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108 records · Page 6

Strain-tunable metamagnetic critical endpoint in Mott insulating rare-earth titanates

Rare-earth titanates are Mott insulators whose magnetic ground state—antiferromagnetic (AFM) or ferromagnetic (FM)—can be tuned by the radius of the rare-earth element. We combine phenomenology and first-principles calculations to shed light on the generic magnetic phase diagram of a chemically substituted titanate on the rare-earth site that interpolates between an AFM and a FM state. Octahedral rotations present in these perovskites cause the AFM order to acquire a small FM component—and vice-versa—removing any multicritical point from the phase diagram. However, for a wide parameter range, a first-order metamagnetic transition line terminating at a critical endpoint survives inside the magnetically ordered phase. Like the liquid-gas transition, a Widom line emerges from the endpoint, characterized by enhanced fluctuations. In contrast to metallic FMs, this metamagnetic transition involves two symmetry-equivalent and insulating canted spin states. Moreover, instead of a magnetic field, we show that uniaxial strain can be used to tune this transition to zero temperature, inducing a quantum critical endpoint.

36 MATERIALS SCIENCE↗

Pressure tuning of Kitaev spin liquid candidate Na 3 Co 2 SbO 6

The search for Kitaev’s quantum spin liquid in real materials has recently expanded with the prediction that honeycomb lattices of divalent, high-spin cobalt ions could host the dominant bond-dependent exchange interactions required to stabilize the elusive entangled quantum state. The layered honeycomb Na 3 Co 2 SbO 6 has been singled out as a leading candidate provided that the trigonal crystal field acting on Co 3d orbitals, which enhances non-Kitaev exchange interactions between $J$ eff = $\frac{1}{2}$ spin-orbital pseudospins, is reduced. Here we show that applied pressure leads to anisotropic compression of the layered structure, significantly reducing the trigonal distortion of CoO 6 octahedra. Ferromagnetic correlations between pseudospins are enhanced in the spin-polarized (3 Tesla) phase up to about 60 GPa. Higher pressures drive a high-spin to low-spin transition destroying the $J$ eff = $\frac{1}{2}$ moments required to map the spin Hamiltonian into Kitaev’s model. The spin transition strongly suppresses the low-temperature magnetic susceptibility and appears to stabilize a paramagnetic phase driven by frustration. The possible emergence of frustrated magnetism of localized $S$ = $\frac{1}{2}$ moments opens the door for exploration of novel magnetic quantum states in compressed honeycomb lattices of divalent cobaltates.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

From hard spheres to hard-core spins

A system of hard spheres exhibits physics that is controlled only by their density. This comes about because the interaction energy is either infinite or zero, so all allowed configurations have exactly the same energy. The low-density phase is liquid, while the high-density phase is crystalline, an example of “order by disorder” as it is driven purely by entropic considerations. Here we study a family of hard spin models, which we call hard-core spin models, where we replace the translational degrees of freedom of hard spheres with the orientational degrees of freedom of lattice spins. Their hard-core interaction serves analogously to divide configurations of the many spin system into allowed and disallowed sectors. We present detailed results on the square lattice in d = 2 for a set of models with $\mathbb{Z}_n$ symmetry, which generalize Potts models, and their U(1) limits, for ferromagnetic and antiferromagnetic senses of the interaction, which we refer to as exclusion and inclusion models. As the exclusion and inclusion angles are varied, we find a Kosterlitz-Thouless phase transition between a disordered phase and an ordered phase with quasi-long-ranged order, which is the form order by disorder takes in these systems. These results follow from a set of height representations, an ergodic cluster algorithm, and transfer matrix calculations.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Pressure tuning of Kitaev spin liquid candidate Na$_3$Co$_2$SbO$_6$goo

