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Sufyan, A., Sajjad, M. & Larsson, J. A. (2024). Evaluating the potential of planar checkerboard lattice Cu2N monolayer as anode material for lithium and sodium-ion batteries using first-principles methods. Applied Surface Science, 654, Article ID 159474.
Open this publication in new window or tab >>Evaluating the potential of planar checkerboard lattice Cu2N monolayer as anode material for lithium and sodium-ion batteries using first-principles methods
2024 (English)In: Applied Surface Science, ISSN 0169-4332, E-ISSN 1873-5584, Vol. 654, article id 159474Article in journal (Refereed) Published
Abstract [en]

We present first-principles insights into the electrical and electrochemical properties of Cu2N, a newly synthesized two-dimensional material that features a planar, checkerboard lattice structure [Hu et al., Nano Lett. 2023, 23 (12), 5610–5616]. We evaluate the suitability of monolayer Cu2N as an anode material for Li and Na-ion batteries by examining its storage capacity, diffusion barrier, open-circuit voltage (OCV), volume expansion, and the impact of defects on its electrochemical performance. The monolayer Cu2N demonstrates a storage capacity of 379.88 mAh.g−1 for both Li and Na, comparable to that of commercial graphite for Li (372 mAh.g−1) and significantly higher for Na (less than 35 mAh.g−1). The migration barriers for Li and Na are found to be 0.1 eV and 0.01 eV, respectively, substantially lower than those theoretically reported for commercial anodes TiO2 (0.4–1.0 eV) and graphite (∼0.4 eV), which imply that monolayer Cu2N demonstrates excellent charge/discharge capabilities. Moreover, the volume growth of monolayer Cu2N is 4.14 % with maximal Li adsorption, which is 2.4 times less than graphite. The analysis of vacancy defects reveals a significant enhancement in the binding energies of Li and Na atoms, accompanied by minimal changes in diffusion barriers. Since monolayer Cu2N has already been successfully synthesized, these findings would pave the way for large-scale experimental fabrication of monolayer Cu2N as a battery anode.

Place, publisher, year, edition, pages
Elsevier B.V., 2024
Keywords
Anode material, Checkerboard lattice, Density functional theory calculations, High stability, Metal-ion batteries, Monolayer Cu2N, Ultra-low diffusion barrier
National Category
Condensed Matter Physics Materials Chemistry
Research subject
Applied Physics
Identifiers
urn:nbn:se:ltu:diva-104178 (URN)10.1016/j.apsusc.2024.159474 (DOI)2-s2.0-85183453929 (Scopus ID)
Note

Funder: Swedish Research Council (2018-05973); Array (2018-05973);

Full text license: CC BY

Available from: 2024-02-05 Created: 2024-02-05 Last updated: 2024-02-05
Sufyan, A., Abbas, G., Sajjad, M. & Larsson, A. (2024). Monolayer TiC—A high-performance Dirac anode with ultralow diffusion barriers and high energy densities for Li-ion and Na-ion batteries. Applied Surface Science, 642, Article ID 158564.
Open this publication in new window or tab >>Monolayer TiC—A high-performance Dirac anode with ultralow diffusion barriers and high energy densities for Li-ion and Na-ion batteries
2024 (English)In: Applied Surface Science, ISSN 0169-4332, E-ISSN 1873-5584, Vol. 642, article id 158564Article in journal (Refereed) Published
Abstract [en]

