| 1. |
- Denoel, Fernand
(författare)
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Electronic and magnetic properties of Tsai quasicrystals and their approximants under pressure
- 2022
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Licentiatavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Quasicrystals constitute a special category of crystals exhibiting long-range order without periodicity. This strange feature allows them to exhibit rotational symmetries prohibited in regular crystals, such as 5-, 8-, 10- or 12-fold symmetry. Amongst them, icosahedral quasicrystals are the only type that is aperiodic along all 3 dimensions. The present work will focus on Tsai-Type quasicrystals and their approximants, which are the most studied type of icosahedral quasicrystals. We will introduce how they can be generated froma hyperspace perspective, their exotic structure and how it relates to their physical properties. Pressure is a key parameter which can be used to alter the condensed matter properties of a material. By reducing the size of samples and using diamond anvil cells, it is possible to obtain the highest experimentally achievable pressures and collect informations such as magnetization, electrical resistivity or Raman signal. This work will introduce the specialized diamond anvil cells we used to investigate electron transport and magnetization under pressure, explain in details how to circumvent the most common difficulties arising with high pressure setups. and describe how high pressure affects Tsai quasicrystals and approximants in terms of structure and magnetic properties.
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| 2. |
- Denoel, Fernand, et al.
(författare)
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Eu Doping in the GdCd7.88 Quasicrystal and Its Approximant Crystal GdCd6
- 2024
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Ingår i: Inorganic Chemistry. - : American Chemical Society (ACS). - 0020-1669 .- 1520-510X. ; 63:11, s. 5040-5051
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Tidskriftsartikel (refereegranskat)abstract
- The effect of Eu doping in the Tsai quasicrystal (QC) GdCd7.88 and its periodic 1/1 approximant crystal (AC) GdCd6 are investigated. This represents the first synthesis of Eu-containing stable QC samples, where three samples with the final composition Gd1-xEuxCd7.6±α at Eu doping concentrations x = 0.06, 0.13, and 0.19 are obtained (α ∼ 0.2). They are compared to two 1/1 ACs with compositions Gd1-xEuxCd6 (x = 0.12, 0.16). In addition, a new type of 1/1 AC, differing only by the inclusion of extra Cd sites unique to the Eu4Cd25 1/1 AC, has been discovered and synthesized for the concentrations Gd1-xEuxCd6+δ (x = 0.25, 0.33, 0.45, 0.69, 0.73, and 0 < δ ≤ 0.085). Due to the preferred cube morphology of its single grains, we refer to them as c-type 1/1 ACs and to the conventional standard ones as s-type. In both QCs and s-type ACs, the Eu content appears to saturate at a concentration of similar to 20%. On the other hand, any Gd| Eu ratio is allowed in the c-type ACs, varying continuously between GdCd6 and Eu4Cd25. We describe and contrast the changes in composition, atomic structure, specific heat, and magnetic properties induced by Eu doping in the quasicrystalline phase and the s-type and c-type 1/1 ACs. By comparing our results to the literature data, we propose that the occupancy of the extra Cd sites can be used to predict the stability of Tsai-type quasicrystalline phases.
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| 3. |
- Denoel, Fernand
(författare)
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Frustrated magnetism in icosahedral structures : The influence of order-disorder in quasicrystals and approximant crystals
- 2024
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- This work will begin with an introduction to quasicrystals (QCs) and their structure, defining the unit cell-equivalent for icosahedral quasiperiodicity: a 3D tiling based on the golden ratio and aperiodic in all three dimensions. We briefly present the cut-and-project method used to generate QCs from a higher dimension hypercrystal, and how to build the 3D Penrose tilings, composed of the two golden rhombohedra. We introduce the atomic elementary units used to understand Tsai-type icosahedral QCs and their related approximant crystals (ACs). Approximants are conventional periodic crystals with local atomic environments very similar to their QC counterparts. Two methods for synthesis of Tsai-type QCs and approximants are introduced, the self-flux method as well as a rapid quench method. We describe briefly the differences between the two methods and aspect about phase stability for QCs and ACs obtained in binary and ternary systems. Various types of structural modulations can be induced in ACs which are absent from QCs. We present a new criterion discovered during the doctoral studies, which links the structure of existing ACs to the existence of stable QC counterparts. Basic concepts of magnetism relevant to Tsai systems are then introduced, with a description of the 4f shell magnetism in lanthanide elements, how it differs from transition metal magnetism, with localized (and relatively large) magnetic moments. In intermetallic systems such as Tsai-type QCs and ACs, the main type of magnetic interaction is of RKKY type. We link their structure to the magnetic behavior and phase transition that can occur in frustrated systems: spin glass, reentrant spin glass, spin ice, etc. and how they can be related to various Tsai systems.
