arXiv subjects

Per Eklund

Publications and source records attributed to Per Eklund.

At least 37 records · Page 2Linked to original sources

arXiv2023

Thermoelectric properties and electronic structure of Cr(Mo,V)Nx thin films studied by synchrotron and lab-based X-ray spectroscopy

Chromium-based nitrides are used in hard, resilient coatings, and show promise for thermoelectric applications due to their combination of structural, thermal, and electronic properties. Here, we investigated the electronic structures and chemical bonding correlated to the thermoelectric properties of epitaxially grown chromium-based multicomponent nitride Cr(Mo,V)Nx thin films. Due to minuscule N vacancies, finite population of Cr 3d and N 2p states appear at the Fermi level and diminishes the band opening for Cr0.51N0.49. Incorporating holes by alloying V in N deficient CrN matrix results in enhanced thermoelectric power factor with marginal change in the charge transfer of Cr to N compared to Cr0.51N0.49. Further alloying Mo isoelectronic to Cr increases the density of states across the Fermi level due to hybridization of the (Cr, V) 3d and Mo 4d-N 2p states in Cr(Mo,V)Nx. The hybridization effect with reduced N 2p states off from stoichiometry drives the system towards metal like electrical resistivity and reduction in Seebeck coefficient compensating the overall power factor still comparable to Cr0.51N0.49. The N deficiency also depicts a critical role in reduction of the charge transfer from metal to N site. The present work envisages ways for enhancing thermoelectric properties through electronic band engineering by alloying and competing effects of N vacancies.

cond-mat.mtrl-sci↗

arXiv2023

Effects of deposition temperature on the mechanical and structural properties of amorphous Al-Si-O thin films prepared by RF magnetron sputtering

Aluminosilicate (Al-Si-O) thin films containing up to 31 at. % Al and 23 at. % Si were prepared by reactive RF magnetron co-sputtering. Mechanical and structural properties were measured by indentation and specular reflectance infrared spectroscopy at varying Si sputtering target power and substrate temperature in the range 100 to 500 °C. It was found that an increased substrate temperature and Al/Si ratio give denser structure and consequently higher hardness (7.4 to 9.5 GPa) and reduced elastic modulus (85 to 93 GPa) while at the same time lower crack resistance (2.6 to 0.9 N). The intensity of the infrared Si-O-Si/Al asymmetric stretching vibrations shows a linear dependence with respect to Al concentration. The Al-O-Al vibrational band (at 1050 cm-1) shifts towards higher wavenumbers with increasing Al concentration which indicates a decrease of the bond length, evidencing denser structure and higher residual stress, which is supported by the increased hardness. The same Al-O-Al vibrational band (at 1050 cm-1) shifts towards lower wavenumber with increasing substrate temperature indicating an increase in the of the average coordination number of Al.

cond-mat.mtrl-sci↗

arXiv2022

Phase formation in CrFeCoNi nitride thin films

As a single-phase alloy, CrFeCoNi is a face centered cubic (fcc) material related to the archetypical high-entropy Cantor alloy CrFeCoNiMn. For thin films, CrFeCoNi of approximately equimolar composition tends to assume an fcc structure when grown at room temperature by magnetron sputtering. However, the single-phase solid solution state is typically not achieved for thin films grown at higher temperatures. The same holds true for Cantor alloy-based ceramics (nitrides and oxides), where phase formation is extremely sensitive to process parameters such as the amount of reactive gas. This study combines theoretical and experimental methods to understand the phase formation in nitrogen-containing CrFeCoNi thin films. Density functional theory calculations considering three competing phases (CrN, Fe-Ni and Co) show that the free energy of mixing, delta G of (CrFeCoNi)1-xNx solid solutions has a maximum at x = 0.20-0.25, and delta G becomes lower when x less than 0.20, greater than 0.25. Thin films of (CrFeCoNi)1-xNx (x = 0.14-0.41) grown by magnetron sputtering show stabilization of the metallic fcc when x lesser than or equal to 0.22 and the stabilization of the NaCl B1 structure when x is greater than 0.33, consistent with the theoretical prediction. In contrast, films with intermediate amounts of nitrogen (x = 0.22) grown at higher temperatures show segregation into multiple phases of CrN, Fe-Ni-rich and Co. These results offer an explanation for the requirement of kinetically limited growth conditions at low temperature for obtaining single-phase CrFeCoNi Cantor-like nitrogen-containing thin films and are of importance for understanding the phase-formation mechanisms in multicomponent ceramics.