Two-dimensional Dirac materials have stimulated substantial research interest as binder-free anodes in metal-ion batteries, owing to their ultrahigh electronic conductivity, large specific area, and higher energy density. Here, using first-principles density functional theory calculations, we have investigated the feasibility of monolayer TiC as a potential anode material for Li/Na-ion batteries. The results indicate that monolayer TiC exhibits excellent dynamical and thermal stability. The electronic structure of monolayer TiC shows semimetallic characteristics with a Dirac cone at the M high symmetry point and the formation of Ti or C vacancies transforms the Dirac cone into a nodal loop or a nodal surface, respectively. Thus, monolayer TiC possesses superior electrical conductivity, which can be further enhanced by the formation of Ti or C vacancies in the material. Furthermore, the calculated adsorption energy values of -0.85 and -0.46 eV for Li-ion and Na-ion, respectively, indicate that Li/Na atom adsorption over monolayer TiC is a favorable process. The density of states plots show that after the adsorption of a single Li/Na atom, monolayer TiC maintains its metallic state, which is advantageous for the diffusion of stored electrons. Most remarkably, monolayer TiC exhibits energy densities of 2684 and 2015 mWh/g for Li and Na, respectively, which are significantly higher than commercial graphite and most other 2D anode materials. The fully loaded TiC anode exhibits excellent cycle stability with volume expansions as low as 0.13 and 0.11%, for Li and Na, respectively. Furthermore, an ultrafast diffusivity with low energy barriers of 0.02 and 0.10 eV is found in monolayer TiC for Li-ion and Na-ion, respectively, which suggests that it has an excellent charge/discharge capability. These exceptional properties make monolayer TiC an excellent candidate as an anode material for Li-ion and Na-ion batteries. Finally, SiC(111) has been proposed as a candidate substrate for monolayer TiC due to its minimal lattice mismatch.

Place, publisher, year, edition, pages
Elsevier B.V., 2024
Keywords
2D Dirac anode, Energy barrier, Energy density, First-principles calculations, Lithium-ion and sodium-ion batteries
National Category
Condensed Matter Physics
Research subject
Applied Physics
Identifiers
urn:nbn:se:ltu:diva-101666 (URN)10.1016/j.apsusc.2023.158564 (DOI)2-s2.0-85173161851 (Scopus ID)
Funder
Knut and Alice Wallenberg FoundationThe Kempe Foundations
Note

Validerad;2023;Nivå 2;2023-10-16 (joosat);

CC BY 4.0 License

Available from: 2023-10-16 Created: 2023-10-16 Last updated: 2023-10-16Bibliographically approved
Zulfiqar, W., Javed, F., Abbas, G., Larsson, J. A. & Alay-e-Abbas, S. M. (2024). Stabilizing the dopability of chalcogens in BaZrO3 through TiZr co-doping and its impact on the opto-electronic and photocatalytic properties: A meta-GGA level DFT study. International journal of hydrogen energy, 58, 409-415
Open this publication in new window or tab >>Stabilizing the dopability of chalcogens in BaZrO3 through TiZr co-doping and its impact on the opto-electronic and photocatalytic properties: A meta-GGA level DFT study
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2024 (English)In: International journal of hydrogen energy, ISSN 0360-3199, E-ISSN 1879-3487, Vol. 58, p. 409-415Article in journal (Refereed) Published
Abstract [en]

Since introducing isovalent cation and anion co-dopants in ABO3 perovskite can facilitate tuning of their band gaps, in the present work we examine the synthesis feasibility of Ti and X (where X = S, Se and Te) dopants at zirconium and oxygen-sites, respectively, of BaZrO3 using first-principles density functional theory calculations. For an accurate determination of thermodynamic, structural and energetic properties of the pristine, mono-doped and TiZr + XO co-doped BaZrO3, we have employed semi-local SCAN meta-GGA functional. Moreover, the TB-mBJ meta-GGA potential functional was used to circumvent the band gap underestimation of the electronic and optical properties made by SCAN. Our results indicate that introducing TiZr as a co-dopant in XO-doped BaZrO3 not only improves the thermodynamics of introducing an chalcogen atom at oxygen-site under optimal chemical environment, it also allows tuning the band gap of cubic BaZrO3 for absorption of radiation in the visible spectrum. We also perform a side-by-side comparison of the photocatalytic water molecule dissociation efficiency of pristine, XO-doped, TiZr-doped and TiZr +XO co-doped BaZrO3 to examine their potential application in hydrogen evolution process. Based on our computed optical properties and band-edge potentials, we propose TiZr+TeO co-doped BaZrO3 as the best candidate for photocatalytic water molecule dissociation under solar irradiation.