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| 4. |
- Dufresnes, Christophe, et al.
(författare)
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Fifteen shades of green : The evolution of Bufotes toads revisited
- 2019
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Ingår i: Molecular Phylogenetics and Evolution. - : Elsevier BV. - 1055-7903 .- 1095-9513. ; 141
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Tidskriftsartikel (refereegranskat)abstract
- The radiation of Palearctic green toads (Bufotes) holds great potential to evaluate the role of hybridization in phylogeography at multiple stages along the speciation continuum. With fifteen species representing three ploidy levels, this model system is particularly attractive to examine the causes and consequences of allopoly-ploidization, a prevalent yet enigmatic pathway towards hybrid speciation. Despite substantial efforts, the evolutionary history of this species complex remains largely blurred by the lack of consistency among the corresponding literature. To get a fresh, comprehensive view on Bufotes phylogeography, here we combined genome-wide multilocus analyses (RAD-seq) with an extensive compilation of mitochondrial, genome size, niche modelling, distribution and phenotypic (bioacoustics, morphometrics, toxin composition) datasets, representing hundreds of populations throughout Eurasia. We provide a fully resolved nuclear phylogeny for Bufotes and highlight exceptional cyto-nuclear discordances characteristic of complete mtDNA replacement (in 20% of species), mitochondrial surfing during post-glacial expansions, and the formation of homoploid hybrid populations. Moreover, we traced the origin of several allopolyploids down to species level, showing that all were exclusively fathered by the West Himalayan B. latastii but mothered by several diploid forms inhabiting Central Asian lowlands, an asymmetry consistent with hypotheses on mate choice and Dobzhansky-Muller incompatibilities. Their intermediate call phenotypes potentially allowed for rapid reproductive isolation, while toxin compositions converged towards the ecologically-closest parent. Across the radiation, we pinpoint a stepwise progression of reproductive isolation through time, with a threshold below which hybridizability is irrespective of divergence (< 6My), above which species barely admix and eventually evolve different mating calls (6-10My), or can successfully cross-breed through allopolyploidization (> 15My). Finally, we clarified the taxonomy of Bufotes (including genetic analyses of type series) and formally described two new species, B. cypriensis sp. nov. (endemic to Cyprus) and B. perrini sp. nov. (endemic to Central Asia). Embracing the genomic age, our framework marks the advent of a new exciting era for evolutionary research in these iconic amphibians.
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| 5. |
- Gebresenbut, Girma Hailu, 1982-, et al.
(författare)
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Atomic-Scale Tuning of Tsai-Type Clusters in RE-Au-Si Systems (RE = Gd, Tb, Ho)
- 2020
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Ingår i: Inorganic Chemistry. - : American Chemical Society (ACS). - 0020-1669 .- 1520-510X. ; 59:13, s. 9152-9162
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Tidskriftsartikel (refereegranskat)abstract
- Tsai-type quasicrystals and approximants are distinguished by a cluster unit made up of four concentric polyhedral shells that surround a tetrahedron at the center. Here we show that for Tsai-type 1/1 approximants in the RE-Au-Si systems (RE = Gd, Tb, Ho) the central tetrahedron of the Tsai clusters can be systematically replaced by a single RE atom. The modified cluster is herein termed a pseudo-Tsai cluster and represents, in contrast to the conventional Tsai cluster, a structural motif without internal symmetry breaking. For each system, single-phase samples of both pseudo-Tsai and Tsai-type 1/1 approximants were independently prepared as millimeter-sized, faceted, single crystals using the self-flux synthesis method. The full replacement of tetrahedral moieties by RE atoms in the pseudo-Tsai 1/1 approximants was ascertained by a combination of single-crystal and powder diffraction studies, as well as energy dispersive X-ray spectroscopy (EDX) analyses with a scanning electron microscope (SEM). Differential scanning calorimetry (DSC) studies revealed distinctly higher decomposition temperatures, by 5-35 K, for the pseudo-Tsai phases. Furthermore, the magnetic properties of pseudo-Tsai phases are profoundly and consistently different from the Tsai counterparts. The onset temperatures of magnetic ordering (T-mag) are lowered in the pseudo-Tsai phases by similar to 30% from 24 to 17 K, 11.5 to 8 K, and 5 to 3.5 K in the Gd-Au-Si, Tb-Au-Si, and Ho-Au-Si systems, respectively. In addition, the Tb-Au-Si and Ho-Au-Si systems exhibit some qualitative changes in their magnetic ordering, indicating decisive changes in the magnetic state/structure by a moment-bearing atom at the cluster center.
