCNTs is necessary. Our highlighted works1,2 focuses on stabilities of SWCNTs and how that relates to growth, in order to reach the ultimate goal of chirality-specific growth. In ref.1 density functional theory (DFT) has been used to calculate the stability of SWCNT-fragments of all chiralities in the (n+m) = 8 to 18 series. The fragment stabilities are compare to the chiralities of actual CCVD products from all properly analysed experiments to date. The results show that in 84% of the cases the experimental products represent chiralities among the most stable SWCNT-fragments (within 0.2 eV) from the calculations. The analysed products from growth experiments show that diameters of SWCNTs are governed by the well-known relation to the size of the catalytic particle and that the specific chirality of SWCNT products are strongly dependent on the stability of the tubes within each series, suggesting thermodynamic control at the early stage of growth. Analysis of the relative energy show that for the lower series 8 to 10, zigzag SWCNTs are the most stable and for the higher series 11 to 18 the most stable chirality changes from zigzag to armchair. This switch in stability between armchair and zigzag chiralities is studied further in ref.2, where DFT was used to calculate the stability of armchair and zigzag SWCNTs and graphene nanoribbons (GNRs) of different lengths. The calculations show that the stability of armchair and zigzag tubes has different linear dependence with regard to their length, with switches in the most stable chirality occurring at specific lengths for each SWCNT-series. These dependencies are explained by competing edge and curvature energies. Within each series armchair nanotubes are the most stable at short lengths, while zigzag nanotubes are the most stable at long lengths, this sheds new light into why armchair and near-armchair tubes are the dominant product from CCVD growth, if templating is not used. Paradoxically, the stability of armchair nanotubes at short lengths favors their growth although zigzag nanotubes are more stable at long lengths, resulting in the production of the least stable SWCNTs.

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  • 8.
    Hedman, Daniel
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    On the Stability of Single-Walled Carbon Nanotubes and how it relates to Growth2017In: CCTN17: 12th International Symposium on Computational Challenges and Tools for Nanotubes, 2017Conference paper (Other academic)
    Abstract [en]

    Many envisioned products and technologies using single-walled carbon nanotubes (SWCNTs) are only possible with a uniform product. Thus, control over the chirality during catalytical chemical vapor deposition (CCVD) growth is necessary. Our highlighted works [1,2] focuses on stabilities of SWCNTs and how they relate to growth. In ref. [1] density functional theory (DFT) is used to calculate the stability of SWCNT-fragments of all chiralities in the 8-18 series. The fragment stabilities are compare with chiralities from actual CCVD products. The results show that 84% of the experimental products represent chiralities among the most stable SWCNT-fragments (within 0.2 eV) from the calculations. The analyzed products from growth experiments show that the chirality of SWCNT products are strongly dependent on the stability of the tubes within each series, suggesting thermodynamic control at the early stage of growth. Analysis of the relative energy show that for lower series 8-10, zigzag SWCNTs are the most stable and for higher series 11-18 the most stable chirality changes from zigzag to armchair. This switch in stability is studied further in ref. [2], where DFT is used to calculate the stability of armchair and zigzag SWCNTs and graphene nanoribbons of different lengths. The calculations show that the stability of armchair and zigzag tubes have different linear dependence with regards to their length, with switches in the most stable chirality occurring at specific lengths for each SWCNT-series. These dependencies are explained by competing edge and curvature energies. Within each series armchair nanotubes are most stable at short lengths, while zigzag nanotubes are most stable at long lengths. This sheds new light into why armchair and near-armchair tubes are dominant products from CCVD growth.

    [1] D. Hedman, H.R Barzegar, A. Rosen, T. Wågberg, J.A Larsson, Sci. Rep., 2015, 5, 16850. [2] D. Hedman, J.A. Larsson, Carbon, 2017, 116, 443.