Place, publisher, year, edition, pages
Elsevier Ltd, 2024
Keywords
Co-doping, Perovskite oxide, Photocatalyst, Water molecule dissociation
National Category
Condensed Matter Physics Theoretical Chemistry
Identifiers
urn:nbn:se:ltu:diva-104171 (URN)10.1016/j.ijhydene.2024.01.202 (DOI)2-s2.0-85183059083 (Scopus ID)
Funder
Swedish Research Council, 2018–05973
Note

Funder: Higher Education Commission of Pakistan for National Research Program for Universities (7107/Punjab/NRPU/R&D/HEC/2017)

Available from: 2024-02-05 Created: 2024-02-05 Last updated: 2024-02-05
Talwelkar Shimpi, M., Sajjad, M., Öberg, S. & Larsson, J. A. (2023). Physical binding energies using the electron localization function in 4-hydroxyphenylboronic acid co-crystals with aza donors. Journal of Physics: Condensed Matter, 35(50), Article ID 505901.
Open this publication in new window or tab >>Physical binding energies using the electron localization function in 4-hydroxyphenylboronic acid co-crystals with aza donors
2023 (English)In: Journal of Physics: Condensed Matter, ISSN 0953-8984, E-ISSN 1361-648X, Vol. 35, no 50, article id 505901Article in journal (Refereed) Published
Abstract [en]

Binding energies are traditionally simulated using cluster models by computation of each synthon for each individual co-crystal former. However, our investigation of the binding strengths using the electron localization function (ELF) reveals that these can be determined directly from the crystal supercell computations. We propose a new modeling protocol for the computation of physical binding energies directly from bulk simulations using ELF analysis. In this work, we establish a correlation between ELF values and binding energies calculated for co-crystals of 4-hydroxyphenylboronic acid (4HPBA) with four different aza donors using density functional theory with varying descriptions of dispersion. Boronic acids are gaining significant interest in the field of crystal engineering, but theoretical studies on their use in materials are still very limited. Here, we present a systematic investigation of the non-covalent interactions in experimentally realized co-crystals. Prior diffraction studies on these complexes have shown the competitive nature between the boronic acid functional group and the para-substituted phenolic group forming heteromeric interactions with aza donors. We determine the stability of the co-crystals by simulating their lattice energies, and the different dispersion descriptions show similar trends in lattice energies and lattice parameters. Our study bolsters the experimental observation of the boronic acid group as a competitive co-crystal former in addition to the well-studied phenolic group. Further research on correlating ELF values for physical binding could potentially transform this approach to a viable alternative for the computation of binding energies.

Place, publisher, year, edition, pages
Institute of Physics (IOP), 2023
Keywords
binding energy, co-crystals, dispersion corrected DFT, ELF, hydrogen-bonds, lattice energy
National Category
Condensed Matter Physics Theoretical Chemistry
Research subject
Applied Physics
Identifiers
urn:nbn:se:ltu:diva-101863 (URN)10.1088/1361-648X/acf638 (DOI)001068765700001 ()37659400 (PubMedID)2-s2.0-85171600035 (Scopus ID)
Funder
Knut and Alice Wallenberg FoundationThe Kempe Foundations
Note

Validerad;2023;Nivå 2;2023-10-31 (hanlid);

Licens full text: CC BY

Available from: 2023-10-31 Created: 2023-10-31 Last updated: 2023-10-31Bibliographically approved
Abbas, G., Johansson, G., Alay-e-Abbas, S. M., Shi, Y. & Larsson, J. A. (2023). Quasi Three-Dimensional Tetragonal SiC Polymorphs as Efficient Anodes for Sodium-Ion Batteries. ACS Applied Energy Materials, 6(17), 8976-8988
Open this publication in new window or tab >>Quasi Three-Dimensional Tetragonal SiC Polymorphs as Efficient Anodes for Sodium-Ion Batteries
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2023 (English)In: ACS Applied Energy Materials, E-ISSN 2574-0962, Vol. 6, no 17, p. 8976-8988Article in journal (Refereed) Published
Abstract [en]

