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We report the magnetic and electronic transport properties of the inversion and time-reversal symmetry breaking Weyl semimetal NdAlGe. This material is analogous to NdAlSi, whose helical magnetism presents a rare example of a Weyl-mediated collective phenomenon, but with a larger spin-orbit coupling. Our neutron diffraction experiments revealed that NdAlGe, similar to NdAlSi, supports an incommensurate Ising spin density wave ($T_{\text{inc}}=6.8$ K) with a small helical spin canting of 3$^\circ$ and a long-wavelength of $\sim$ 35 nm, which transitions to a commensurate ferrimagnetic state below $T_{\text{com}}=5.1$ K. Using small-angle neutron scattering, we showed that the zero-field cooled ferrimagnetic domains form stripes in real space with characteristic length scales of 18 nm and 72 nm parallel and perpendicular to the [110] direction, respectively. Interestingly, for the transport properties, NdAlSi does not exhibit an anomalous Hall effect (AHE) that is commonly observed in magnetic Weyl semimetals. In contrast to NdAlSi, we identify two different AHE regimes in NdAlGe that are respectively governed by intrinsic Berry curvature and extrinsic disorders/spin fluctuations. Our study suggests that Weyl-mediated magnetism prevails in this group of noncentrosymmetric magnetic Weyl semimetals NdAl$X$, but transport properties including AHE are affected by material-specific extrinsic effects such as disorders, despite the presence of prominent Berry curvature., Preprint, 16 pages, 6 main figures, 6 supplementary figures

Emergent relativistic quasiparticles in Weyl semimetals are the source of exotic electronic properties such as surface Fermi arcs, the anomalous Hall effect and negative magnetoresistance, all observed in real materials. Whereas these phenomena highlight the effect of Weyl fermions on the electronic transport properties, less is known about what collective phenomena they may support. Here, we report a Weyl semimetal, NdAlSi, that offers an example. Using neutron diffraction, we found a long-wavelength helical magnetic order in NdAlSi, the periodicity of which is linked to the nesting vector between two topologically non-trivial Fermi pockets, which we characterize using density functional theory and quantum oscillation measurements. We further show the chiral transverse component of the spin structure is promoted by bond-oriented Dzyaloshinskii–Moriya interactions associated with Weyl exchange processes. Our work provides a rare example of Weyl fermions driving collective magnetism. The Weyl fermions in NdAlSi mediate a helical incommensurate spin density wave, providing a rare example of Weyl-mediated collective phenomena.

Phonons are known to generate a thermal Hall effect in certain insulators, including oxides with rare-earth impurities, quantum paraelectrics, multiferroic materials, and cuprate Mott insulators. In each case, a special feature of the material is presumed relevant for the underlying mechanism that confers chirality to phonons in a magnetic field. A fundamental question is whether a phonon Hall effect is an unusual occurrence-linked to special characteristics such as skew scattering off rare-earth impurities, structural domains, ferroelectricity, or ferromagnetism-or a much more common property of insulators than hitherto believed. To help answer this question, we have turned to a material with none of the previously encountered special features: the cubic antiferromagnet Cu

Phonons are known to generate a thermal Hall effect in certain insulators, including oxides with rare-earth impurities, quantum paraelectrics, multiferroic materials, and cuprate Mott insulators. In each case, a special feature of the material is presumed relevant for the underlying mechanism that confers chirality to phonons in a magnetic field. A fundamental question is whether a phonon Hall effect is an unusual occurrence—linked to special characteristics such as skew scattering off rare-earth impurities, structural domains, ferroelectricity, or ferromagnetism—or a much more common property of insulators than hitherto believed. To help answer this question, we have turned to a material with none of the previously encountered special features: the cubic antiferromagnet Cu3TeO6. We find that its thermal Hall conductivityκxyis among the largest of any insulator so far. We show that this record-highκxysignal is due to phonons, and it does not require the presence of magnetic order, as it persists above the ordering temperature. We conclude that the phonon Hall effect is likely to be a fairly common property of solids.

Recent observations of novel spin-orbit coupled states have generated tremendous interest in $4d/5d$ transition metal systems. A prime example is the $J_{\text{eff}}=\frac{1}{2}$ state in iridate materials and $\alpha$-RuCl$_{3}$ that drives Kitaev interactions. Here, by tuning the competition between spin-orbit interaction ($\lambda_{\text{SOC}}$) and trigonal crystal field splitting ($\Delta_\text{T}$), we restructure the spin-orbital wave functions into a novel $\mu=\frac{1}{2}$ state that drives Ising interactions. This is done via a topochemical reaction that converts Li$_{2}$RhO$_{3}$ to Ag$_{3}$LiRh$_{2}$O$_{6}$, leading to an enhanced trigonal distortion and a diminished spin-orbit coupling in the latter compound. Using perturbation theory, we present an explicit expression for the new $\mu=\frac{1}{2}$ state in the limit $\Delta_\text{T}\gg \lambda_{\text{SOC}}$ realized in Ag$_{3}$LiRh$_{2}$O$_{6}$, different from the conventional $J_\text{eff}=\frac{1}{2}$ state in the limit $\lambda_{\text{SOC}}\gg \Delta_\text{T}$ realized in Li$_{2}$RhO$_{3}$. The change of ground state is followed by a dramatic change of magnetism from a 6 K spin-glass in Li$_{2}$RhO$_{3}$ to a 94 K antiferromagnet in Ag$_{3}$LiRh$_{2}$O$_{6}$. These results open a pathway for tuning materials between the two limits and creating a rich magnetic phase diagram., Comment: 22 pages, 4 figures