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  • 9.
    Hedman, Daniel
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Single-Walled Carbon Nanotubes: A theoretical study of stability, growth and properties2019Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    Since their discovery over 25 years ago, scientists have explored the remarkable properties of single-walled carbon nanotubes (SWCNTs) for use in high-tech materials and devices, such as strong light-weight composites, efficient electrical wires, supercapacitors and high-speed transistors. However, the mass production of such materials and devices is still limited by the capability of producing uniform high-quality SWCNTs. The properties of a SWCNT are determined by the orientation of the hexagonal grid of carbon atoms constituting the tube wall, this is known as the chirality of the SWCNT.

    Today's large-scale methods for producing SWCNTs, commonly known as growth, give products with a large spread of different chiralities. A mixture of chiralities give products with a mixture of different properties. This is one of the major obstacles preventing large-scale use of SWCNTs in future materials and devices. The goal is to achieve growth where the resulting product is uniform, meaning that all SWCNTs have the same chirality, a process termed chirality-specific growth. To achieve this requires a deep fundamental understanding of how SWCNTs grow, both from an experimental and a theoretical perspective.

    This work focuses on theoretical studies of SWCNTs and their growth mechanisms. With the goal of achieving a deeper understanding of how chirality arises during growth and how to control it. Thus, taking us ever closer to the ultimate goal of achieving chirality-specific growth. In this thesis, an introduction to the field is given and the current research questions are stated. Followed by chapters on carbon nanomaterials, SWCNTs and computational physics. A review of the state-of-the-art experimental and theoretical works relating to chirality specific growth is also given.

    The results presented in this thesis are obtained using first principle density functional theory calculations. Results show that the stability of short SWCNT-fragments can be linked to the products observed in experiments. In 84% of the investigate cases, the chirality of experimental products matches the chirality of the most stable SWCNT-fragments (within 0.2 eV). Further studies also reveal a previously unknown link between the stability of SWCNT-fragments and their length. Calculations show that at specific lengths the most stable chirality changes. Thus, introducing the concept of a switching length for SWCNT stabilities.

    This newly found property of SWCNTs is used in combination with previously published works to create a state-of-the-art analytical model to investigate growth of SWCNTs any temperature. Results from the model show that the most stable chirality obtained is dependent on the diameter, length of the SWCNT, the growth temperature and the composition of the catalyst. Finally, a detailed study on the ability of catalyst metals to sustain SWCNT growth points to Pt as an interesting candidate to achieve growth of rarely seen chiralities. The new knowledge gained from these results takes us even closer to achieving chirality-specific growth.

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  • 10.
    Hedman, Daniel
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Barzegar, Hamid Reza
    Department of Physics, Umeå University, Department of Physics, University of California.
    Rosén, Arne
    Physics Department, Göteborg University.
    Wågberg, Thomas
    Department of Physics, Umeå University.
    Larsson, Andreas
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    On the Stability and Abundance of Single Walled Carbon Nanotubes2015In: Scientific Reports, E-ISSN 2045-2322, Vol. 5, article id 16850Article in journal (Refereed)
    Abstract [en]

    Many nanotechnological applications, using single-walled carbon nanotubes (SWNTs), are only possible with a uniform product. Thus, direct control over the product during chemical vapor deposition (CVD) growth of SWNT is desirable, and much effort has been made towards the ultimate goal of chirality-controlled growth of SWNTs. We have used density functional theory (DFT) to compute the stability of SWNT fragments of all chiralities in the series representing the targeted products for such applications, which we compare to the chiralities of the actual CVD products from all properly analyzed experiments. From this comparison we find that in 84% of the cases the experimental product represents chiralities among the most stable SWNT fragments (within 0.2 eV) from the computations. Our analysis shows that the diameter of the SWNT product is governed by the well-known relation to size of the catalytic nanoparticles, and the specific chirality is normally determined by the product’s relative stability, suggesting thermodynamic control at the early stage of product formation. Based on our findings, we discuss the effect of other experimental parameters on the chirality of the product. Furthermore, we highlight the possibility to produce any tube chirality in the context of recent published work on seeded-controlled growth.