cond-mat.mtrl-sci↗

arXiv2022

Single photon detection performance of highly disordered NbTiN thin films

We experimentally investigated the detection performance of highly disordered NbxTi1-xN based superconducting nanowire single photon detectors (SNSPDs). The dependence on the composition of the transition temperature Tc for NbxTi1-xN films show a dome-like behavior on the Nb content, with a maximal Tc at xNb~0.65 , and the Nb0.65Ti0.35N films also combine relatively large sheet resistance and intermediate residual resistivity ratio. Moreover, 60-nm-wide and 7-nm-thick Nb0.65Ti0.35N nanowires show a switching current as high as 14.5 uA, and saturated intrinsic detection efficiency with a plateau of more than 2 uA at 2.4 K. Finally, the corresponding SNSPDs on an alternative SiO2/Ta2O5 dielectric mirror showed a system detection efficiency of approximately 92% for 1550 nm photons, and the timing jitter is around 26 ps. Our results demonstrate that the highly disordered NbxTi1-xN films are promising for fabricating SNSPDs for near- and middle-infrared single photons with high detection efficiency and low timing jitter.

cond-mat.supr-con↗

arXiv2022

Chemical-scissor-mediated structural editing of layered transition metal carbides

Intercalation of non-van der Waals (vdW) layered materials can produce new 2D and 3D materials with unique properties, but it is difficult to achieve. Here, we describe a structural editing protocol for 3D non-vdW layered ternary carbides and nitrides (MAX phases) and their 2D vdW derivatives (MXenes). Gap-opening and species-intercalating stages were mediated by chemical scissors and guest intercalants, creating a large family of layered materials with unconventional elements and structures in MAX phases, as well as MXenes with versatile termination species. Removal of surface terminations by metal scissors and stitching of carbide layers by metal atoms leads to a reverse transformation from MXenes to MAX phases, and metal-intercalated 2D carbides. This scissor-mediated structural editing may enable structural and chemical tailoring of other layered ceramics.

cond-mat.mtrl-sci↗

arXiv2022

Solid-state Janus nanoprecipitation enables amorphous-like heat conduction in crystalline Mg3Sb2-based thermoelectric materials

Solid-state precipitation can be used to tailor materials properties, ranging from ferromagnets and catalysts to mechanical strengthening and energy storage. Thermoelectric properties can be modified by precipitation to enhance phonon scattering while retaining charge-carrier transmission. Here, we uncover unconventional dual Janus-type nanoprecipitates in Mg3Sb1.5Bi0.5 formed by side-by-side Bi- and Ge-rich appendages, in contrast to separate nanoprecipitate formation. These Janus nanoprecipitates result from local co-melting of Bi and Ge during sintering, enabling an amorphous-like lattice thermal conductivity. A precipitate size effect on phonon scattering is observed due to the balance between alloy-disorder and nanoprecipitate scattering. The thermoelectric figure-of-merit ZT reaches 0.6 near room temperature and 1.6 at 773 K. The Janus nanoprecipitation can be introduced into other materials and may act as a general property-tailoring mechanism.

cond-mat.mtrl-sci↗

arXiv2022

P-type behavior of CrN thin films by control of point defects

We report the results of a combined experimental and theoretical study on nonstoichiometric CrN1+d thin films grown by reactive magnetron sputtering on c-plane sapphire, MgO (100) and LaAlO3 (100) substrates in a Ar/N2 gas mixture using different percentage of N2. There is a transition from n-type to p-type behavior in the layers as a function of nitrogen concentration varying from 48 at. % to 52 at. % in CrN films. The compositional change follows a similar trend for all substrates, with a N/Cr ratio increasing from approximately 0.7 to 1.06-1.10 by increasing percentage of N2 in the gas flow ratio. As a result of the change in stoichiometry, the lattice parameter and the Seebeck coefficient increase together with the increase of N in CrN1+d; in particular, the Seebeck value coefficient transitions from -50 uV.K-1 for CrN0.97 to +75 uV.K-1 for CrN1.1. Density functional theory calculations show that Cr vacancies can account for the change in Seebeck coefficient, since they push the Fermi level down in the valence band, whereas N interstitial defects in the form of N2 dumbbells are needed to explain the increasing lattice parameter. Calculations including both types of defects, which have a strong tendency to bind together, reveal a slight increase in the lattice parameter and a simultaneous formation of holes in the valence band. To explain the experimental trends, we argue that both Cr vacancies and N2 dumbbells, possibly in combined configurations, are present in the films. We demonstrate the possibility of controlling the semiconducting behavior of CrN with intrinsic defects from n- to p-type, opening possibilities to integrate this compound in energy-harvesting thermoelectric devices.

