| 1. |
- Mende, Max, et al.
(författare)
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Strong Rashba Effect and Different f−d Hybridization Phenomena at the Surface of the Heavy-Fermion Superconductor CeIrIn 5
- 2022
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Ingår i: Advanced Electronic Materials. - : Wiley. - 2199-160X .- 2199-160X. ; 8:3
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Tidskriftsartikel (refereegranskat)abstract
- New temperature scales and remarkable differences from bulk properties have increasingly placed the surfaces of strongly correlated f materials into the focus of research activities. Applying first-principles calculations and angle-resolved photoelectron spectroscopy measurements, a strong Rashba effect and spin-split surface states at the CeIn surface of the heavy-fermion superconductor CeIrIn5 are revealed. The unveiled 4f-derived electron landscape is remarkably distinct for surface and bulk Ce implying the existence of novel temperature scales near the surface region in this material. These results show that ab initio calculations can reliably predict the unusual electronic and spin structure of surfaces of strongly correlated 4f systems where Rashba spin-orbit-coupling phenomena emerge. It is suggested that the structural blocks of such materials can be combined with magnetically active layers for engineering of novel nanostructural objects with appropriate substrates where the diversity of f-driven properties can be applied for the development of novel functionalities.
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| 2. |
- Mende, Max, et al.
(författare)
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Strong Rashba Effect and Different f−d Hybridization Phenomena at the Surface of the Heavy-Fermion Superconductor CeIrIn5
- 2022
-
Ingår i: Advanced Electronic Materials. - : Wiley. - 2199-160X. ; 8:3
-
Tidskriftsartikel (refereegranskat)abstract
- New temperature scales and remarkable differences from bulk properties have increasingly placed the surfaces of strongly correlated f materials into the focus of research activities. Applying first-principles calculations and angle-resolved photoelectron spectroscopy measurements, a strong Rashba effect and spin-split surface states at the CeIn surface of the heavy-fermion superconductor CeIrIn5 are revealed. The unveiled 4f-derived electron landscape is remarkably distinct for surface and bulk Ce implying the existence of novel temperature scales near the surface region in this material. These results show that ab initio calculations can reliably predict the unusual electronic and spin structure of surfaces of strongly correlated 4f systems where Rashba spin-orbit-coupling phenomena emerge. It is suggested that the structural blocks of such materials can be combined with magnetically active layers for engineering of novel nanostructural objects with appropriate substrates where the diversity of f-driven properties can be applied for the development of novel functionalities.
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| 3. |
- Poelchen, Georg, et al.
(författare)
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Unexpected differences between surface and bulk spectroscopic and implied Kondo properties of heavy fermion CeRh2Si2
- 2020
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Ingår i: npj Quantum Materials. - : Springer Science and Business Media LLC. - 2397-4648. ; 5:1
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Tidskriftsartikel (refereegranskat)abstract
- Ultra-violet angle-resolved photoemission spectroscopy (UV-ARPES) was used to explore the temperature dependence of the Ce-4f spectral responses for surface and bulk in the antiferromagnetic Kondo lattice CeRh2Si2. Spectra were taken from Ce- and Si-terminated surfaces in a wide temperature range, and reveal characteristic 4f patterns for weakly (surface) and strongly (bulk) hybridized Ce, respectively. The temperature dependence of the Fermi level peak differs strongly for both cases implying that the effective Kondo temperature at the surface and bulk can be rather distinct. The greatly reduced crystal–electric-field (CEF) splitting at the surface gives reason to believe that the surface may exhibit a larger effective Kondo temperature because of a higher local-moment effective degeneracy. Further, the hybridization processes could strongly affect the 4f peak intensity at the Fermi level. We derived the k-resolved dispersion of the Kondo peak which is also found to be distinct due to different sets of itinerant bands to which the 4f states of surface and bulk Ce are coupled. Overall our study brings into reach the ultimate goal of quantitatively testing many-body theories that link spectroscopy and transport properties, for both the bulk and the surface, separately. It also allows for a direct insight into the broader problem of Kondo lattices with two different local-moment sublattices, providing some understanding of why the cross-talking between the two Kondo effects is weak.
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| 4. |
- Svirskiy, Gleb I., et al.