In the present work, we investigate, for the first time, quasi 3D porous tetragonal silicon–carbon polymorphs t(SiC)12 and t(SiC)20 on the basis of first-principles density functional theory calculations. The structural design of these q3-t(SiC)12 and q3-t(SiC)20 polymorphs follows an intuitive rational approach based on armchair nanotubes of a tetragonal SiC monolayer where C–C and Si–Si bonds are arranged in a paired configuration for retaining a 1:1 ratio of the two elements. Our calculations uncover that q3-t(SiC)12 and q3-t(SiC)20 polymorphs are thermally, dynamically, and mechanically stable with this lattice framework. The results demonstrate that the smaller polymorph q3-t(SiC)12 shows a small band gap (∼0.59 eV), while the larger polymorph of q3-t(SiC)20 displays a Dirac nodal line semimetal. Moreover, the 1D channels are favorable for accommodating Na ions with excellent (>300 mAh g–1) reversible theoretical capacities. Thus confirming potential suitability of the two porous polymorphs with an appropriate average voltage and vanishingly small volume change (<6%) as anodes for Na-ion batteries.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2023
Keywords
SiC polymorphs, Na-ion battery, anode material, density functional theory, first principles
National Category
Theoretical Chemistry Condensed Matter Physics
Research subject
Applied Physics; Machine Elements
Identifiers
urn:nbn:se:ltu:diva-100745 (URN)10.1021/acsaem.3c01703 (DOI)2-s2.0-85170284081 (Scopus ID)
Funder
The Kempe FoundationsKnut and Alice Wallenberg Foundation
Note

Validerad;2023;Nivå 2;2023-11-13 (hanlid);

Full text license: CC BY

Available from: 2023-08-28 Created: 2023-08-28 Last updated: 2023-11-13Bibliographically approved
Alay-e-Abbas, S. M., Abbas, G., Zulfiqar, W., Sajjad, M., Singh, N. & Larsson, J. A. (2023). Structure inversion asymmetry enhanced electronic structure and electrical transport in 2D A3SnO (A = Ca, Sr, and Ba) anti-perovskite monolayers. Nano Reseach, 16(1), 1779-1791
Open this publication in new window or tab >>Structure inversion asymmetry enhanced electronic structure and electrical transport in 2D A3SnO (A = Ca, Sr, and Ba) anti-perovskite monolayers
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2023 (English)In: Nano Reseach, ISSN 1998-0124, E-ISSN 1998-0000, Vol. 16, no 1, p. 1779-1791Article in journal (Refereed) Published
Abstract [en]

Anti-perovskites A3SnO (A = Ca, Sr, and Ba) are an important class of materials due to the emergence of Dirac cones and tiny mass gaps in their band structures originating from an intricate interplay of crystal symmetry, spin-orbit coupling, and band overlap. This provides an exciting playground for modulating their electronic properties in the two-dimensional (2D) limit. Herein, we employ first-principles density functional theory (DFT) calculations by combining dispersion-corrected SCAN + rVV10 and mBJ functionals for a comprehensive side-by-side comparison of the structural, thermodynamic, dynamical, mechanical, electronic, and thermoelectric properties of bulk and monolayer (one unit cell thick) A3SnO anti-perovskites. Our results show that 2D monolayers derived from bulk A3SnO anti-perovskites are structurally and energetically stable. Moreover, Rashba-type splitting in the electronic structure of Ca3SnO and Sr3SnO monolayers is observed owing to strong spin-orbit coupling and inversion asymmetry. On the other hand, monolayer Ba3SnO exhibits Dirac cone at the high-symmetry Γ point due to the domination of band overlap. Based on the predicted electronic transport properties, it is shown that inversion asymmetry plays an essential character such that the monolayers Ca3SnO and Sr3SnO outperform thermoelectric performance of their bulk counterparts.

Place, publisher, year, edition, pages
Springer Nature, 2023
Keywords
electrical transport, anti-perovskites, low-dimensional materials, electronic structure, mechanical properties
National Category
Materials Chemistry Atom and Molecular Physics and Optics
Research subject
Applied Physics
Identifiers
urn:nbn:se:ltu:diva-92203 (URN)10.1007/s12274-022-4637-3 (DOI)000824315800001 ()2-s2.0-85134331945 (Scopus ID)
Funder
Knut and Alice Wallenberg FoundationThe Kempe FoundationsSwedish Research Council, 2018-05973
Note

Validerad;2023;Nivå 2;2023-04-20 (hanlid)

Available from: 2022-07-19 Created: 2022-07-19 Last updated: 2023-09-05Bibliographically approved
Sufyan, A. & Larsson, J. A. (2023). Topological Nodal Surface and Quadratic Dirac Semimetal States and van Hove Singularities in ScH3 and LuH3 Superconductors. ACS Omega, 8(10), 9607-9613
Open this publication in new window or tab >>Topological Nodal Surface and Quadratic Dirac Semimetal States and van Hove Singularities in ScH3 and LuH3 Superconductors
2023 (English)In: ACS Omega, E-ISSN 2470-1343, Vol. 8, no 10, p. 9607-9613Article in journal (Refereed) Published
Abstract [en]