The search for Kitaev's quantum spin liquid (KQSL) state in real materials has recently expanded with the prediction that honeycomb lattices of divalent, high-spin cobalt ions could host the dominant bond-dependent exchange interactions required to stabilize the elusive entangled quantum state. The layered honeycomb Na$_3$Co$_2$SbO$_6$ has been singled out as a leading candidate provided that the trigonal crystal field acting on Co $3d$ orbitals, which enhances non-Kitaev exchange interactions between $J_{\rm eff}=\frac{1}{2}$ spin-orbital pseudospins, is reduced. We find that applied pressure leads to anisotropic compression of the layered structure, significantly reducing the trigonal distortion of CoO$_6$ octahedra. A strong enhancement of ferromagnetic correlations between pseudospins is observed in the spin-polarized (3 Tesla) phase up to about 60 GPa. Higher pressures drive a spin transition into a low-spin state destroying the $J_{\rm eff}=\frac{1}{2}$ local moments required to map the spin Hamiltonian into Kitaev's model. The spin transition strongly suppresses the low-temperature magnetic susceptibility and appears to stabilize a paramagnetic phase driven by frustration. Although applied pressure fails to realize a KQSL state, the possible emergence of frustrated magnetism of localized, low-spin $S=\frac{1}{2}$ moments opens the door for exploration of novel magnetic quantum states in compressed honeycomb lattices of divalent cobaltates.

FOS: Physical sciences↗

Tablelike magnetocaloric effect and enhanced refrigerant capacity in EuO 1- δ thin films

The effect of electron doping of EuO 1- δ thin films through oxygen vacancies ( δ = 0, 0.025, and 0.09) upon the magnetocaloric response is presented here. The films each showed a paramagnetic to ferromagnetic transition around 65 K, with an additional magnetic ordering transition at higher temperatures in the oxygen deficient samples. All transitions are observed to be of second order. A maximum magnetic entropy change of 6.4 J/kg K over a field change of 2 T with a refrigerant capacity of 223 J/kg was found in the sample with δ = 0, and in all cases the refrigerant capacities of the thin films under study were found to exceed that reported for bulk EuO. Adjusting the oxygen content was shown to produce tablelike magnetocaloric effects, desirable for ideal Ericsson-cycle magnetic refrigeration. These films are thus excellent candidates for small-scale magnetic cooling technology in the liquid nitrogen temperature range.

36 MATERIALS SCIENCE↗

Observation of Topological Chirality Switching Induced Freezing of a Skyrmion Crystal

Magnetic skyrmions are topologically protected quasi-particles with a well-defined chirality. Control over their chirality is proposed as an additional feature for encoding data bits or as qubits in quantum computing due to their high efficiency and stability against achiral magnetic textures. Here it is shown that an in-plane magnetic field can be utilized to reshape the energy barriers between different skyrmionic bubbles (e.g., Bloch type, type-II) enabling spontaneous chirality fluctuations with a frequency that increases with the strength of the in-plane field. The insulating van der Waals ferromagnet CrBr3 is used as an archetypal system for low damping, reduced energy dissipation and a high number of magnetic phases to capture the chirality dynamics in real time through cryo-Lorentz transmission electron microscopy. It is observed that the interplay between the intrinsic Dzyaloshinskii–Moriya interaction and out-of-plane field biased the chirality dynamics, favoring one handedness over the other. A remarkable consequence of the spontaneous chirality switching mechanism is that it induces a freezing (or crystallization) process in the skyrmion lattice. As the bubbles fluctuate between Bloch and type-II they elongate and shrink parallel to the in-plane field. Subsequently, the overall lattice crystallizes along the in-plane field direction, inducing a phase transition from a disordered liquid state to a hexatic phase where skyrmions are highly ordered resembling that of a solid. The results indicate chirality as an active element in the creation of topologically protected skyrmion crystals unveiling pathways toward chiral spintronic device platforms with tunable embedded configuration.