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  • 11.
    Hedman, Daniel
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Barzegar, Hamid Reza
    Department of Physics, Umeå University, Umeå, Sweden.
    Rosén, Arne
    Department of Physics, Göteborg University, Göteborg, Sweden.
    Wågberg, Thomas
    Department of Physics, Umeå University, Umeå, Sweden.
    Larsson, J. Andreas
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    The relation between stability and abundance of single walled carbon nanotubes2015Conference paper (Other academic)
    Abstract [en]

    The ability to utilize the remarkable electrical and mechanical properties of single walled carbon nanotubes (SWNTs) can be hugely beneficial for technological applications. The limiting factors for these technological applications is that many of them rely on specific electrical/mechanical properties of the SWNT. The mechanical and electrical properties of a SWNT depends on its chiral indecencies n and m, which means that in order to get a desired electrical/mechanical property one needs to synthesize SWNTs with specific chiral indecencies.Huge effort has been put on trying to synthesize SWNTs with specific chiral indecencies or to post-purify them after synthesis. Although post-purification methods can result in a relatively high yield of SWNTs with specific chiralities, such methods are expensive, time consuming and may damage the SWNTs. A more efficient method would be to selectively grow/synthesize SWNTs with the desired properties. Chemical vapor deposition (CVD) has become a favored technique for trying to achieve selective SWNT growth since the process involves several controllable growth parameters.In our work we have investigated the relation between the relative stability of different SWNTs and compared that to the experimentally observed statistical abundance of the same SWNTs. The relative energy of the SWNTs was calculated using density functional theory with the VASP-code. We have chosen to include all the SWNTs in the (n+m) = 8,9,10,11,12,13,14,15,16,17 and 18-series in our calculations, this equals 80 SWNTs in total. The SWNT models used in our calculations are six layered hydrogen terminated SWNT fragments where each layer contains 2(n+m) carbon atoms.Our calculations show a remarkable connection between the relative stability of the SWNTs and their statistical abundance in experiments. The most stable SWNT in each series correlates with the most abundant SWNT in that series, as found in the experimental results gathered from the literature.

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  • 12.
    Hedman, Daniel
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science. Research Center for Computational Design of Advanced Functional Materials, National Institute of Advanced Industrial Science and Technology (AIST), Central 2, 1-1-1 Umezono, Tsukuba, Ibaraki, 305-8568, Japan; Center for Multidimensional Carbon Materials, Institute for Basic Science (IBS), Ulsan, 44919, South Korea.
    Feltrin, Ana Carolina
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Miyamoto, Yoshiyuki
    Research Center for Computational Design of Advanced Functional Materials, National Institute of Advanced Industrial Science and Technology (AIST), Central 2, 1-1-1 Umezono, Tsukuba, Ibaraki, 305-8568, Japan.
    Akhtar, Farid
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Ab initio aided design of novel quaternary, quinary and senary high-entropy borocarbides2022In: Journal of Materials Science, ISSN 0022-2461, E-ISSN 1573-4803, Vol. 57, no 1, p. 422-443Article in journal (Refereed)
    Abstract [en]

    High-entropy materials have attracted considerable interest due to their unique, improved properties and large configurational entropy. Out of these, high-entropy ceramics (HECs) are of particular interest since the independent solubility of cations and anions results in increased configurational entropy. However, most HEC research considers only a single element occupying the anion sublattice, which limits the maximum attainable configurational entropy. Here, we expand our previous work on high-entropy borocarbides where both boron and carbon occupy the anion sublattice. By applying an ab initio based screening procedure, we identify six elements Li, Ti, V, Zr, Nb and Hf suitable for forming high-entropy borocarbides. With these elements, we propose six novel HEC compositions, and by computing their entropy forming ability, we identify that three are likely to form single-phase during synthesis. Material properties and lattice distortions for all proposed compositions are studied using density functional theory calculations with special quasirandom structures. The directional lattice distortions, a concept we introduce in this work, show that lattice distortions have an elemental and directional preference for certain HEC compositions. We also show that the novel inclusion of Li improves the mechanical properties of the proposed HECs, the details of which are studied using the electron localization function.

