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result(s) for
"Puphal, Pascal"
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Magnetism and anomalous transport in the Weyl semimetal PrAlGe: possible route to axial gauge fields
2020
In magnetic Weyl semimetals, where magnetism breaks time-reversal symmetry, large magnetically sensitive anomalous transport responses are anticipated that could be useful for topological spintronics. The identification of new magnetic Weyl semimetals is therefore in high demand, particularly since in these systems Weyl node configurations may be easily modified using magnetic fields. Here we explore experimentally the magnetic semimetal PrAlGe, and unveil a direct correspondence between easy-axis Pr ferromagnetism and anomalous Hall and Nernst effects. With sizes of both the anomalous Hall conductivity and Nernst effect in good quantitative agreement with first principles calculations, we identify PrAlGe as a system where magnetic fields can connect directly to Weyl nodes via the Pr magnetisation. Furthermore, we find the predominantly easy-axis ferromagnetic ground state co-exists with a low density of nanoscale textured magnetic domain walls. We describe how such nanoscale magnetic textures could serve as a local platform for tunable axial gauge fields of Weyl fermions.
Journal Article
Synthesis and Optical Properties of Single‐Crystalline Phosphors Gd3In2Ga3O12:RE3+ (RE = Nd3+ and Ho3+) Grown via the Optical Float Zone Method
2025
The continuous development of innovative optical materials with lanthanoid ions as activators has emerged as a modern sector of materials chemistry. The experience with the fabrication of single crystals with the optical float zone has motivated one to investigate the luminescence of Nd3+ and Ho3+ ions in the garnets (Gd3−xREx)In2Ga3O12 (RE = Nd and Ho, x = 0; 0.15–0.30). Upon usage of an Ar/O2 (80:20 ratio) atmosphere and application of an auxiliary pressure (6 bar) to suppress In2O3 evaporation, single‐crystalline domain sizes in the order of ≈6 × 6 × 1 mm3 are obtained. Structural analysis confirms the formation of a cubic garnet phase with space group Ia3¯d $I a \\bar{3} d$ , with the substituents incorporated in accordance with Vegard's law. Backscattered electron imaging and energy‐dispersive X‐ray spectroscopy are conducted, demonstrating a homogeneous elemental distribution within the crystals. Photoluminescence studies are carried out, revealing the characteristic narrow‐line 4f n → 4f n transitions of Nd3+ and Ho3+, with decay times in the submillisecond range, suggesting non‐negligible cross‐relaxation effects are present. Despite this, the large nearest‐neighbor Gd–Gd distance (3.88 Å) in Gd3In2Ga3O12 and the low phonon cutoff energy (≈700 cm−1) are found to limit cross‐relaxation pathways, preserving significant photoluminescence brightness. These results highlight the potential of Gd3In2Ga3O12:RE3+ single crystals as promising candidates for advanced optical applications. Nd3+‐ and Ho3+‐doped Gd3In2Ga3O12 single crystals have been successfully synthesized via the optical float zone method. Their structure and optical characterization demonstrate efficient narrow‐line 4f–4f emission, low cross‐relaxation, and bright photoluminescence, indicating their potential as advanced optical materials for photonic applications.
Journal Article
Floating Zone Growth of Sr Substituted Han Purple: Ba0.9Sr0.1CuSi2O6
by
Puphal, Pascal
,
Allenspach, Stephan
,
Pomjakushina, Ekaterina
in
copper silicate
,
Crystal growth
,
Crystal structure
2019
We present a route to grow single crystals of Ba 0.9 Sr 0.1 CuSi 2 O 6 suitable for inelastic neutron studies via the floating zone technique. Neutron single crystal diffraction was utilized to check their bulk quality and orientation. Finally, the high quality of the grown crystals was proven by X-ray diffraction and magnetic susceptibility.
Journal Article
Absence of Spin Frustration in the Kagomé Layers of Cu2+ Ions in Volborthite Cu3V2O7(OH)2·2H2O and Observation of the Suppression and Re-Entrance of Specific Heat Anomalies in Volborthite under an External Magnetic Field
by
Kremer, Reinhard K.