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| 6. |
- Shiino, Takayuki, et al.
(författare)
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Nonequilibrium dynamical behavior in noncoplanar magnets with chiral spin texture
- 2022
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Ingår i: Physical Review B. - : American Physical Society. - 2469-9950 .- 2469-9969. ; 105:18
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Tidskriftsartikel (refereegranskat)abstract
- We observe nonequilibrium dynamical magnetic behavior in the magnetically ordered phase of a Tsai-type Tb-Au-Si quasicrystal approximant system. The magnetic texture in the ordered phase is found to exhibit scalar spin chirality (SSC) order, inferring that SSC is the order parameter of the present magnetic system. We further find that the introduction of “pseudo-Tsai” clusters, associated with additional Tb atoms in the structure, induces spin-glass dynamics. We discuss the observed dynamical magnetic behavior in the Tb-Au-Si systems, considering the effect of the pseudo-Tsai clusters on the magnetic configuration and local spin chirality.
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| 7. |
- Shiino, Takayuki, et al.
(författare)
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Singular magnetic dilution behavior in a quasicrystal approximant
- 2021
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Ingår i: Physical Review B. - : American Physical Society. - 2469-9950 .- 2469-9969. ; 104:22
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Tidskriftsartikel (refereegranskat)abstract
- We report the effect of magnetic dilution on the physical properties of (Gd1−xYx)Cd6 approximant crystals (ACs), close siblings of their corresponding quasicrystal (QC). Compared to the pure system GdCd6, we observe remarkable changes in the thermodynamic and magnetic bulk properties near and below the static-ordering temperatures from diluting the magnetic Gd atoms with nonmagnetic Y atoms by only 1–3% (x=0.01–0.03). On the other hand, the corresponding QC system exhibits a monotonic change in its spin-glass behavior upon the magnetic dilution. We discuss the origin of the magnetic-dilution behavior in the present AC system in terms of possible magnetic frustration and short-range magnetic correlation that can be linked to its peculiar structure.
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| 8. |
- Shiino, Takayuki, et al.
(författare)
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Singular magnetic dilution behavior in a quasicrystal approximant
- 2021
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Ingår i: Physical Review B. - 2469-9950 .- 2469-9969. ; 104:22
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Tidskriftsartikel (refereegranskat)abstract
- We report the effect of magnetic dilution on the physical properties of (Gd1−xYx)Cd6 approximant crystals (ACs), close siblings of their corresponding quasicrystal (QC). Compared to the pure system GdCd6, we observe remarkable changes in the thermodynamic and magnetic bulk properties near and below the static-ordering temperatures from diluting the magnetic Gd atoms with nonmagnetic Y atoms by only 1–3% (x=0.01–0.03). On the other hand, the corresponding QC system exhibits a monotonic change in its spin-glass behavior upon the magnetic dilution. We discuss the origin of the magnetic-dilution behavior in the present AC system in terms of possible magnetic frustration and short-range magnetic correlation that can be linked to its peculiar structure.
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| 9. |
- Shiino, Takayuki, et al.
(författare)
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Superconductivity at 1 K in Y-Au-Si quasicrystal approximants
- 2021
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Ingår i: Physical Review B. - : American Physical Society. - 2469-9950 .- 2469-9969. ; 103:5
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Tidskriftsartikel (refereegranskat)abstract
- We report the structural and physical properties of two Y-Au-Si (YAS) compounds, Y(14.1)AU(69.2)Si(16.7) and Y15.4Au68.6Si16.1, which are 1/1 approximant crystals of a Tsai-type quasicrystal without intrinsic magnetic moments. The compounds differ by the presence of either a tetrahedron (Au,Si)(4) or a single Y atom at the center of their characteristic structural building unit consisting of concentric polyhedral shells. Both compounds exhibit bulk superconductivity, which seems to be of a conventional type-II BCS type. The compound with Y atoms at the cluster center has a slightly higher transition temperature with a sharper step in the specific heat than the compound with tetrahedral units. We discuss the occurrence of this superconducting state in the light of the specific structural and physical properties of these quasicrystal approximants.
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