Interplay of magnetism and electronic band topology in unconventional magnets enables the creation and fine control of novel electronic phenomena. In this work, we use scanning tunneling microscopy and spectroscopy to study thin films of a prototypical kagome magnet Fe3Sn2. Our experiments reveal an unusually large number of densely-spaced spectroscopic features straddling the Fermi level. These are consistent with signatures of low-energy Weyl fermions and associated topological Fermi arc surface states predicted by theory. By measuring their response as a function of magnetic field, we discover a pronounced evolution in energy tied to the magnetization direction. Electron scattering and interference imaging further demonstrates the tunable nature of a subset of related electronic states. Our experiments provide a direct visualization of how in-situ spin reorientation drives changes in the electronic density of states of the Weyl fermion band structure. Combined with previous reports of massive Dirac fermions, flat bands, and electronic nematicity, our work establishes Fe3Sn2 as an interesting platform that harbors an extraordinarily wide array of topological and correlated electron phenomena.

Weyl semimetal (WSM), a novel state of quantum matter, hosts Weyl fermions as emergent quasiparticles resulting from the breaking of either inversion or time-reversal symmetry. Magnetic WSMs that arise from broken time-reversal symmetry provide an exceptional platform to understand the interplay between magnetic order and Weyl physics, but few WSMs have been realized. Here, we identify CeAlSi as a new non-centrosymmetric magnetic WSM via angle-resolved photoemission spectroscopy (ARPES) and first-principles, density-functional theory based calculations. Our surface-sensitive vacuum ultraviolet ARPES data confirms the presence of surface Fermi arcs as, the smoking gun evidence for the existence of the Weyl semimetallic state in CeAlSi. We also observe bulk Weyl cones in CeAlSi using bulk-sensitive soft-X-ray ARPES measurements. In addition, Ce 4f at bands are found near the Fermi level, indicating that CeAlSi is a unique platform for investigating exotic quantum phenomena resulting from the interaction of topology, magnetism and electronic correlations., Comment: 12 pages, 4 figures; supplementary information included

Nearly two decades ago, Alexei Kitaev proposed a model for spin-$1/2$ particles with bond-directional interactions on a two-dimensional honeycomb lattice which had the potential to host a quantum spin-liquid ground state. This work initiated numerous investigations to design and synthesize materials that would physically realize the Kitaev Hamiltonian. The first-generation of such materials, such as Na$_{2}$IrO$_{3}$, $\alpha$-Li$_{2}$IrO$_{3}$, and $\alpha$-RuCl$_{3}$, revealed the presence of non-Kitaev interactions such as the Heisenberg and off-diagonal exchange. Both physical pressure and chemical doping were used to tune the relative strength of the Kitaev and competing interactions; however, little progress was made towards achieving a purely Kitaev system. Here, we review the recent breakthrough in modifying Kitaev magnets via topochemical methods that has led to the second-generation of Kitaev materials. We show how structural modifications due to the topotactic exchange reactions can alter the magnetic interactions in favor of a quantum spin-liquid phase., Comment: 18 pages, 7 figures

We report full vector mapping of local magnetization in CeAlSi, a Weyl semimetal in which both inversion and time-reversal symmetries are broken. The vector maps reveal unanticipated features both within domains and at their boundaries. Boundaries between domains form two kinds of walls with distinct topology and therefore different interactions with Weyl fermions. Domain walls aligned along the tetragonal axes, e.g. (100), exhibit emergent chirality forbidden by the bulk space group, while diagonal walls are non-chiral. Within the domains, we observe that the previously reported set of four easy axes aligned along the in-plane diagonals of the tetragonal structure actually split to form an octet with decreasing temperature below the magnetic transition. All the above phenomena are ultimately traced to the noncollinear magnetic structure of CeAlSi., 5+8 pages, 4+3 figures

The van der Waals class of materials offer an approach to two-dimensional magnetism as their spin fluctuations can be tuned upon exfoliation of layers. Moreover, it has recently been shown that spin-lattice coupling and long-range magnetic ordering can be modified with pressure in van der Waals materials. In this work, the magnetic properties of quasi two-dimensional CrBr3 are reported applying hydrostatic pressure. The application of pressure (0 - 0.8 GPa) shows a 72 % decrease in saturation magnetization with small decrease in the Curie temperature from 33 to 29 K. Density functional theory calculations with pressure up to 1 GPa show a reduction in volume and interplanar distance as pressure increases. To further understand magnetic properties with applied pressure, the magnetocrystalline anisotropy energy (MAE) and exchange coupling parameter (J) are calculated. There is minimal decrease in MAE and the first nearest neighbor interaction (J1) (U = 2.7 eV and J = 0.7 eV), shows an increase in J1 with respect to pressure. Overall, CrBr3 displays ferromagnetic interlayer coupling and the calculated exchange coupling and MAE parameters match well with the observations from the experimental work.