cond-mat.mtrl-sci↗

arXiv2021

Electron-Phonon Coupling and Quantum Correction to Topological Magnetoconductivity in Bi2GeTe4

We report on structure, vibrational properties and weak-antilocalization-(WAL-) induced quantum correction to magnetoconductivity in single crystal Bi2GeTe4. Surface band structure calculations show a single Dirac cone corresponding to topological surface states in Bi2GeTe4. An estimated phase coherence length, l_ϕ ~ 143 nm and prefactor α ~ - 1.54 from Hikami-Larkin-Nagaoka fitting of magnetoconductivity describe the quantum correction to conductivity. An anomalous temperature dependence of A1g Raman modes confirms enhanced electron-phonon interactions. Our results establish the involvement of vibrations of Bi-Te with existence of topological surface states and WAL in Bi2GeTe4.

cond-mat.mtrl-sci↗

arXiv2021

Early stages of dissolution corrosion in 316L and DIN 1.4970 austenitic stainless steels with and without anticorrosion coatings in static liquid lead-bismuth eutectic (LBE) at 500$^\circ$C

This work addresses the early stages ($\le$1000 h) of the dissolution corrosion behavior of 316L and DIN 1.4970 austenitic stainless steels in contact with oxygen-poor (C$_O$ < 10$^-$$^8$ mass%), static liquid lead-bismuth eutectic (LBE) at 500°C for 600-1000 h. The objective of this study was to determine the relative early-stage resistance of the uncoated steels to dissolution corrosion and to assess the protectiveness of select candidate coatings (Cr$_2$AlC, Al$_2$O$_3$, V$_2$Al$_x$C$_y$). The simultaneous exposure of steels with intended differences in microstructure and thermomechanical state showed the effects of steel grain size, density of annealing/deformation twins, and secondary precipitates on the steel dissolution corrosion behavior. The findings of this study provide recommendations on steel manufacturing with the aim of using the steels to construct Gen-IV lead-cooled fast reactors.

cond-mat.mtrl-sci↗

arXiv2021

Near-Room-Temperature Ferromagnetic Behavior of Single-Atom-Thick 2D Iron in Nanolaminated Ternary MAX Phases

Two dimensional (2D) ferromagnetic materials have attracted much attention in the fields of condensed matter physics and materials science, but their synthesis is still a challenge given their limitations on structural stability and susceptibility to oxidization. MAX phases nanolaminated ternary carbides or nitrides possess a unique crystal structure in which single-atom-thick A sublayers are interleaved by two dimensional MX slabs, providing nanostructured templates for designing 2D ferromagnetic materials if the non-magnetic A sublayers can be substituted replaced by magnetic elements. Here, we report three new ternary magnetic MAX phases (Ta2FeC, Ti2FeN and Nb2FeC) with A sublayers of single-atom-thick 2D iron through an isomorphous replacement reaction of MAX precursors (Ta2AlC, Ti2AlN and Nb2AlC) with a Lewis acid salts (FeCl2). All these MAX phases exhibit ferromagnetic (FM) behavior. The Curie temperature (Tc) of Ta2FeC and Nb2FeC MAX phase are 281 K and 291 K, respectively, i.e. close to room temperature. The saturation magnetization of these ternary magnetic MAX phases is almost two orders of magnitude higher than that of V2(Sn,Fe)C MAX phase whose A-site is partial substituted by Fe. Theoretical calculations on magnetic orderings of spin moments of Fe atoms in these nanolaminated magnetic MAX phases reveal that the magnetism can be mainly ascribed to intralayer exchange interaction of the 2D Fe atomic layers. Owning to the richness in composition of MAX phases, there is a large compositional space for constructing functional single-atom-thick 2D layers in materials using these nanolaminated templates.

cond-mat.mtrl-sci↗

arXiv2021

Characterization and identification of Au pathfinder minerals from an artisanal mine site using X-ray diffraction