  • 13.
    Hedman, Daniel
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Fjellström, Mattias
    Modeling the interactions between magnetic particles2013Report (Other academic)
    Abstract [en]

    The aim of the work presented here is to describe the appearance of force curves from atomic force microscopy measurements between two interacting magnetic particles. A model treating particles as points is first presented. This model is found to accurately describe interactions involving spherical particles, but is not equally successful in describing interactions between particles of cylindrical and conical geometries at short surface separations. Effects from particle geometries are introduced in the dimensional model through dimensional analysis. A characteristic length describing the vertical extent of the particles is defined. An example calculation of the characteristic length for a spherical particle of known radius is presented. The same computational method is then applied to several experimental force curves from atomic force microscopy measurements. The calculated characteristic lengths are of comparable size to the known vertical extent of the particles. Reconstruction of the experimental force curves using the calculated characteristic lengths in the dimensional model gives good agreement between theory and experiment.

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  • 14.
    Hedman, Daniel
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Larsson, Andreas
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Analytical modelling of single-walled carbon nanotube energies: the impact of curvature, length and temperature2020In: SN Applied Sciences, ISSN 2523-3963, E-ISSN 2523-3971, Vol. 2, no 3, article id 367Article in journal (Refereed)
    Abstract [en]

    Recent breakthroughs in the field of single-walled carbon nanotube (SWCNT) growth have been achieved by combining theoretical models with experiments. Theoretical models rely on accurate energies for SWCNTs, obtained via first principle calculations in the form of density functional theory (DFT). Such calculations are accurate, but time and resource intensive which limits the size and number of systems that can be studied. Here, we present a new analytical model consisting of three fundamental energy expressions, parametrized using DFT, for fast and accurate calculation of SWCNT energies at any temperature. Tests against previously published results show our model having excellent accuracy, with an root mean square error in total energies below 2 meV per atom as compared to DFT. We apply the model to study SWCNT growth on Ni catalysts at elevated temperatures by investigating the SWCNT/catalyst interface energy. Results show that the most stable interface shifts towards chiral edges as the temperature increases. The model’s ability to perform calculations at any temperature in combination with its speed and flexibility will allow researcher to study more and larger systems, aiding future research into SWCNT growth

  • 15.
    Hedman, Daniel
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Larsson, Andreas
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Length dependent stability of single-walled carbon nanotubes and how it affects their growth2017In: Carbon, ISSN 0008-6223, E-ISSN 1873-3891, Vol. 116, p. 443-447Article in journal (Refereed)
    Abstract [en]

    Using density-functional theory the stability of armchair and zigzag single-walled carbon nanotubes and graphene nanoribbons was investigated. We found that the stability of armchair and zigzag nanotubes has different linear dependence with regard to their length, with switches in the most stable chirality occurring at specific lengths for each nanotube series. We explain these dependencies by competing edge and curvature effects. We have found that within each series armchair nanotubes are the most stable at short lengths, while zigzag nanotubes are the most stable at long lengths. These results shed new insights into why (near) armchair nanotubes are the dominant product from catalytic chemical vapor deposition growth, if templating is not used. Paradoxically, the stability of armchair nanotubes at short lengths favors their growth although zigzag nanotubes are more stable at long lengths, resulting in the production of the least stable nanotubes.