We use x-ray spectroscopy at the Ir ${L}_{3}/{L}_{2}$ absorption edge to study powder samples of the intercalated honeycomb magnet ${\mathrm{Ag}}_{3}\mathrm{Li}{\mathrm{Ir}}_{2}{\mathrm{O}}_{6}$. Based on x-ray absorption and resonant inelastic x-ray scattering measurements, and exact diagonalization calculations including nearest-neighbor Ir-Ir electron hopping integrals, we argue that the intercalation of Ag atoms results in a delocalized electronic structure with enhanced Ir-O hybridization, departing from the local relativistic ${j}_{\mathrm{eff}}=1/2$ state. We find that the relative orbital contribution to the magnetic moment is increased and the magnetization density is spatially extended and asymmetric in this hybridized state. Our results confirm the importance of metal-ligand hybridization in the magnetism of transition metal oxides and provide empirical guidance for understanding the collective magnetism in intercalated honeycomb iridates.

We present a comprehensive study of the three-metal boride alloys Mn0.95−δFe1.05 + δ−xCoxB ( δ = 0 − 0.15 and x = 0 − 1.05 ) synthesized via arc melting and annealing. The alloys crystallize in a body-centered tetragonal unit cell in the same space group ( I 4 / m c m ) as the parent compound Mn2B. A small amount of MB (M = Mn, Fe, Co) impurity forms in the as-cast samples which is removed by acid treatment. Rietveld refinement on the powder X-ray data reveals an anisotropic variation of lattice parameters in the series. The c-axis increases with increasing Co content but the a-axis decreases. Magnetic measurements show a non-monotonic variation of both T c and the saturated magnetization M s as a function of x. These findings highlight the tunable nature of Mn0.95−δFe1.05 + δ−xCoxB and motivate further studies of metal-rich boride alloys.

Strongly correlated electrons in layered perovskite structures have been the birthplace of high-temperature superconductivity, spin liquid, and quantum criticality. Specifically, the cuprate materials with layered structures made of corner sharing square planar CuO$_4$ units have been intensely studied due to their Mott insulating grounds state which leads to high-temperature superconductivity upon doping. Identifying new compounds with similar lattice and electronic structures has become a challenge in solid state chemistry. Here, we report the hydrothermal crystal growth of a new copper tellurite sulfate Cu$_3$(TeO$_4$)(SO$_4$)$\cdot$H$_2$O, a promising alternative to layered perovskites. The orthorhombic phase (space group $Pnma$) is made of corrugated layers of corner-sharing CuO$_4$ square-planar units that are edge-shared with TeO$_4$ units. The layers are linked by slabs of corner-sharing CuO$_4$ and SO$_4$. Using both the bond valence sum analysis and magnetization data, we find purely Cu$^{2+}$ ions within the layers, but a mixed valence of Cu$^{2+}$/Cu${^+}$ between the layers. Cu$_3$(TeO$_4$)(SO$_4$)$\cdot$H$_2$O undergoes an antiferromagnetic transition at $T_N$=67 K marked by a peak in the magnetic susceptibility. Upon further cooling, a spin-canting transition occurs at $T^{\star}$=12 K evidenced by a kink in the heat capacity. The spin-canting transition is explained based on a $J_1$-$J_2$ model of magnetic interactions, which is consistent with the slightly different in-plane super-exchange paths. We present Cu$_3$(TeO$_4$)(SO$_4$)$\cdot$H$_2$O as a promising platform for the future doping and strain experiments that could tune the Mott insulating ground state into superconducting or spin liquid states., 29 pages

Strongly correlated electrons in layered perovskite structures have been the birthplace of high-temperature superconductivity, spin liquids, and quantum criticality. Specifically, the cuprate materials with layered structures made of corner-sharing square-planar CuO