2D Phase Transition↗

Quantum phases in the honeycomb-lattice J 1 – J 3 ferro-antiferromagnetic model

The significant role of quantum effects in magnets with competing interactions remains at the forefront of condensed matter physics for over 50 years, inspiring a multitude of quests for exotic states, models that can realize them, and real materials that can host them. The elusive spin-liquid states with strong entanglement are but one example; others include valence-bond phases with spatial symmetry breaking, quantum spin nematics that are quantum analogues of liquid crystals, and an especially extensive class of unconventional magnetically ordered phases that do not appear in the classical solutions of the underlying spin models. It is the latter group of phenomena that creates a broader context for the research effort in the present work concerning the search for and an identification of the novel ground states of quantum magnets. In this work, we have studied one of the paradigmatic models in quantum magnetism that is also attracting a significant recent interest because it appears to be providing a tantalizingly close description for many of the newly synthesized materials. We demonstrated that the phase diagram of the quantum ferro-antiferromagnetic model on the honeycomb lattice differs dramatically from the classical one. It hosts the double-zigzag and Ising-z phases as unexpected intermediaries between ferromagnetic and zigzag states that are also extended beyond their classical regions of stability. In broad agreement with quantum order-by-disorder arguments, these collinear phases completely supersede the classical spiral state.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Directional solidification and characterization of near eutectic Sm2CO17/Co alloys

The effects of directional solidification processing on the microstructural, compositional, and magnetic properties of near eutectic Co-Sm alloys (about 9 at. pct Sm) have been studied. Initial investigations have been performed at modest thermal gradients in the liquid, G(L) less than 60 C/cm and over a range of furnace (solidification) velocities, V = 0.8 45.4 cm/h. The primary dendrite spacing for near eutectic Sm2Co17/Co scaled with 1/sq rt V and varied from about 50 microns for V greater than or equal to 20 cm/h to hundreds of microns for V less than 10 cm/h, while the rod eutectic diameter and interrod spacing were an order of magnitude smaller. For both dendritic and cooperative growth, the associated permanent magnet properties were rather poor, e.g., remanence less than 4 kG and coercive force less than 1 kOe for the smallest dendrite and rod diameter dimensions encountered, although the magnetic hardness for the rod eutetic was larger than for the dendritic microstructure. Magnetization as a function of sample orientation indicated that the easy axis of magnetization was primarily along the direction of solidification for both ferromagnetic phases.

Pirich, Ronald G.↗

Ballistic Ejection of Microdroplets from Overpacked Interfacial Assemblies

Spontaneous emulsification, resulting from the assembly and accumulation of surfactants at liquid–liquid interfaces, is an interfacial instability where microdroplets are generated and diffusively spread from the interface until complete emulsification. Here, it is shown that an external magnetic field can modulate the assembly of paramagnetic nanoparticle surfactants (NPSs) at liquid–liquid interfaces to trigger an oversaturation in the areal density of the NPSs at the interface, as evidenced by a marked reduction in the interfacial tension, γ, and corroborated with a magnetostatic continuum theory. Despite the significant reduction in γ, the presence of the magnetic field does not cause stable interfaces to become unstable. Upon rapid removal of the field, however, an explosive ejection of a plume of microdroplets from the surface occurs, a dynamical interfacial instability which is termed explosive emulsification. Further, this explosive event rapidly reduces the areal density of the NPSs to its pre-field level, stabilizing the interface. The ability to externally suppress or trigger the explosive emulsification and controlled generation of tens of thousands of microdroplets, uncovers an efficient energy storage and release process, that has potential applications for controlled and directed delivery of chemicals and remotely controlled soft microrobots, taking advantage of the ferromagnetic nature of the microdroplets.

36 MATERIALS SCIENCE↗

Frustration- and doping-induced magnetism in a Fermi–Hubbard simulator

Geometrical frustration in strongly correlated systems can give rise to a plethora of novel ordered states and intriguing magnetic phases, such as quantum spin liquids. Promising candidate materials for such phases can be described by the Hubbard model on an anisotropic triangular lattice, a paradigmatic model capturing the interplay between strong correlations and magnetic frustration. However, the fate of frustrated magnetism in the presence of itinerant dopants remains unclear, as well as its connection to the doped phases of the square Hubbard model. Here we investigate the local spin order of a Hubbard model with controllable frustration and doping, using ultracold fermions in anisotropic optical lattices continuously tunable from a square to a triangular geometry. At half-filling and strong interactions U/t ≈ 9, we observe at the single-site level how frustration reduces the range of magnetic correlations and drives a transition from a collinear Néel antiferromagnet to a short-range correlated 120° spiral phase. Away from half-filling, the triangular limit shows enhanced antiferromagnetic correlations on the hole-doped side and a reversal to ferromagnetic correlations at particle dopings above 20%, hinting at the role of kinetic magnetism in frustrated systems. Furthermore, this work paves the way towards exploring possible chiral ordered or superconducting phases in triangular lattices and realizing t–t' square lattice Hubbard models that may be essential to describe superconductivity in cuprate materials.