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  • 16.
    Hedman, Daniel
    et al.
    Center for Multidimensional Carbon Materials (CMCM), Institute for Basic Science (IBS), 44919, Ulsan, Republic of Korea.
    McLean, Ben
    Center for Multidimensional Carbon Materials (CMCM), Institute for Basic Science (IBS), 44919, Ulsan, Republic of Korea; School of Engineering, RMIT University, 3001, Victoria, Australia.
    Bichara, Christophe
    Aix-Marseille Univ, CNRS, CINaM, UMR7325, 13288, Marseille, France.
    Maruyama, Shigeo
    Department of Mechanical Engineering, The University of Tokyo, 113-8656, Tokyo, Japan.
    Larsson, J. Andreas
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Ding, Feng
    Center for Multidimensional Carbon Materials (CMCM), Institute for Basic Science (IBS), 44919, Ulsan, Republic of Korea; Department of Materials Science and Engineering, Ulsan National Institute of Science and Technology (UNIST), 44919, Ulsan, Republic of Korea; Faculty of Materials Science and Engineering, Institute of Technology for Carbon Neutrality, Shenzhen Institute of Advanced Technology Chinese Academy of Sciences, 518055, Shenzhen, China.
    Dynamics of growing carbon nanotube interfaces probed by machine learning-enabled molecular simulations2024In: Nature Communications, E-ISSN 2041-1723, Vol. 15, article id 4076Article in journal (Refereed)
    Abstract [en]

    Carbon nanotubes (CNTs), hollow cylinders of carbon, hold great promise for advanced technologies, provided their structure remains uniform throughout their length. Their growth takes place at high temperatures across a tube-catalyst interface. Structural defects formed during growth alter CNT properties. These defects are believed to form and heal at the tube-catalyst interface but an understanding of these mechanisms at the atomic-level is lacking. Here we present DeepCNT-22, a machine learning force field (MLFF) to drive molecular dynamics simulations through which we unveil the mechanisms of CNT formation, from nucleation to growth including defect formation and healing. We find the tube-catalyst interface to be highly dynamic, with large fluctuations in the chiral structure of the CNT-edge. This does not support continuous spiral growth as a general mechanism, instead, at these growth conditions, the growing tube edge exhibits significant configurational entropy. We demonstrate that defects form stochastically at the tube-catalyst interface, but under low growth rates and high temperatures, these heal before becoming incorporated in the tube wall, allowing CNTs to grow defect-free to seemingly unlimited lengths. These insights, not readily available through experiments, demonstrate the remarkable power of MLFF-driven simulations and fill long-standing gaps in our understanding of CNT growth mechanisms.

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  • 17.
    Hedman, Daniel
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science. Research Center for Computational Design of Advanced Functional Materials, National Institute of Advanced Industrial Science and Technology (AIST), Central 2, 1-1-1 Umezono, Tsukuba, Ibaraki 305-8568, Japan.
    Rothe, Tom
    Institute of Physics, Faculty of Natural Sciences, Chemnitz University of Technology, Chemnitz 09126, Germany.
    Johansson, Gustav
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Sandin, Fredrik
    Luleå University of Technology, Department of Computer Science, Electrical and Space Engineering, Embedded Internet Systems Lab.
    Larsson, J. Andreas
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Miyamoto, Yoshiyuki
    Research Center for Computational Design of Advanced Functional Materials, National Institute of Advanced Industrial Science and Technology (AIST), Central 2, 1-1-1 Umezono, Tsukuba, Ibaraki 305-8568, Japan.
    Impact of training and validation data on the performance of neural network potentials: A case study on carbon using the CA-9 dataset2021In: Carbon Trends, ISSN 2667-0569, Vol. 3, article id 100027Article in journal (Refereed)
    Abstract [en]