${\mathrm{Ag}}_{3}\mathrm{Li}{\mathrm{Ir}}_{2}{\mathrm{O}}_{6}$ is a Kitaev spin-liquid candidate material synthesized from $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{Li}}_{2}\mathrm{Ir}{\mathrm{O}}_{3}$ through a topotactic reaction. We investigate the structural and magnetic properties of two samples of ${\mathrm{Ag}}_{3}\mathrm{Li}{\mathrm{Ir}}_{2}{\mathrm{O}}_{6}$ based on the $^{7}\mathrm{Li}$ nuclear magnetic resonance line shape, Knight shift, and spin-lattice relaxation rate $1/{T}_{1}$. The first sample A shows signatures of magnetically ordered spins, and exhibits one sharp $^{7}\mathrm{Li}$ peak with the full width at half maximum increasing significantly below 14 K. $1/{T}_{1}^{\text{stretch}}$ of this sample displays a broad local maximum at 40 K, followed by a very sharp peak at ${T}_{N}=9\ifmmode\pm\else\textpm\fi{}1\phantom{\rule{0.16em}{0ex}}\mathrm{K}$ due to a critical slowing down of Ir spin fluctuations, a typical signature of magnetic long-range order. In order to shed light on the position-by-position variation of $1/{T}_{1}$ throughout the sample, we use a numerical inverse Laplace transform ${T}_{1}$ analysis based on Tikhonov regularization to deduce the density distribution function $P(1/{T}_{1})$. We demonstrate that $\ensuremath{\sim}60%$ of Ir spins are statically ordered at the NMR measurement timescale but the rest of the sample volume remains paramagnetic even at 4.2 K, presumably because of structural disorder induced primarily by stacking faults. In order to further investigate the influence of structural disorder, we compare these NMR results with those of a second sample B, which has been shown by transmission electron microscopy to have domains with unwanted Ag inclusion at the Li and Ir sites within the Ir honeycomb planes. Sample B displays an additional NMR peak with a relative intensity of $\ensuremath{\sim}17%$. The small Knight shift and $1/{T}_{1}$ of these defect-induced $^{7}\mathrm{Li}$ sites and the enhancement of bulk susceptibility at low temperatures suggest that these defects generate domains of only weakly magnetic Ir spins accompanied by free spins, leading to a lack of clear signatures of long-range order. The apparent lack of long-range order could be easily misinterpreted as evidence for the realization of a spin-liquid ground state in highly disordered Kitaev lattices.

Precision magnetometry is fundamental to the development of novel magnetic materials and devices. Recently, the nitrogen-vacancy (NV) center in diamond has emerged as a promising probe for static magnetism in 2D van der Waals materials, capable of quantitative imaging with nanoscale spatial resolution. However, the dynamic character of magnetism, crucial for understanding the magnetic phase transition and achieving technological applications, has rarely been experimentally accessible in single 2D crystals. Here, we coherently control the NV center's spin precession to achieve ultra-sensitive, quantitative ac susceptometry of a 2D ferromagnet. Combining dc hysteresis with ac susceptibility measurements varying temperature, field, and frequency, we illuminate the formation, mobility, and consolidation of magnetic domain walls in few-layer CrBr3. We show that domain wall mobility is enhanced in ultrathin CrBr3, with minimal decrease for excitation frequencies exceeding hundreds of kilohertz, and is influenced by the domain morphology and local pinning of the flake. Our technique extends NV magnetometry to the multi-functional ac and dc magnetic characterization of wide-ranging spintronic materials at the nanoscale., 11 pages, 5 figures

The search for an ideal Kitaev spin liquid candidate with anyonic excitations and long-range entanglement has motivated the synthesis of a new family of intercalated Kitaev magnets such as ${\mathrm{H}}_{3}\mathrm{Li}{\mathrm{Ir}}_{2}{\mathrm{O}}_{6}$, ${\mathrm{Cu}}_{2}\mathrm{Ir}{\mathrm{O}}_{3}$, and ${\mathrm{Ag}}_{3}\mathrm{Li}{\mathrm{Ir}}_{2}{\mathrm{O}}_{6}$. The absence of a susceptibility peak and a two-step release of the magnetic entropy in these materials have been proposed as evidence of proximity to the Kitaev spin liquid. Here we present a comparative study of the magnetic susceptibility, heat capacity, and muon spin relaxation ($\ensuremath{\mu}\mathrm{SR}$) between two samples of ${\mathrm{Ag}}_{3}\mathrm{Li}{\mathrm{Ir}}_{2}{\mathrm{O}}_{6}$ in the clean and disordered limits. In the disordered limit, the absence of a peak in either susceptibility or heat capacity and the lack of zero-field muon precession in the $\ensuremath{\mu}\mathrm{SR}$ signal give the impression of a proximate spin liquid state. However, in the clean limit, peaks are resolved in both susceptibility and heat capacity, and spontaneous oscillations appear in the $\ensuremath{\mu}\mathrm{SR}$ signal, confirming long-range antiferromagnetic order in the ground state. The $\ensuremath{\mu}\mathrm{SR}$ oscillations fit to a Bessel function, characteristic of incommensurate order, as reported in the parent compound $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{Li}}_{2}\mathrm{Ir}{\mathrm{O}}_{3}$. Our results clarify the role of structural disorder in the intercalated Kitaev magnets.

Whereas electron-phonon scattering relaxes the electron’s momentum in metals, a perpetual exchange of momentum between phonons and electrons may conserve total momentum and lead to a coupled electron-phonon liquid. Such a phase of matter could be a platform for observing electron hydrodynamics. Here we present evidence of an electron-phonon liquid in the transition metal ditetrelide, NbGe2, from three different experiments. First, quantum oscillations reveal an enhanced quasiparticle mass, which is unexpected in NbGe2 with weak electron-electron correlations, hence pointing at electron-phonon interactions. Second, resistivity measurements exhibit a discrepancy between the experimental data and standard Fermi liquid calculations. Third, Raman scattering shows anomalous temperature dependences of the phonon linewidths that fit an empirical model based on phonon-electron coupling. We discuss structural factors, such as chiral symmetry, short metallic bonds, and a low-symmetry coordination environment as potential design principles for materials with coupled electron-phonon liquid., It was predicted that in the regime of strong electron-phonon interactions, electrons and phonons can form a coupled non-equilibrium state, characterized by the conservation of the total momentum and by hydrodynamic transport. Here, the authors report experimental evidence for such a coupled electron-phonon liquid in NbGe2.