74 ATOMIC AND MOLECULAR PHYSICS↗

Local distortion driven magnetic phase switching in pyrochlore Yb 2 ( Ti 1 - x Sn x ) 2 O 7

While it is commonly accepted that the disorder induced by magnetic ion doping in quantum magnets usually generates a rugged free-energy landscape resulting in slow or glassy spin dynamics, the disorder/distortion effects associated with nonmagnetic ion sites doping are still illusive. Here, using AC susceptibility measurements, we show that the mixture of Sn/Ti on the nonmagnetic ion sites of pyrochlore Yb 2 ⁢(Ti 1-x⁢ Sn x ) 2⁢ O 7 induces an antiferromagnetic ground state despite both parent compounds, Yb 2 ⁢Ti 2 ⁢O 7 and Yb 2 ⁢Sn 2⁢ O 7 , order ferromagnetically. Local structure studies through neutron total scattering reveals the local distortion in the nonmagnetic ion sites and its strong correlation with the magnetic phase switching. Further, our study demonstrates the local distortion as induced by the nonmagnetic ion site mixture could be a new path to achieve magnetic phase switching, which has been traditionally obtained by external stimuli such as temperature, magnetic field, pressure, strain, light, etc.

74 ATOMIC AND MOLECULAR PHYSICS↗

Electronic Structure Correspondence of Singlet-Triplet Scale Separation in Strained Sr2RuO4

At a temperature of roughly 1 K, Sr 2 RuO 4 undergoes a transition from a normal Fermi liquid to a superconducting phase. Even while the former is relatively simple and well understood, the superconducting state has not even been understood after 25 years of study. More recently, it has been found that critical temperatures can be enhanced by the application of uniaxial strain, up to a critical strain, after which it falls off. In this work, we take an “instability” approach and seek divergences in susceptibilities. This provides an unbiased way to distinguish tendencies to competing ground states. We show that in the unstrained compound, the singlet and triplet instabilities of the normal Fermi liquid phase are closely spaced. Under uniaxial strain, electrons residing on all orbitals contributing to the Fermiology become more coherent, while the electrons of the Ru-dxy character become heavier, and the electrons of the Ru d x z , y z characters become lighter. In the process, Im χ(q,ω) increases rapidly around q = ( 0.3 , 0.3 , 0 ) 2 π / a and q = ( 0.5 , 0.25 , 0 ) 2 π / a , while it gets suppressed at all other commensurate vectors, in particular at q = 0, which is essential for spin-triplet superconductivity. We observe that the magnetic anisotropy under strain drops smoothly, which is concomitant with the increment in singlet instability. Thus, the triplet superconducting instability remains the lagging instability of the system, and the singlet instability enhances under strain, leading to a large energy-scale separation between these competing instabilities. However, since this happens even without spin-orbit coupling, we believe it is primarily the enhancement in the spin fluctuation glue around quasi-anti-ferromagnetic vectors that drives the Cooper pairing instead of the magnetic anisotropy. At large strain, an instability to a spin density wave overtakes the superconducting one. The analysis relies on a high-fidelity, ab initio description of the one-particle properties and two-particle susceptibilities, based on the quasiparticle self-consistent GW approximation augmented by dynamical mean field theory. This approach is described and its high fidelity confirmed by comparing to observed one- and two-particle properties.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Ubiquity of amplitude-modulated magnetic ordering in the H - T phase diagram of the frustrated non-Fermi-liquid YbAgGe