,
Whangbo, Myung-Hwan
,
Puphal, Pascal
in
Anomalies
,
Antiferromagnetism
,
Chains
2022
We determined the spin exchanges between the Cu2+ ions in the kagomé layers of volborthite, Cu3V2O7(OH)2·2H2O, by performing the energy-mapping analysis based on DFT+U calculations, to find that the kagomé layers of Cu2+ ions are hardly spin-frustrated, and the magnetic properties of volborthite below ~75 K should be described by very weakly interacting antiferromagnetic uniform chains made up of effective S = 1/2 pseudospin units. This conclusion was verified by synthesizing single crystals of not only Cu3V2O7(OH)2·2H2O but also its deuterated analogue Cu3V2O7(OD)2·2D2O and then by investigating their magnetic susceptibilities and specific heats. Each kagomé layer consists of intertwined two-leg spin ladders with rungs of linear spin trimers. With the latter acting as S = 1/2 pseudospin units, each two-leg spin ladder behaves as a chain of S = 1/2 pseudospins. Adjacent two-leg spin ladders in each kagomé layer interact very weakly, so it is required that all nearest-neighbor spin exchange paths of every two-leg spin ladder remain antiferromagnetically coupled in all spin ladder arrangements of a kagomé layer. This constraint imposes three sets of entropy spectra with which each kagomé layer can exchange energy with the surrounding on lowering the temperature below ~1.5 K and on raising the external magnetic field B. We discovered that the specific heat anomalies of volborthite observed below ~1.5 K at B = 0 are suppressed by raising the magnetic field B to ~4.2 T, that a new specific heat anomaly occurs when B is increased above ~5.5 T, and that the imposed three sets of entropy spectra are responsible for the field-dependence of the specific heat anomalies.
Journal Article
Realization of a classical Ruddlesden Popper type bilayer nickelate in Sr3Ni2−xAlxO7−δ with unusual Ni4
by
Yilmaz, Hasan
,
Küster, Kathrin
,
Puphal, Pascal
in
Crystal growth
,
High temperature superconductors
,
Magnetic transitions
2024
The discovery of 80 K superconductivity in bilayer La3Ni2O7 at pressures greater than 14 GPa presents a unique opportunity to study a novel class of high-temperature superconductors. Therefore, other bilayer nickelates following the classical (T4+) Ruddlesden-Popper (RP) series of Sr3Ni2O7 would present an interesting new candidate. In this work, we study the stabilization of RP n = 2 phase in Sr3Ni2−xAlxO7−δ, via floating zone growth of crystals. With powder and single-crystal XRD, we study the stability range of the RP-type phase. Our Thermogravimetric Analysis (TGA), X-ray photoelectron spectroscopy (XPS) and gas extraction studies reveal a remarkably high oxidation state of Ni4+ stabilized by chemical strain from Al. The obtained black crystals are insulating in transport and show a magnetic transition around 12 K.
Journal Article
Synthesis and Optical Properties of Single‐Crystalline Phosphors Gd 3 In 2 Ga 3 O 12 :RE 3+ (RE = Nd 3+ and Ho 3+ ) Grown via the Optical Float Zone Method
2025
The continuous development of innovative optical materials with lanthanoid ions as activators has emerged as a modern sector of materials chemistry. The experience with the fabrication of single crystals with the optical float zone has motivated one to investigate the luminescence of Nd 3+ and Ho 3+ ions in the garnets (Gd 3− x RE x )In 2 Ga 3 O 12 (RE = Nd and Ho, x = 0; 0.15–0.30). Upon usage of an Ar/O 2 (80:20 ratio) atmosphere and application of an auxiliary pressure (6 bar) to suppress In 2 O 3 evaporation, single‐crystalline domain sizes in the order of ≈6 × 6 × 1 mm 3 are obtained. Structural analysis confirms the formation of a cubic garnet phase with space group , with the substituents incorporated in accordance with Vegard's law. Backscattered electron imaging and energy‐dispersive X‐ray spectroscopy are conducted, demonstrating a homogeneous elemental distribution within the crystals. Photoluminescence studies are carried out, revealing the characteristic narrow‐line 4 f n → 4 f n transitions of Nd 3+ and Ho 3+ , with decay times in the submillisecond range, suggesting non‐negligible cross‐relaxation effects are present. Despite this, the large nearest‐neighbor Gd–Gd distance (3.88 Å) in Gd 3 In 2 Ga 3 O 12 and the low phonon cutoff energy (≈700 cm −1 ) are found to limit cross‐relaxation pathways, preserving significant photoluminescence brightness. These results highlight the potential of Gd 3 In 2 Ga 3 O 12 :RE 3+ single crystals as promising candidates for advanced optical applications.