Whereas electron-phonon scattering typically relaxes the electron's momentum in metals, a perpetual exchange of momentum between phonons and electrons conserves total momentum and can lead to a coupled electron-phonon liquid with unique transport properties. This theoretical idea was proposed decades ago and has been revisited recently, but the experimental signatures of an electron-phonon liquid have been rarely reported. We present evidence of such a behavior in a transition metal ditetrelide, NbGe$_2$, from three different experiments. First, quantum oscillations reveal an enhanced quasiparticle mass, which is unexpected in NbGe$_2$ due to weak electron-electron correlations, hence pointing at electron-phonon interactions. Second, resistivity measurements exhibit a discrepancy between the experimental data and calculated curves within a standard Fermi liquid theory. Third, Raman scattering shows anomalous temperature dependence of the phonon linewidths which fits an empirical model based on phonon-electron coupling. We discuss structural factors, such as chiral symmetry, short metallic bonds, and a low-symmetry coordination environment as potential sources of coupled electron-phonon liquids., Comment: Preprint, 18 pages, 4 figures

$\mathrm{Cu_2IrO_3}$ is among the newest layered honeycomb iridates and a promising candidate to harbor a Kitaev quantum spin liquid state. Here, we investigate the pressure and temperature dependence of its structure through a combination of powder x-ray diffraction and x-ray absorption fine structure measurements, as well as $ab$-$initio$ evolutionary structure search. At ambient pressure, we revise the previously proposed $C2/c$ solution with a related but notably more stable $P2_1/c$ structure. Pressures below 8 GPa drive the formation of Ir-Ir dimers at both ambient and low temperatures, similar to the case of $\mathrm{Li_2IrO_3}$. At higher pressures, the structural evolution dramatically depends on temperature. A large discontinuous reduction of the Ir honeycomb interplanar distance is observed around 15 GPa at room temperature, likely driven by a collapse of the O-Cu-O dumbbells. At 15 K, pressures beyond 20 GPa first lead to an intermediate phase featuring a continuous reduction of the interplanar distance, which then collapses at 30 GPa across yet another phase transition. However, the resulting structure around 40 GPa is not the same at room and low temperatures. Remarkably, the reduction in interplanar distance leads to an apparent healing of the stacking faults at room temperature, but not at 15 K. Possible implications on the evolution of electronic structure of $\mathrm{Cu_2IrO_3}$ with pressure are discussed., Comment: 11 pages, 7 figures, see ancillary file for Supplemental Material

Dynamics and textures of magnetic domain walls (DWs) may largely alter the electronic behaviors in a Weyl semimetal system via emergent gauge fields. However, very little is known about even the basic properties of these domain walls in Weyl materials. In this work, we imaged the spontaneous magnetization and magnetic susceptibility of a ferromagnetic (FM) Weyl semimetal CeAlSi using scanning SQUID microscopy. We observed the ferromagnetic DWs lined-up with the [100] direction (or other degenerate directions). We also discovered the coexistence of stable and metastable domain phases, which arise likely due to magnetoelastic and magnetostriction effects and are expected to be highly tunable with small strains. We applied an in-plane external field as the CeAlSi sample was cooled down to below the magnetic phase transition of 8.3K, showing that the pattern of FM domains is strongly correlated with both the amplitude and the orientation of the external field even for weak fields of a few Gausses. The area of stable domains increases with field and reaches maximum when the field is parallel to the main crystallographic axes of the CeAlSi crystal. Our results suggest that the manipulation of these heterogeneous phases can provide a practical way to study the interplay between magnetism and electronic properties in Weyl systems, and that these systems can even serve as a new platform for magnetic sensors.

Emergent relativistic quasiparticles in Weyl semimetals are the source of exotic electronic properties such as surface Fermi arcs, the anomalous Hall effect and negative magnetoresistance, all observed in real materials. Whereas these phenomena highlight the effect of Weyl fermions on the electronic transport properties, less is known about what collective phenomena they may support. Here, we report a Weyl semimetal, NdAlSi, that offers an example. Using neutron diffraction, we found a long-wavelength helical magnetic order in NdAlSi, the periodicity of which is linked to the nesting vector between two topologically non-trivial Fermi pockets, which we characterize using density functional theory and quantum oscillation measurements. We further show the chiral transverse component of the spin structure is promoted by bond-oriented Dzyaloshinskii-Moriya interactions associated with Weyl exchange processes. Our work provides a rare example of Weyl fermions driving collective magnetism.