(författare)
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Electronic structure of the [Ni(Salen)] complex studied by core-level spectroscopies
- 2021
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Ingår i: Physical Chemistry Chemical Physics. - : Royal Society of Chemistry (RSC). - 1463-9076 .- 1463-9084. ; 23:18, s. 11015-11027
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Tidskriftsartikel (refereegranskat)abstract
- The nature and structure of occupied and empty valence electronic states (molecular orbitals, MOs) of the [Ni(Salen)] molecular complex (NiO2N2C16H14) have been studied by X-ray photoemission and absorption spectroscopy combined with density functional theory (DFT) calculations. As a result, the composition of the high-lying occupied and low-lying unoccupied electronic states has been identified. In particular, the highest occupied molecular orbital (HOMO) of the complex is found to be predominantly located on the phenyl rings of the salen ligand, while the states associated with the occupied Ni 3d-derived molecular orbitals (MOs) are at higher binding energies. The lowest unoccupied molecular orbital (LUMO) is also located on the salen ligand and is formed by the 2pπ orbitals of carbon atoms in phenyl groups of the salen macrocycle. The unoccupied MOs above the LUMO reflect σ- and π-bonding between Ni and its nearest neighbours. All valence states have highly mixed character. The specific nature of the unoccupied Ni 3d-derived σ-MO is a consequence of donor-acceptor chemical bonding in [Ni(Salen)]. This journal is
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| 5. |
- Ahmad, Mariam, et al.
(författare)
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Uncovering the Electronic State Interplay at Metal Oxide Electron Transport Layer/Nonfullerene Acceptor Interfaces in Stable Organic Photovoltaic Devices
- 2023
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Ingår i: ACS Applied Materials and Interfaces. - : American Chemical Society (ACS). - 1944-8244 .- 1944-8252. ; 15:47, s. 55065-55072
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Tidskriftsartikel (refereegranskat)abstract
- The implementation of sputter-deposited TiOx as an electron transport layer in nonfullerene acceptor-based organic photovoltaics has been shown to significantly increase the long-term stability of devices compared to conventional solution-processed ZnO due to a decreased photocatalytic activity of the sputtered TiOx. In this work, we utilize synchrotron-based photoemission and absorption spectroscopies to investigate the interface between the electron transport layer, TiOx prepared by magnetron sputtering, and the nonfullerene acceptor, ITIC, prepared in situ by spray deposition to study the electronic state interplay and defect states at this interface. This is used to unveil the mechanisms behind the decreased photocatalytic activity of the sputter-deposited TiOx and thus also the increased stability of the organic solar cell devices. The results have been compared to similar measurements on anatase TiOx since anatase TiOx is known to have a strong photocatalytic activity. We show that the deposition of ITIC on top of the sputter-deposited TiOx results in an oxidation of Ti3+ species in the TiOx and leads to the emergence of a new O 1s peak that can be attributed to the oxygen in ITIC. In addition, increasing the thickness of ITIC on TiOx leads to a shift in the O 1s and C 1s core levels toward higher binding energies, which is consistent with electron transfer at the interface. Resonant photoemission at the Ti L-edge shows that oxygen vacancies in sputtered TiOx lie mostly in the surface region, which contrasts the anatase TiOx where an equal distribution between surface and subsurface oxygen vacancies is observed. Furthermore, it is shown that the subsurface oxygen vacancies in sputtered TiOx are strongly reduced after ITIC deposition, which can reduce the photocatalytic activity of the oxide, while the oxygen vacancies in model anatase TiOx are not affected upon ITIC deposition. This difference can explain the inferior photocatalytic activity of the sputter-deposited TiOx and thus also the increased stability of devices with sputter-deposited TiOx used as an electron transport layer.
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| 6. |
- Beyer, Paul, et al.
(författare)
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Fermi level pinned molecular donor/acceptor junctions : Reduction of induced carrier density by interfacial charge transfer complexes
- 2020
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Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry (RSC). - 2050-7534 .- 2050-7526. ; 8:43, s. 15199-15207
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Tidskriftsartikel (refereegranskat)abstract
- Increased hole density in an electron donor-type organic semiconductor can be achieved by deposition of a strong acceptor-type molecular layer on top, and has been shown to enable adjusting the carrier density in organic field effect transistors (OFETs). This interfacial charge transfer is due to simultaneous Fermi level (EF) pinning of the donor's highest occupied level and the acceptor's lowest unoccupied level. Here, we investigate the electrical properties of such an EF-pinned junction formed by diindenoperylene (DIP, as donor) and hexafluoro-tetracyano-naphthoquinodimethane (F6, as acceptor) in OFETs, as well as its electronic properties by photoelectron spectroscopy and electrostatic modelling. We find that, in addition to the EF-pinning induced integer charge transfer across the interface, DIP and F6 form charge transfer complexes (CPXs) at their junction. The molecularly thin CPX interlayer acts as insulator and significantly reduces the density of carriers induced on either side of the junction, compared to a scenario without such an interlayer. CPX formation is thus unfavourable for the effectiveness of controlling carrier density at molecular donor/acceptor junctions by EF-pinning. This journal is
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| 7. |
- Larsson, Alfred, et al.