    The use of machine learning to accelerate computer simulations is on the rise. In atomistic simulations, the use of machine learning interatomic potentials (ML-IAPs) can significantly reduce computational costs while maintaining accuracy close to that of ab initio methods. To achieve this, ML-IAPs are trained on large datasets of images, which are atomistic configurations labeled with data from ab initio calculations. Focusing on carbon, we use deep learning to train neural network potentials (NNPs), a form of ML-IAP, based on the state-of-the-art end-to-end NNP architecture SchNet and investigate how the choice of training and validation data affects the performance of the NNPs. Training is performed on the CA-9 dataset, a 9-carbon allotrope dataset constructed using data obtained via ab initio molecular dynamics (AIMD). Our results show that image generation with AIMD causes a high degree of similarity between the generated images, which has a detrimental effect on the performance of the NNPs. But by carefully choosing which images from the dataset are included in the training and validation data, this effect can be mitigated. We conclude by benchmarking our trained NNPs in applications such as relaxation and phonon calculation, where we can reproduce ab initio results with high accuracy.

  • 18.
    Yusupov, Khabib
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Hedman, Daniel
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Tsapenko, Alexey P.
    Skolkovo Institute of Science and Technology, Moscow, Russian Federation. Department of Applied Physics, Aalto University, Espoo, Finland.
    Ishteev, A.
    Department of Functional Nanosystems and High-Temperature Materials, National University of Science and Technology “MISiS” Moscow, Russian Federation.
    You, Shujie
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Khovaylo, V.
    Department of Functional Nanosystems and High-Temperature Materials, National University of Science and Technology “MISiS” Moscow, Russian Federation. National Research South Ural State University, Chelyabinsk, Russian Federation.
    Larsson, Andreas
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Nasibulin, Albert G.
    Skolkovo Institute of Science and Technology, Moscow, Russian Federation. Department of Applied Physics, Aalto University, Espoo, Finland.
    Vomiero, Alberto
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science. Department of Molecular Sciences and Nanosystems, Ca’ Foscari University of Venice, Venezia Mestre, Italy.
    Enhancing the thermoelectric performance of single-walled carbon nanotube-conducting polymer nanocomposites2020In: Journal of Alloys and Compounds, ISSN 0925-8388, E-ISSN 1873-4669, Vol. 845, article id 156354Article in journal (Refereed)
    Abstract [en]

    Harnessing energy lost in the form of heat is an important challenge today. Organic thermoelectric materials (TE) can convert lost heat into electricity at relatively low temperature. Single-walled carbon nanotubes (SWCNTs) are known to boost the TE properties of organic-based materials at room temperature (TR). However, the TE performance decreases with the increasing temperature, which restricts the working temperature region of the devices. Here, we present a three steps investigation: initially, the influence of the net of SWCNTs on TE properties of polymer matrix; secondly, creation of hybrid fillers via SWCNTs treatment with gold chloride; lastly, chemical post-treatment of obtained systems in the temperature range 325–410 K. In the process of HAuCl4 aerosolization (gold chloride treatment) on the surface of nanotubes, different ionic conformations (Au and AuCl4−) can be formed. For this reason, we performed a theoretical investigation on the influence of ionic conformations on SWCNTs on the electronic structure. Implementation of SWCNTs net into polymer matrix alongside gold chloride doping and chemical post-treatment successfully increased the power factor of the system in the temperature interval from 300 to 410 K. These results demonstrate the potential of combined approach in creation of hybrid fillers based on organic/inorganic materials with chemical post-treatment in boosting the thermoelectric performance within the whole operating temperature of polymer-based composite alongside the importance of theoretical modeling in tuning the electronic structure of composite systems through a material-by-design approach.