The magnetic properties of iron-based superconductors $A{\mathrm{Fe}}_{2}{\mathrm{As}}_{2}$ ($A=\mathrm{K}$, Cs, and Rb), which are characterized by the V-shaped dependence of the critical temperature (${T}_{\mathrm{c}}$) on pressure ($P$), were studied by means of the muon spin rotation/relaxation technique. In all three systems studied the magnetism was found to appear for pressures slightly below the critical one (${P}_{\mathrm{c}}$), i.e., at pressure where ${T}_{\mathrm{c}}(P)$ changes the slope. Rather than competing, magnetism and superconductivity in $A{\mathrm{Fe}}_{2}{\mathrm{As}}_{2}$ are coexisting at the $P\ensuremath{\gtrsim}{P}_{\mathrm{c}}$ pressure region. Our results support the scenario of a transition from one pairing state to another, with different symmetries on either side of ${P}_{\mathrm{c}}$.

Van der Waals (VdW) materials have opened new directions in the study of low dimensional magnetism. A largely unexplored arena is the intrinsic tuning of VdW magnets toward new ground-states. The chromium trihalides provided the first such example with a change of inter-layer magnetic coupling emerging upon exfoliation. Here, we take a different approach to engineer new ground-states, not by exfoliation, but by tuning the spin-orbit coupling (SOC) of the non-magnetic ligand atoms (Cl,Br,I). We synthesize a three-halide series, CrCl$_{3-x-y}$Br$_{x}$I$_{y}$, and map their magnetic properties as a function of Cl, Br, and I content. The resulting triangular phase diagrams unveil a frustrated regime near CrCl$_{3}$. First-principles calculations confirm that the frustration is driven by a competition between the chromium and halide SOCs. Furthermore, we reveal a field-induced change of inter-layer coupling in the bulk of CrCl$_{3-x-y}$Br$_{x}$I$_{y}$ crystals at the same field as in the exfoliation experiments., Comment: 22 pages, 6 figures

A developing frontier in condensed matter physics is the emergence of novel electromagnetic responses, such as topological and anomalous Hall effect (AHE), in ferromagnetic Weyl semimetals (FM-WSMs). Candidates of FM-WSM are limited to materials that preserve inversion symmetry and generate Weyl crossings by breaking time-reversal symmetry. These materials share three common features: a centrosymmetric lattice, a collinear FM ordering, and a large AHE observed when the field is parallel to the magnetic easy-axis. Here, we present CeAlSi as a new type of FM-WSM, where the Weyl nodes are stabilized by breaking inversion symmetry, but their positions are tuned by breaking time-reversal symmetry. Unlike the other FM-WSMs, CeAlSi has a noncentrosymmetric lattice, a noncollinear FM ordering, and a novel AHE that is anisotropic between the easy- and hard-axes. It also exhibits large FM domains that are promising for both device applications and an interplay between the Weyl nodes and FM domain walls., Preprint, 20 pages, 4 figures

Recent reports of superconductivity and magnetism in single crystals of [Li1−xFexOH]FeS show unexplained variations in both superconducting and magnetic properties. We investigate the effect of hydrothermal growth conditions on these properties and find that increasing the growth temperature systematically increases the superconducting transition temperature (Tc), sharpens the magnetic transition, and decreases the scattering rate (Γ). The slow rate of Tc suppression with increasing Γ indicates a conventional s-wave superconducting state according to the Abrikosov-Gorkov expression. Samples with higher scattering rate show broader magnetic transitions and a stronger temperature dependence in the magnetic susceptibility. These results identify disorder, due to interstitial iron impurities, as the unique internal parameter responsible for the unexplained variations in Tc and magnetic ordering. We demonstrate the optimal hydrothermal growth conditions to minimize disorder and maximize Tc in [Li1−xFexOH]FeS crystals.

Electrochemical CO2 reduction can convert CO2 into fuels and valuable chemicals using renewable electricity, which provides a prospective path toward large-scale energy storage. Au nanostructured e...

The properties of cuprate high-temperature superconductors are largely shaped by competing phases whose nature is often a mystery. Chiefly among them is the pseudogap phase, which sets in at a doping $p^*$ that is material-dependent. What determines $p^*$ is currently an open question. Here we show that the pseudogap cannot open on an electron-like Fermi surface, and can only exist below the doping $p_{FS}$ at which the large Fermi surface goes from hole-like to electron-like, so that $p^*$ $\leq$ $p_{FS}$. We derive this result from high-magnetic-field transport measurements in La$_{1.6-x}$Nd$_{0.4}$Sr$_x$CuO$_4$ under pressure, which reveal a large and unexpected shift of $p^*$ with pressure, driven by a corresponding shift in $p_{FS}$. This necessary condition for pseudogap formation, imposed by details of the Fermi surface, is a strong constraint for theories of the pseudogap phase. Our finding that $p^*$ can be tuned with a modest pressure opens a new route for experimental studies of the pseudogap., 15 pages, 5 figures, 7 supplemental figures

We present the first copper iridium binary metal oxide with the chemical formula Cu2IrO3. The material is synthesized from the parent compound Na2IrO3 by a topotactic reaction where sodium is exchanged with copper under mild conditions. Cu2IrO3 has the same monoclinic space group (C2/c) as Na2IrO3 with a layered honeycomb structure. The parent compound Na2IrO3 is proposed to be relevant to the Kitaev spin liquid on the basis of having Ir4+ with an effective spin of 1/2 on a honeycomb lattice. Remarkably, whereas Na2IrO3 shows a long-range magnetic order at 15 K and fails to become a true spin liquid, Cu2IrO3 remains disordered until 2.7 K, at which point a short-range order develops. Rietveld analysis shows less distortions in the honeycomb structure of Cu2IrO3 with bond angles closer to 120° compared to Na2IrO3. Thus, the weak short-range magnetism combined with the nearly ideal honeycomb structure places Cu2IrO3 closer to a Kitaev spin liquid than its predecessors.