(författare)
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Dynamics of early-stage oxide formation on a Ni-Cr-Mo alloy
- 2024
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Ingår i: NPJ MATERIALS DEGRADATION. - : Springer Nature. - 2397-2106. ; 8:1
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Tidskriftsartikel (refereegranskat)abstract
- Corrosion results in large costs and environmental impact but can be controlled by thin oxide films that passivate the metal surfaces and hinder further oxidation or dissolution in an aqueous environment. The structure, chemistry, and thickness of these oxide films play a significant role in determining their anti-corrosion properties and the early-stage oxidation dynamics affect the properties of the developed oxide. Here, we use in situ X-ray Photoelectron Spectroscopy (XPS) to study the early-stage oxidation of a Ni-Cr-Mo alloy at room temperature and up to 400 degrees C. Cr and Mo begin to oxidize immediately after exposure to O2, and Cr3+, Mo4+, and Mo6+ oxides are formed. In contrast, Ni does not contribute significantly to the oxide film. A self-limiting oxide thickness, which did not depend on temperature below 400 degrees C, is observed. This is attributed to the consumption of available Cr and Mo near the surface, which results in an enrichment of metallic Ni under the oxide. The self-limited oxide thickness is 6-8 angstrom, which corresponds to 3-4 atomic layers of cations in the oxide. At 400 degrees C, sublimation of Mo6+ oxide is observed, resulting in the formation of an almost pure layer of Cr2O3 on the alloy surface. Lastly, a mechanism is presented that explains the formation of the bi-layer oxide structure observed for Ni-Cr-Mo alloys, which involves the enhanced migration of hexavalent Mo ions in the electric field, which drives mass transport during oxidation according to both the Cabrera Mott model and the Point Defect Model.
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| 8. |
- Poelchen, Georg, et al.
(författare)
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Interlayer Coupling of a Two-Dimensional Kondo Lattice with a Ferromagnetic Surface in the Antiferromagnet CeCo2P2
- 2022
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Ingår i: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 16:3, s. 3573-3581
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Tidskriftsartikel (refereegranskat)abstract
- The f-driven temperature scales at the surfaces of strongly correlated materials have increasingly come into the focus of research efforts. Here, we unveil the emergence of a two-dimensional Ce Kondo lattice, which couples ferromagnetically to the ordered Co lattice below the P-terminated surface of the antiferromagnet CeCo2P2. In its bulk, Ce is passive and behaves tetravalently. However, because of symmetry breaking and an effective magnetic field caused by an uncompensated ferromagnetic Co layer, the Ce 4f states become partially occupied and spin-polarized near the surface. The momentum-resolved photoemission measurements indicate a strong admixture of the Ce 4f states to the itinerant bands near the Fermi level including surface states that are split by exchange interaction with Co. The temperature-dependent measurements reveal strong changes of the 4f intensity at the Fermi level in accordance with the Kondo scenario. Our findings show how rich and diverse the f-driven properties can be at the surface of materials without f-physics in the bulk.
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| 9. |
- Pramanik, Arindam, et al.
(författare)
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Dirac states in the noncentrosymmetric superconductor BiPd
- 2021
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Ingår i: Physical Review B. - 2469-9950. ; 103:15
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Tidskriftsartikel (refereegranskat)abstract
- Quantum materials having Dirac fermions in conjunction with superconductivity is believed to be the candidate material to realize exotic physics as well as advanced technology. Angle-resolved photoemission spectroscopy (ARPES), a direct probe of the electronic structure, has been extensively used to study these materials. However, experiments often exhibit conflicting results on dimensionality and momentum of the Dirac fermions (e.g., Dirac states in BiPd, a novel noncentrosymmetric superconductor), which is crucial for the determination of the symmetry, time-reversal invariant momenta, and other emerging properties. Employing high-resolution ARPES at varied conditions, we demonstrated a methodology to identify the location of the Dirac node accurately and discover that the deviation from two dimensionality of the Dirac states in BiPd proposed earlier is not a material property. These results helped to reveal the topology of the anisotropy of the Dirac states accurately. We have constructed a model Hamiltonian considering higher-order spin-orbit terms and demonstrate that this model provides an excellent description of the observed anisotropy. Intriguing features of the Dirac states in a noncentrosymmetric superconductor revealed in this study are expected to have significant implications regarding the properties of topological superconductors.
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| 10. |
- Pramanik, Arindam, et al.
(författare)
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Surface states in noncentrosymmetric superconductor BiPd
- 2022
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Ingår i: Journal of Physics: Conference Series. - : IOP Publishing. - 1742-6588 .- 1742-6596. ; 2164
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Konferensbidrag (refereegranskat)abstract
- BiPd is a noncentrosymmetric superconductor with Dirac-like surface states on both (010) and (01¯0) faces. The Dirac cone on (010) surface is intense and appears at 0.66 eV binding energy. These states have drawn much attention due to contradictory reports on dimensionality and the momentum of these Dirac fermions. We have studied the properties of these Dirac fermions using varied photon energies and different experimental conditions. The behavior of the Dirac cone is found to be two-dimensional. In addition, we found few more surface states appearing at higher binding energies compared to the Dirac cone.
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