The coexistence of non-trivial topology and superconductivity in a material may induce a novel physical phenomenon known as topological superconductivity. Topological superconductors have been the subject of intense research, yet there are severe limitations in their application due to a lack of suitable materials. Topological nodal surface semimetals with nearly flat nodal surfaces near the Fermi level can be promising materials to achieve topological superconductivity. Here, we use first-principles calculations to examine the topological electronic characteristics of two new superconductors, ScH3 and LuH3, at both ambient and high pressures. Our studies show that both ScH3 and LuH3 have van Hove singularities, which confirms their superconductivity. Interestingly, both materials host topological nodal surface states under the protection of time reversal and spatial inversion symmetries in the absence of spin–orbit coupling (SOC). These nodal surfaces are distinguished by a pair of unique drum-head-like surface states not previously observed in nodal surface semimetals. Moreover, the nodal surfaces transform into essential spin–orbit quadratic Dirac points when SOC is included. Our findings demonstrate that ScH3 and LuH3 are good candidates to investigate the exotic properties of both nodal surface semimetals (NSSMs) and quadratic Dirac semimetal states and also provide a platform to explore the coexistence of topology and superconductivity in NSSMs with promising applications in high-speed electronics and topological quantum computing.

Place, publisher, year, edition, pages
American Chemical Society, 2023
National Category
Condensed Matter Physics
Research subject
Applied Physics
Identifiers
urn:nbn:se:ltu:diva-95855 (URN)10.1021/acsomega.3c00207 (DOI)000942632000001 ()36936326 (PubMedID)2-s2.0-85149152460 (Scopus ID)
Funder
The Kempe FoundationsSwedish Research Council, 2018-05973Knut and Alice Wallenberg Foundation
Note

Validerad;2023;Nivå 2;2023-04-18 (joosat);

Licens fulltext: CC BY License

Available from: 2023-03-13 Created: 2023-03-13 Last updated: 2023-09-05Bibliographically approved
Sajjad, M., Badawy, K., Larsson, A., Umer, R. & Singh, N. (2023). Two dimensional holey graphyne: An excellent anode and anchoring material for metal–ion and metal–sulfur batteries. Carbon, 214, Article ID 118340.
Open this publication in new window or tab >>Two dimensional holey graphyne: An excellent anode and anchoring material for metal–ion and metal–sulfur batteries
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2023 (English)In: Carbon, ISSN 0008-6223, E-ISSN 1873-3891, Vol. 214, article id 118340Article in journal (Refereed) Published
Abstract [en]

Based on first-principles calculations, the potential of holey graphyne is investigated for battery applications in terms of the storage capacity, volume expansion, diffusion barrier, and metal polysulfides binding. We found substantially higher storage capacities of Li (873 mAh/g) and Na (558 mAh/g) than typical graphite anodes (372 mAh/g for Li and <35 mAh/g for Na) and other carbonaceous materials (450–750 mAh/g for Li and 200–500 mAh/g for Na). The migration barriers of Li and Na turn out to be 0.28 eV and 0.32 eV, respectively, lower than those theoretically reported for commercial anodes TiO2 (0.4–1.0 eV) and silicon (0.6–0.8 eV). Holey graphyne with maximum Li adsorption expands only 0.5%, in contrast to the 10% volume growth in graphite. The lithium and sodium polysulfides and S8 cluster adsorb with moderate binding energies ranging from −0.73 eV to −2.08 eV, which is sufficient to prevent the unintended decomposition of polysulfides. Our findings demonstrate that holey graphyne is a promising anode material for metal-ion batteries and an anchoring material for metal-sulfur batteries to mitigate the shuttle effect.