Solid oxides with transition metals ions in unusual oxidation states attract enormous attention due to their electronic, magnetic and catalytic properties. Yet, no crystalline oxide compounds based on purely trivalent iridium have been characterized to date. Here, we present the synthesis and thorough investigation of the properties of the compounds K0.75Na0.25IrO2 and IrOOH, both containing trivalent iridium on a triangular lattice in layers of [IrO2]x-. K0.75Na0.25IrO2 crystallizes in a P2-structure with the space group P63mmc, while the crystal structure of IrOOH adopts the direct maximal subgroup P-3m1. The trivalent state of the iridium ion is discussed with regards to the iridium-oxygen bond length from X-ray diffraction, the chemical composition, the electronic and magnetic behavior of the material as well as X-ray photoemission spectroscopy. The discovery of a new valence state in ternary crystalline iridium oxides is not only of interest from a fundamental perspective, but has far-reaching implic...

Broadening the knowledge and understanding on the magnetic correlations in van der Waals layered magnets is critical in realizing their potential next-generation applications. In this study, we employ high frequency (240 GHz) electron spin resonance (ESR) spectroscopy on plate-like CrBr$_{3}$ to gain insight into the magnetic interactions as a function of temperature (200 - 4 K) and the angle of rotation ${\theta}$. We find that the temperature dependence of the ESR linewidth is well described by the Ginzberg-Landau critical model as well as Berezinskii-Kosterlitz-Thouless (BKT) transition model, indicative of the presence of two-dimensional (2D) correlations. This suggests that the three-dimensional ferromagnet CrBr$_{3}$, which has been described as an Ising or Heisenberg ferromagnet, could present 2D magnetic correlations and BKT-like behavior even in its bulk form; an observation that, to the best of our knowledge, has not been reported in the literature. Furthermore, our findings show that the resonance field follows a $(3cos^2{\theta} - 1)$-like angular dependence, while the linewidth follows a $(3cos^2{\theta} - 1)^2$-like angular dependence. This observed angular dependence of the resonance field and linewidth further confirm an unanticipated 2D magnetic behavior in CrBr$_{3}$. This behavior is likely due to the interaction of the external magnetic field applied during the ESR experiment that allows for the mediation of long-range vortex-like correlations between the spin clusters that may have formed due to magnetic phase separation. This study demonstrates the significance of employing spin sensitive techniques such as ESR to better understand the magnetic correlations in similar van der Waals magnets., Comment: 6 pages, 5 figures, 1 table

Kitaev magnets are materials with bond-dependent Ising interactions between localized spins on a honeycomb lattice. Such interactions could lead to a quantum spin-liquid (QSL) ground state at zero temperature. Recent theoretical studies suggest two potential signatures of a QSL at finite temperatures, namely, a scaling behavior of thermodynamic quantities in the presence of quenched disorder, and a two-step release of the magnetic entropy. Here, we present both signatures in ${\mathrm{Ag}}_{3}{\mathrm{LiIr}}_{2}{\mathrm{O}}_{6}$ which is synthesized from $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{Li}}_{2}{\mathrm{IrO}}_{3}$ by replacing the interlayer Li atoms with Ag atoms. In addition, the dc susceptibility data confirm the absence of a long-range order, and the ac susceptibility data rule out a spin-glass transition. These observations suggest a closer proximity to the QSL in ${\mathrm{Ag}}_{3}{\mathrm{LiIr}}_{2}{\mathrm{O}}_{6}$ compared to its parent compound $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{Li}}_{2}{\mathrm{IrO}}_{3}$ that orders at 15 K. We discuss an enhanced spin-orbit coupling due to a mixing between silver $d$ and oxygen $p$ orbitals as a potential underlying mechanism.

Nuclear magnetic resonance experiments reveal how electron spins fluctuate in Cu${}_{2}$IrO${}_{3}$, a test as to whether this material meets the criteria for an exotic---and still theoretical---magnetic state known as a Kitaev spin liquid.

Anyonic excitations emerging from a Kitaev spin liquid can form a basis for quantum computers. Searching for such excitations motivated intense research on the honeycomb iridate materials. However, access to a spin liquid ground state has been hindered by magnetic ordering. Cu2IrO3 is a new honeycomb iridate without thermodynamic signatures of a long-range order. Here, we use muon spin relaxation to uncover the magnetic ground state of Cu2IrO3. We find a two-component depolarization with slow and fast relaxation rates corresponding to distinct regions with dynamic and static magnetism, respectively. X-ray absorption spectroscopy and first principles calculations identify a mixed copper valence as the origin of this behavior. Our results suggest that a minority of Cu2+ ions nucleate regions of static magnetism whereas the majority of Cu+/Ir4+ on the honeycomb lattice give rise to a Kitaev spin liquid.