Gold-associated pathfinder minerals have been investigated by identifying host minerals of Au for samples collected from an artisanal mining site near a potential gold mine (Kubi Gold Project) in Dunkwa-On-Offin in the central region of Ghana. We find that for each composition of Au powder (impure) and the residual black hematite/magnetite sand that remains after gold panning, there is a unique set of associated diverse indicator minerals. These indicator minerals are identified as SiO2 (quartz), Fe3O4 (magnetite), and Fe2O3 (hematite), while contributions from pyrite, arsenopyrites, iridosmine, scheelite, tetradymite, garnet, gypsum, and other sulfate materials are insignificant. This constitutes a confirmative identification of Au pathfinding minerals in this particular mineralogical area. The findings suggest that X-ray diffraction could also be applied in other mineralogical sites to aid in identifying indicator minerals of Au and the location of ore bodies at reduced environmental and exploration costs.

cond-mat.mtrl-sci↗

arXiv2021

An upgraded ultra-high vacuum magnetron-sputtering system for high-versatility and software-controlled deposition

Magnetron sputtering is a widely used physical vapor deposition technique. Reactive sputtering is used for the deposition of, e.g, oxides, nitrides and carbides. In fundamental research, versatility is essential when designing or upgrading a deposition chamber. Furthermore, automated deposition systems are the norm in industrial production, but relatively uncommon in laboratory-scale systems used primarily for fundamental research. Combining automatization and computerized control with the required versatility for fundamental research constitutes a challenge in designing, developing, and upgrading laboratory deposition systems. The present article provides a detailed description of the design of a lab-scale deposition chamber for magnetron sputtering used for the deposition of metallic, oxide, nitride and oxynitride films with automated controls, dc or pulsed bias, and combined with a coil to enhance the plasma density near the substrate. LabVIEW software (provided as Supplementary Information) has been developed for a high degree of computerized or automated control of hardware and processes control and logging of process details.

physics.app-ph↗

arXiv2020

Deposition of MAX phase containing thin films from a (Ti,Zr)2AlC compound target

This work reports on sputter depositions carried out from a compound (Ti,Zr)2AlC target, whereupon Al-containing (Ti,Zr)C thin films (30-40 nm in thickness) were deposited on MgO(111) and Al2O3(0001) substrates at temperatures ranging between 500 and 900 °C. The presence of Al within the carbide structure was evidenced by lattice parameter variations. Furthermore, chemical analyses showed that the Al distribution throughout the film thickness was fairly homogeneous. Thicker films (80-90 nm) deposited from the same compound target consisted of the pseudo-binary (Ti,Zr)C and intermetallic compounds in the Ti-Zr-Al system up to 800 °C, as well as solid solution MAX phases with different Ti:Zr ratios at 900 °C. X-ray diffraction and transmission electron microscopy showed that both (Ti,Zr)2AlC and (Ti,Zr)3AlC2 solid solution MAX phases were formed. Moreover, this work discusses the growth mechanism of the thicker films, which started with the formation of the mixed (Ti,Zr)C carbide, followed by the nucleation and growth of aluminides, eventually leading to the formation of the MAX phases, which was the primary objective of the sputter depositions.

cond-mat.mtrl-sci↗

arXiv2020

Halogenated MXenes with Electrochemically Active Terminals for High Performance Zinc Ion Batteries

The class of two-dimensional metal carbides and nitrides known as MXenes offer a distinct manner of property tailoring for a wide range of applications. The ability to tune the surface chemistry for expanding the property space of MXenes is thus an important topic, although experimental exploration of new surface terminals remains a challenge. Here, we synthesized Ti3C2 MXene with unitary, binary and ternary halogen terminals, e.g. -Cl, -Br, -I, -BrI and -ClBrI, to investigate the effect of surface chemistry on the properties of MXenes. The electrochemical activity of Br and I element result in the extraordinary electrochemical performance of the MXenes as cathodes for aqueous zinc ion batteries. The -Br and -I containing MXenes, e.g. Ti3C2Br2 and Ti3C2I2, exhibit distinct discharge platforms with considerable capacities of 97.6 mAh g-1 and 135 mAh g-1. Ti3C2(BrI) and Ti3C2(ClBrI) exhibit dual discharge platforms with capacities of 117.2 mAh g-1 and 106.7 mAh g-1. In contrast, the previously discovered MXenes Ti3C2Cl2 and Ti3C2(OF) exhibit no discharge platforms, and only ~50% of capacities and energy densities of Ti3C2Br2. These results emphasize the effectiveness of the Lewis-acidic-melt etching route for tuning the surface chemistry of MXenes, and also show promise for expanding the MXene family towards various applications.

cond-mat.mtrl-sci↗

arXiv2019

Mechanical properties of VMoNO as a function of oxygen concentration: toward development of hard and tough refractory oxynitrides