Journal Article
Tuning Two Dimensional Cu-Based Quantum Spin Systems
2017
Die Arbeit beschäftigt sich mit der Herstellung sowie der strukturellen und magnetischen Charakterisierung von zwei Materialklassen von kupferbasierten zweidimensionalen Quanten-Spin-Systemen: Quadratische Gitter von Dimeren sowie geometrisch frustrierte Kagomé Gitter. In beiden Systemen werden Substitutionen vorgestellt die zu verbesserten Eigenschaften führen.
Dissertation
Lattice dynamics of the infinite-layer nickelate LaNiO\\(_2\\)
by
Hayashida, Shohei
,
Wu, Wenfeng
,
Keller, Thomas
in
Inelastic scattering
,
Lattice vibration
,
Neutron scattering
2025
Infinite-layer (IL) nickelates have rapidly emerged as a new class of superconductors. However, due to the technical challenges of their topotactic synthesis, they have so far been realized primarily as thin films or polycrystalline powder samples, limiting comprehensive investigations of fundamental physical properties such as the lattice dynamics. Here, we present a time-of-flight inelastic neutron scattering study on a sample composed of a large number of co-aligned bulk crystals of the IL nickelate LaNiO\\(_2\\). We observe several dispersive phonon branches, which are in good agreement with lattice dynamical calculations based on density-functional perturbation theory. In addition, we compare the characteristics of selected LaNiO\\(_2\\) phonon modes to those of isostructural cuprate superconductors. Our findings provide a reference point for future experimental and theoretical efforts aimed at understanding the interplay between lattice dynamics and electronic properties in IL nickelates.
Topochemical Fluorination of La\\(_2\\)NiO\\(_4+\\) Single Crystals
by
Yilmaz, Hasan
,
Clemens, Oliver
,
Isobe, Masahiko
in
Anion exchanging
,
Antiferromagnetism
,
Float zones
2026
Topochemical fluorination offers a low--temperature route for modifying the anion chemistry and electronic ground states of layered transition-metal oxides, providing access to metastable phases and functionalities that are not able to be achieved through conventional solid--state synthesis. Despite extensive work on polycrystalline samples and thin films, topochemical fluorination of bulk single crystals has not been studied, limiting insights into intrinsic structure property relationships. Here, we investigate the topochemical fluorination of optical float zone grown (OFZ) La\\(_2\\)NiO\\(_4+\\) single crystals using polymer-based PTFE, PVDF and inorganic CuF\\(_2\\) fluorination agents and compare it to our topochemical pathways of reduction of LaNiO\\(_3-x\\). By systematically investigating direct and indirect contact reaction pathways, we can understand fluorination mechanisms, quantify the degree of fluorine incorporation, and evaluate the resulting structural and magnetic modifications in a detail that was not possible in powder and thin films. Powder and single--crystal X-ray diffraction reveal that fluorination proceeds without destroying the Ruddlesden--Popper framework, while inducing lattice parameter changes consistent with anion intercalation in the bulk and ion exchange on the surface. This even induces a clear superstructure, which was not reported before and extends the understanding of anion insertion reactions beyond what is known on stage ordering in nickelates. Energy-dispersive X--ray spectroscopy confirms strong fluorine incorporation on the surface and reduced homogeneity in the bulk. Magnetic susceptibility measurements demonstrate a change in antiferromagnetic ordering upon fluorination.
Emergence of a Fluctuating Ground State in Y-kapellasite under Pressure
by
Joao Elias F S Rodrigues
,
Capitani, Francesco
,
Dressel, Martin
in
Anisotropy
,
Frustrated magnetism
,
Ground state
2026
Y-kapellasite (Y\\(_3\\)Cu\\(_9\\)(OH)\\(_19\\)Cl\\(_8\\)), which hosts an original anisotropic kagome sublattice, is a promising candidate for studying elusive and complex correlated physics. It exhibits a theoretically predicted in-plane \\((1/3, 1/3)\\) magnetic order [1] but its magnetic interaction values place it close to a phase boundary to a spin liquid state [2]. Our \\(\\)SR measurements under hydrostatic pressure demonstrate the complete suppression of static magnetism in favor of a fully dynamical ground state at \\(2.3\\)~GPa. Complementary high-pressure x-ray and optical phonon measurements reveal a gradual reduction of the kagome anisotropy, enhancing magnetic frustration without structural transitions. Our results establish Y-kapellasite as a rare clean kagome model in which long-range order is suppressed by pressure-tuned frustration, the first fingerprint for the realization of a quantum spin liquid without strong disorder.