Place, publisher, year, edition, pages
Elsevier, 2023
Keywords
Porous holey graphyne, Anode material, Anchoring material, Metal-ion batteries, Metal-sulfur batteries
National Category
Metallurgy and Metallic Materials
Research subject
Applied Physics
Identifiers
urn:nbn:se:ltu:diva-99705 (URN)10.1016/j.carbon.2023.118340 (DOI)2-s2.0-85169603425 (Scopus ID)
Funder
Knut and Alice Wallenberg FoundationThe Kempe FoundationsSwedish Research Council, 2018–05973
Note

Validerad;2023;Nivå 2;2023-08-15 (joosat);

Licens fulltext: CC BY-NC-ND License

Funder: Khalifa University of Science and Technology (CIRA-2020-007), (ESIG-2023-004);

Available from: 2023-08-15 Created: 2023-08-15 Last updated: 2023-10-11Bibliographically approved
Fadaei Naeini, V., Björling, M., Larsson, A. & Larsson, R. (2023). Unraveling the pressure-viscosity behavior and shear thinning in glycerol using atomic scale molecular dynamics simulations. Journal of Molecular Liquids, 390(part A), Article ID 122990.
Open this publication in new window or tab >>Unraveling the pressure-viscosity behavior and shear thinning in glycerol using atomic scale molecular dynamics simulations
2023 (English)In: Journal of Molecular Liquids, ISSN 0167-7322, E-ISSN 1873-3166, Vol. 390, no part A, article id 122990Article in journal (Refereed) Published
Abstract [en]

In order to increase the usage and explore new applications of glycerol as a replacement for fossil-based lubricants its properties needs to be known at the fundamental level. In this study, the viscosity of pure glycerol at high pressures and strain rates has been investigated using of molecular dynamics (MD) simulations, utilizing both the Green-Kubo (GK) formalism and the SLLOD algorithm. Although the viscosity acquired by the GK method is in agreement with the corresponding experimental values at low pressure, a significant distinction was identified between the viscosity obtained by the GK method and the experimental values at higher pressures (P > 0.5 GPa). This results in a clear difference between the viscosity-pressure coefficient attained by the GK method and the corresponding experimental value. The SLLOD method using a non-equilibrium MD (NEMD) platform was exploited to take into account the simultaneous effects of strain rate and pressure on viscosity. As a result, the pressure-viscosity coefficient acquired by the SLLOD algorithm approaches the experimental value. By combining the experimental outputs for viscosity at low strain rates ( < 104 s−1) with the SLLOD outputs at higher rates ( > 105 s−1), the evolutions of glycerol viscosity with pressure and strain rate were ultimately achieved. Implementing this computational platform depicts the shear thinning process in pure glycerol in a wide range of pressures and strain rates.

Place, publisher, year, edition, pages
Elsevier, 2023
Keywords
Glycerol, Pressure-viscosity coefficient, Green-Kubo Formalism, SLLOD algorithm, Shear thinning, Molecular dynamics simulation
National Category
Condensed Matter Physics
Research subject
Machine Elements; Applied Physics
Identifiers
urn:nbn:se:ltu:diva-102857 (URN)10.1016/j.molliq.2023.122990 (DOI)2-s2.0-85171625047 (Scopus ID)
Funder
The Kempe Foundations, JCK-1903.2Knut and Alice Wallenberg FoundationSwedish Research Council, 2021-05621
Note

Validerad;2023;Nivå 2;2023-11-23 (joosat);

CC BY 4.0 License

Available from: 2023-11-23 Created: 2023-11-23 Last updated: 2023-11-23Bibliographically approved
Sufyan, A., Abbas, G. G., Sajjad, M. & Larsson, J. A. (2023). V4C3 MXene: a Type‐II Nodal Line Semimetal with Potential as High‐Performing Anode Material for Mg‐Ion Battery. ChemSusChem, Article ID e202301351.
Open this publication in new window or tab >>V4C3 MXene: a Type‐II Nodal Line Semimetal with Potential as High‐Performing Anode Material for Mg‐Ion Battery
2023 (English)In: ChemSusChem, ISSN 1864-5631, E-ISSN 1864-564X, article id e202301351Article in journal (Refereed) Accepted
Place, publisher, year, edition, pages
John Wiley & Sons, 2023
National Category
Other Materials Engineering
Research subject
Applied Physics
Identifiers
urn:nbn:se:ltu:diva-103203 (URN)10.1002/cssc.202301351 (DOI)
Funder
Knut and Alice Wallenberg FoundationThe Kempe Foundations
Available from: 2023-12-05 Created: 2023-12-05 Last updated: 2023-12-05
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Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0003-3455-2877

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