YbAgGe contains a magnetic geometrically frustrated kagome-like lattice that also features significant local single-ion anisotropy. The electronic state is established by hybridization of 4f and conduction electrons leading to heavy electronic masses. The competition between these various interactions leads to nontrivial behavior under external magnetic field, including a sequence of magnetic phase transitions, non-Fermi-liquid states, and possibly a quantum critical point. We present a series of neutron diffraction experiments performed in the mK temperature range and under magnetic fields up to 8 T in the hexagonal plane, revealing the microscopic nature of the first four subsequent magnetic states of this phase diagram. The magnetic phases are associated with the propagation vectors K 1 =($\frac{1}{3}$ 0 $\frac{1}{3}$) for H < 2 T, K 2 = (0 0 0.32) for 2 T < H < 3 T, K 1 = ($\frac{1}{3}$ 0 $\frac{1}{3}$) for 3 T < H < 4.5 T and k 3 = (0.195 0.195 0.38) for 4.5 T < H < 7 T. Our structural refinements reveal a strong modulation of the magnetic moment amplitude in all phases. We observe that the ordered moments of the three magnetically different Yb sites become increasingly different in field, which complies with the principle local anisotropy directions relative to the field direction. While the ordered moments are aligned predominantly in the hexagonal plane, we also find a significant out-of-plane component and a ferromagnetic contribution above 2 T. Here we discuss possible scenarios that may evolve around the phase boundary at 4.5 T, which is associated with putative quantum criticality as identified by various bulk probes. We propose further steps that are required to better understand the microscopic interactions in this material.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Enhancement of charge-neutral fermionic excitations near the spin-flop transition in the magnetic Kondo material YbIr 3 Si 7

The new Kondo material YbIr 3 Si 7 , similar to other Kondo insulators, has been reported to exhibit charge-neutral fermionic excitations through measurements of specific heat and thermal conductivity at low temperatures. We performed 29 Si-NMR on YbIr 3 Si 7 to investigate the magnetic response of charge-neutral fermions from a microscopic perspective. In low magnetic fields parallel to the c axis, a single NMR peak in the paramagnetic state splits into three peaks below TN. In contrast, only a slight shift of the single NMR peak was observed in high magnetic fields. This spectral change as a function of the c-axis magnetic field is interpreted as a spin-flop transition, at which the magnetic moments oriented along the c axis antiferromagnetic (AFM-I) phase are rotated to the ab plane with a ferromagnetic component along the c-axis (AFM-II phase). In the vicinity of the spin-flop magnetic field H M , the nuclear spin-lattice relaxation rate 1/T 1 was found to be proportional to temperature at low temperatures, indicating the existence of charge-neutral fermions. Furthermore, a peak of 1/T 1 versus the c-axis magnetic field suggests that the charge-neutral fermions in YbIr 3 Si 7 are closely related to its magnetic properties. Our findings shed light on the origin of charge-neutral fermions in insulators.

36 MATERIALS SCIENCE↗

Radiation-induced transients on solid and molten Li and K iodides

The study, quantification, and monitoring of iodine in nuclear power generation systems have been paramount due to its environmental and health implications. Thorough speciation and transport studies strengthened the development and deployment of water reactors, which are now required for the new generation of Molten Salt Reactors (MSR), where the fuel and coolant are a complex liquid system of suitable halides. The speciation, radiation-induced chemistry, and transport of iodine (I-127, I-129 and I-131) under extreme conditions of temperature and ionizing radiation are among the challenges for the future implementation of MSR’s. In aqueous systems, the triiodide-iodine-iodide (I3--I2-I-) equilibrium is strongly dependent on the conditions of the medium. In molten iodides and chlorides, the triiodide detection (and its disproportionation) poses challenges due to the extreme conditions of temperature and radiation, but studies have shown a dependence on temperature, absorbed dose and salt composition. Through absorption spectroscopy techniques (diffuse reflectance and high-temperature UV-Vis), as well as resonance (Electron Paramagnetic Resonance) it is possible to identify primary transients induced by ionizing radiation trapped in the solid phase (Solid-state radiolysis), and steady-state main absorption components with a fast-acquisition real-time spectroscopy. The presence of heterogeneous phase (colloids), viscosity changes, and gas evolution are among the observed processes. A specific case of study is speciation in the presence of Ni. A corrosion product with magnetic properties due to unpaired electrons in its electronic structure. Ferromagnetic materials are monitored in solidified salts to identify aggregation and phase separation. Comparative studies of eutectic mixtures of LiI-KI and LiCl-KCl with known addition of dopants will be presented, with a perspective of radiation chemistry and its possible implications in complex systems.