Improved toughness is a central goal in the development of wear-resistant refractory ceramic coatings. Extensive theoretical and experimental research has revealed that NaCl structure VMoN alloys exhibit surprisingly high ductility combined with high hardness and toughness. However, during operation, protective coatings inevitably oxidize, a problem which may compromise material properties and performance. Here, we explore the role of oxidation in altering VMoN properties. Density functional theory and theoretical intrinsic hardness models are used to investigate the mechanical behavior of cubic V0.5Mo0.5N1-xOx solid solutions as a function of the oxygen concentration x. Elastic-constant and intrinsic hardness calculations show that oxidation does not degrade the mechanical properties of V0.5Mo0.5N. Electronic structure analyses indicate that the presence of oxygen reduces the covalent bond character, which slightly lowers the alloy strength and intrinsic hardness. Nevertheless, the character of metallic d-d states, which are crucial for allowing plastic deformation and enhancing toughness, remains unaffected. Overall, our results suggest that VMoNO oxynitrides, with oxygen concentrations as high as 50%, possess high intrinsic hardness, while still being ductile.

cond-mat.mtrl-sci↗

arXiv2019

Influence of Si doping and O2-flow on arc deposited (Al,Cr)2O3 coatings

(Al,Cr)2O3 coatings with Al/(Al+Cr) = 0.5 or Al = 70 at.%, doped with 0, 5 or 10 at.% Si, were deposited on hard metal and Si(100) substrates to elucidate the influence of Si on the resulting coatings. The chemical analysis of the coatings showed between 3.3 and 7.4 at.% metal fraction Si incorporated into all studied coatings depending on cathode Si-composition. The incorporated Si content does not change significantly with different oxygen flow covering a wide range of deposition conditions from low to high O2 flow during growth. The addition of Si promotes the metastable B1-like cubic structure over the thermodynamically stable corundum structure. The hardness determined by nanoindentation of the as-deposited coatings is slightly reduced upon Si-incorporation as well as upon increased Al-content. Si is found enriched in droplets but can also be found at a lower content, evenly spread, without visible segregation on the ~5 nm scale, in the actual oxide coating. The positive effect of improved cathode erosion upon Si-incorporation has to be balanced against the promotion of the metastable B1-like structure, having lower room temperature hardness and inferior thermal stability compared to the corundum structure.

cond-mat.mtrl-sci↗

arXiv2019

A general Lewis acidic etching route for preparing MXenes with enhanced electrochemical performance in non-aqueous electrolyte

Two-dimensional carbides and nitrides of transition metals, known as MXenes, are a fast-growing family of 2D materials that draw attention as energy storage materials. So far, MXenes are mainly prepared from Al-containing MAX phases (where A = Al) by Al dissolution in F-containing solution, but most other MAX phases have not been explored. Here, a redox-controlled A-site-etching of MAX phases in Lewis acidic melts is proposed and validated by the synthesis of various MXenes from unconventional MAX phase precursors with A elements Si, Zn, and Ga. A negative electrode of Ti3C2 MXene material obtained through this molten salt synthesis method delivers a Li+ storage capacity up to 738 C g-1 (205 mAh g-1) with high-rate performance and pseudocapacitive-like electrochemical signature in 1M LiPF6 carbonate-based electrolyte. MXene prepared from this molten salt synthesis route offer opportunities as high-rate negative electrode material for electrochemical energy storage applications.

physics.app-ph↗

arXiv2019

Multielemental single-atom-thick A layers in nanolaminated V2(Sn, A)C (A=Fe, Co, Ni, Mn) for tailoring magnetic properties

Tailoring of individual single-atom-thick layers in nanolaminated materials offers atomic-level control over material properties. Nonetheless, multielement alloying in individual atomic layers in nanolaminates is largely unexplored. Here, we report a series of inherently nanolaminated V2(A'xSn1-x)C (A'=Fe, Co, Ni and Mn, and combinations thereof, with x=1/3) synthesized by an alloy-guided reaction. The simultaneous occupancy of the four magnetic elements and Sn, the individual single-atom-thick A layers in the compound constitute high-entropy-alloy analogues, two-dimensional in the sense that the alloying exclusively occurs in the A layers. V2(A'xSn1-x)C exhibit distinct ferromagnetic behavior that can be compositionally tailored from the multielement A-layer alloying. This two-dimensional alloying provides a structural-design route with expanded chemical space for discovering materials and exploit properties.

cond-mat.mtrl-sci↗