  • 19.
    Zhang, Hanzhu
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Hedman, Daniel
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Feng, P.
    China University of Mining and Technology - School of Materials Science and Engineering, Xuzhou, CHINA.
    Han, G.
    University of Science and Technology Beijing - School of Materials Science and Engineering, Beijing, CHINA.
    Akhtar, Farid
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    High Entropy B2(HfMoTaTi)C and SiC Ceramic Composite2019In: XVI Conference and Exhibition of the European Ceramic Society: Book of Abstracts, European Ceramic Society (ECerS) , 2019, p. 338-338Conference paper (Refereed)
    Abstract [en]

    Refractory carbides HfC, Mo2C, TiC, TaC, B4C, and SiC were mixed with a molar ratio of 2:1:2:2:1:2 to fabricate multicomponent ceramic composite by pulsed current processing (PCP). From the starting materials that consist of face-centered cubic (FCC), hexagonal and rhombohedral crystal structures, the investigated carbide system is reported to form a single phase B2(HfMoTaTi)C high-entropy ceramic (HEC) with SiC. The HEC phase contains uniform distribution of constitutional elements Hf, Mo, Ta, Ti, B and C, according to Energy dispersive X-ray spectroscopy (EDS) and wavelength dispersive X-ray spectroscopy (WDS) results.

    The fabricated HEC phase displays a hexagonal close-packed (HCP) crystal structure, with a high average lattice distortion of 8.26% (see Figure). The HCP structure was observed by X-ray diffraction and selected area diffraction in transmission electron microscopy (TEM). Density-functional theory (DFT) optimization suggested that the hexagonal close-packed (HCP) crystal structure has alternating layers of metal atoms and carbon/boron atoms, i.e. metal atoms of Hf, Mo, Ta and Ti were distributed on the (0001) plane in the HCP lattice, while the carbon/boron atoms formed hexagonal 2D grids on the (0002) plane in the HCP unit cell. Despite of the vast differences in the crystal structures and lattice parameters among the utilized carbides, the formation of the unique hexagonal lattice structure of B2(HfMoTaTi)C can be a result of independent diffusion of the metal and nonmetal atoms. The sintered HEC ceramic composite exhibits excellent oxidation resistance at mediate temperature, 900 ºC for 50h, and elevated temperature, 2000 ºC for 20 s. Nanoindentation test shows that the HEC phase has a high hardness of 35 GPa. The remarkable improvement compared to the theoretical hardness value estimated based on the rule of mixtures (23 GPa) was contributed by the severe lattice distortion in the HCP structure. 

  • 20.
    Zhang, Hanzhu
    et al.
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Hedman, Daniel
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    Feng, Peizhong
    China University of Mining and Technology.
    Han, Gang
    University of Science and Technology Beijing.
    Akhtar, Farid
    Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.
    A high-entropy B4(HfMo2TaTi)C and SiC ceramic composite2019In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 48, no 16, p. 5161-5167Article in journal (Refereed)
    Abstract [en]

    A multicomponent composite of refractory carbides, B4C, HfC, Mo2C, TaC, TiC and SiC, of rhombohedral, face-centered cubic (FCC) and hexagonal crystal structures is reported to form a single phase B4(HfMo2TaTi)C ceramic with SiC. The independent diffusion of the metal and nonmetal atoms led to a unique hexagonal lattice structure of the B4(HfMo2TaTi)C ceramic with alternating layers of metal atoms and C/B atoms. In addition, the classical differences in the crystal structures and lattice parameters among the utilized carbides were overcome. Electron microscopy, X-ray diffraction and calculations using density functional theory (DFT) confirmed the formation of a single phase B4(HfMo2TaTi)C ceramic with a hexagonal close-packed (HCP) crystal structure. The DFT based crystal structure prediction suggests that the metal atoms of Hf, Mo, Ta and Ti are distributed on the (0001) plane in the HCP lattice, while the carbon/boron atoms form hexagonal 2D grids on the (0002) plane in the HCP unit cell. The nanoindentation of the high-entropy phase showed hardness values of 35 GPa compared to the theoretical hardness value estimated based on the rule of mixtures (23 GPa). The higher hardness was contributed by the solid solution strengthening effect in the multicomponent hexagonal structure. The addition of SiC as the secondary phase in the sintered material tailored the microstructure of the composite and offered oxidation resistance to the high-entropy ceramic composite at high temperatures.

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