36 - MATERIALS SCIENCE↗

Molecular beam epitaxy of the magnetic Kagome metal FeSn on LaAlO 3 (111)

Materials with Kagome layers are expected to give rise to rich physics arising from band structures with topological properties, spin liquid behavior, and the formation of Skyrmions. Until now, most work on Kagome materials has been performed on bulk samples due to difficulties in thin film synthesis. Here, by using molecular beam epitaxy, layered Kagome-structured FeSn films are synthesized on the (111) oriented LaAlO3 substrate. Both in situ and ex situ characterizations indicate that these films are highly crystalline and c-axis oriented, with atomically smooth surfaces. The films grow as disconnected islands, with lateral dimensions on the micron meter scale. By patterning Pt electrodes using a focused electron beam, the longitudinal and transverse resistance of single islands have been measured in magnetic fields. Our work opens a pathway for exploring mesoscale transport properties in thin films of Kagome materials and related devices.

36 MATERIALS SCIENCE↗

Observation of novel charge ordering and spin reorientation in perovskite oxide PbFeO 3

Pb M O 3 ( M = 3 d transition metals) family shows systematic variations in charge distribution and intriguing physical properties due to its delicate energy balance between Pb 6 s and transition metal 3 d orbitals. However, the detailed structure and physical properties of PbFeO 3 remain unclear. Herein, we reveal that PbFeO 3 crystallizes into an unusual 2 a p × 6 a p × 2 a p orthorhombic perovskite super unit cell with space group Cmcm . The distinctive crystal construction and valence distribution of Pb 2+ 0.5 Pb 4+ 0.5 FeO 3 lead to a long range charge ordering of the -A-B-B- type of the layers with two different oxidation states of Pb (Pb 2+ and Pb 4+ ) in them. A weak ferromagnetic transition with canted antiferromagnetic spins along the a -axis is found to occur at 600 K. In addition, decreasing the temperature causes a spin reorientation transition towards a collinear antiferromagnetic structure with spin moments along the b -axis near 418 K. Our theoretical investigations reveal that the peculiar charge ordering of Pb generates two Fe 3+ magnetic sublattices with competing anisotropic energies, giving rise to the spin reorientation at such a high critical temperature.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Laplacian-level meta-generalized gradient approximation for solid and liquid metals

In this work, we derive and motivate a Laplacian-level, orbital-free meta-generalized-gradient approximation (LL-MGGA) for the exchange-correlation energy, targeting accurate ground-state properties of sp and sd metallic condensed matter, in which the density functional for the exchange-correlation energy is only weakly nonlocal due to perfect long-range screening. Our model for the orbital-free kinetic energy density restores the fourth-order gradient expansion for exchange to the r 2 SCAN meta-GGA [Furness et al., J. Phys. Chem. Lett. 11, 8208 (2020)], yielding a LL-MGGA we call OFR2. OFR2 matches the accuracy of SCAN for prediction of common lattice constants and improves the equilibrium properties of alkali metals, transition metals, and intermetallics that were degraded relative to the PBE GGA values by both SCAN and r 2 SCAN. We compare OFR2 to the r 2 SCAN -L LL-MGGA [Mejia-Rodriguez and Trickey, Phys. Rev. B 102, 121109(R) (2020)] and show that OFR2 tends to outperform r 2 SCAN -L for the equilibrium properties of solids, but r 2 SCAN -L much better describes the atomization energies of molecules than OFR2 does. For best accuracy in molecules and nonmetallic condensed matter, we continue to recommend SCAN and r 2 SCAN. Numerical performance is discussed in detail, and our paper provides an outlook to machine learning.

36 MATERIALS SCIENCE↗