| 1. |
- Posey, Victoria A., et al.
(författare)
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Two-dimensional heavy fermions in the van der Waals metal CeSiI
- 2024
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Ingår i: Nature. - : Springer Nature. - 0028-0836 .- 1476-4687. ; 625:7995, s. 483-488
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Tidskriftsartikel (refereegranskat)abstract
- Heavy-fermion metals are prototype systems for observing emergent quantum phases driven by electronic interactions1-6. A long-standing aspiration is the dimensional reduction of these materials to exert control over their quantum phases7-11, which remains a significant challenge because traditional intermetallic heavy-fermion compounds have three-dimensional atomic and electronic structures. Here we report comprehensive thermodynamic and spectroscopic evidence of an antiferromagnetically ordered heavy-fermion ground state in CeSiI, an intermetallic comprising two-dimensional (2D) metallic sheets held together by weak interlayer van der Waals (vdW) interactions. Owing to its vdW nature, CeSiI has a quasi-2D electronic structure, and we can control its physical dimension through exfoliation. The emergence of coherent hybridization of f and conduction electrons at low temperature is supported by the temperature evolution of angle-resolved photoemission and scanning tunnelling spectra near the Fermi level and by heat capacity measurements. Electrical transport measurements on few-layer flakes reveal heavy-fermion behaviour and magnetic order down to the ultra-thin regime. Our work establishes CeSiI and related materials as a unique platform for studying dimensionally confined heavy fermions in bulk crystals and employing 2D device fabrication techniques and vdW heterostructures12 to manipulate the interplay between Kondo screening, magnetic order and proximity effects.
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| 2. |
- Chang, Yueqing, et al.
(författare)
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Downfolding from ab initio to interacting model Hamiltonians : comprehensive analysis and benchmarking of the DFT+cRPA approach
- 2024
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Ingår i: npj Computational Materials. - 2057-3960. ; 10:1
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Tidskriftsartikel (refereegranskat)abstract
- Model Hamiltonians are regularly derived from first principles to describe correlated matter. However, the standard methods for this contain a number of largely unexplored approximations. For a strongly correlated impurity model system, here we carefully compare a standard downfolding technique with the best possible ground-truth estimates for charge-neutral excited-state energies and wave functions using state-of-the-art first-principles many-body wave function approaches. To this end, we use the vanadocene molecule and analyze all downfolding aspects, including the Hamiltonian form, target basis, double-counting correction, and Coulomb interaction screening models. We find that the choice of target-space basis functions emerges as a key factor for the quality of the downfolded results, while orbital-dependent double-counting corrections diminish the quality. Background screening of the Coulomb interaction matrix elements primarily affects crystal-field excitations. Our benchmark uncovers the relative importance of each downfolding step and offers insights into the potential accuracy of minimal downfolded model Hamiltonians.
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| 3. |
- Keshavarz, Samara, et al.
(författare)
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Electronic structure, magnetism, and exchange integrals in transition-metal oxides : Role of the spin polarization of the functional in DFT+U calculations
- 2018
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Ingår i: Physical Review B. - 2469-9950 .- 2469-9969. ; 97:18
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Tidskriftsartikel (refereegranskat)abstract
- Density functional theory augmented with Hubbard-U corrections (DFT+U) is currently one of the most widely used methods for first-principles electronic structure modeling of insulating transition-metal oxides (TMOs). Since U is relatively large compared to bandwidths, the magnetic excitations in TMOs are expected to be well described by a Heisenberg model. However, in practice the calculated exchange parameters J(ij) depend on the magnetic configuration from which they are extracted and on the functional used to compute them. In this work we investigate how the spin polarization dependence of the underlying exchange-correlation functional influences the calculated magnetic exchange constants of TMOs. We perform a systematic study of the predictions of calculations based on the local density approximation plus U (LDA+U) and the local spin density approximation plus U (LSDA+U) for the electronic structures, total energies, and magnetic exchange interactions Jij extracted from ferromagnetic (FM) and antiferromagnetic (AFM) configurations of several transition-metal oxide materials. We report that for realistic choices of Hubbard U and Hund's J parameters, LSDA+U and LDA+U calculations result in different values of the magnetic exchange constants and band gap. The dependence of the band gap on the magnetic configuration is stronger in LDA+U than in LSDA+U and we argue that this is the main reason why the configuration dependence of Jij is found to be systematically more pronounced in LDA+U than in LSDA+U calculations. We report a very good correspondence between the computed total energies and the parametrized Heisenberg model for LDA+U calculations, but not for LSDA+U, suggesting that LDA+U is a more appropriate method for estimating exchange interactions.
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| 4. |
- Werner, Philipp, et al.
(författare)
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Satellites and large doping and temperature dependence of electronic properties in hole-doped BaFe2As2
- 2012
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Ingår i: Nature Physics. - 1745-2473. ; 8:4, s. 331-337
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Tidskriftsartikel (refereegranskat)abstract
- Superconductivity has recently been discovered in several families of iron-based compounds, but despite intense research even such basic electronic properties of these materials as Fermi surfaces, effective electron masses and orbital characters are still subject to debate. Here, we address an issue that has not been considered before, namely the consequences of dynamical screening of the Coulomb interactions between Fe d electrons. We demonstrate that dynamical screening effects are important not only for higher-energy spectral features, such as correlation satellites seen in photoemission spectroscopy, but also for the low-energy electronic structure. Our analysis indicates that BaFe2As2 is a strongly correlated compound with strongly doping- and temperature-dependent properties. In the hole-overdoped regime an incoherent metal is found, whereas Fermi-liquid behaviour is recovered in the undoped compound. At optimal doping, the self-energy exhibits an unusual square-root energy dependence, which leads to strong band renormalizations near the Fermi level.
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