Materials with strong magnetoresistive responses are the backbone of spintronic technology, magnetic sensors, and hard drives. Among them, manganese oxides with a mixed valence and a cubic perovskite structure stand out due to their colossal magnetoresistance (CMR). A double exchange interaction underlies the CMR in manganates, whereby charge transport is enhanced when the spins on neighboring Mn3+ and Mn4+ ions are parallel. Prior efforts to find different materials or mechanisms for CMR resulted in a much smaller effect. Here we show an enormous CMR at low temperatures in EuCd2P2 without manganese, oxygen, mixed valence, or cubic perovskite structure. EuCd2P2 has a layered trigonal lattice and exhibits antiferromagnetic ordering at 11 K. The magnitude of CMR (104 percent) in as-grown crystals of EuCd2P2 rivals the magnitude in optimized thin films of manganates. Our magnetization, transport, and synchrotron X-ray data suggest that strong magnetic fluctuations are responsible for this phenomenon. The realization of CMR at low temperatures without heterovalency leads to a new regime for materials and technologies related to antiferromagnetic spintronics.

This work presents an integrated approach to study the crystal chemistry and phonon heat capacity of complex layered oxides. Two quaternary delafossites are synthesized from ternary parent compounds and copper monohalides via a topochemical exchange reaction that preserves the honeycomb ordering of the parent structures. For each compound, Rietveld refinement of the powder X-ray diffraction patterns is examined in both monoclinic C2/ c and rhombohedral R3̅ m space groups. Honeycomb ordering occurs only in the monoclinic space group. Bragg peaks associated with honeycomb ordering acquire an asymmetric broadening known as the Warren line shape that is commonly observed in layered structures with stacking disorder. Detailed TEM analysis confirms honeycomb ordering within each layer in both title compounds and establishes a twinning between the adjacent layers instead of the more conventional shifting or skipping stacking faults. The structural model is then used to calculate phonon dispersions and heat capacity from first principles. In both compounds, the calculated heat capacity accurately describes the experimental data. The integrated approach presented here offers a platform to carefully analyze the phonon heat capacity in complex oxides where the crystal structure can produce magnetic frustration. Isolating phonon contribution from total heat capacity is a necessary and challenging step toward a quantitative study of spin liquid materials with exotic magnetic excitations such as spinons and Majorana fermions. A quantitative understanding of phonon density of states based on crystal chemistry as presented here also paves the way toward higher efficiency thermoelectric materials.

A quantum spin liquid is an exotic quantum state of matter that does not exhibit any classical magnetic ordered ground state. The realization of such a state in actual materials is of significant importance as it would provide a path to protected states for quantum information applications and also to Majorana fermions - both areas of vigorous current activity and interest in condensed matter physics. However, no solid evidence for the existence of such materials has been established in the laboratory, despite a decades-long search. Here, the authors report the pressure-induced melting of magnetic order and emergence of a new quantum state in \ensuremath{\alpha}-RuCl${}_{3}$, a candidate compound in the proximity of a quantum spin-liquid state. The high-pressure phase is found to be extremely robust against applied pressure up to ~140 GPa.

Recent debates in the literature over the relationship between topology and Extreme Magnetoresistance (XMR) have drawn attention to the Lanthanum Monopnictide family of binary compounds. Angle resolved photoemission spectroscopy (ARPES) is used to measure the electronic structure of the XMR topological semimetal candidates LaBi, LaSb, and LaAs. The orbital content of the near-E F states in LaBi and LaSb are extracted using varying photon polarizations and both dominant d and p bands are observed near X. The measured bulk bands are shifted in energy when compared to the results of Density Functional Calculations. This disagreement is minor in LaBi, but large in LaSb and LaAs. The measured bulk band structure of LaBi shows a clear band inversion and puts LaBi in the υ = 1 class of Topological Insulators (or semimetals), as predicted by calculations and consistent with the measured Dirac-like surface states. LaSb is on the verge of a band inversion with a less-clear case for any distinctly topological surface states and in disagreement with calculations. Lastly, these same bands in LaAs are clearly non-inverted implying its topological triviality and demonstrating a topological phase transition in the Lanthanum monopnictides. Using a wide range of photon energies the true bulk states are cleanly disentangled from the various types of surface states which are present. These surface states exist due to surface projections of bulk states in LaSb and for topological reasons in LaBi. Lanthanum monopnictides are drawing interest because they are topological semimetal candidates and they exhibit extreme magnetoresistance, that is, they transition from being good metals to having high resistance when a magnetic field is applied. Extreme magnetoresistance is very interesting in view of applications, but the mechanism behind it is not understood yet. Daniel Dessau at the University of Colorado and collaborators performed angle-resolved photoemission spectroscopy measurements and density functional theory calculations to investigate the electronic structure of lanthanum monopnictides and its connection with extreme magnetoresistance. LaBi shows band inversion and is thus a topological material, whereas the case is less clear for LaSb, which is close to band inversion. LaAs is topologically trivial. The results suggest that the connection between topology and extreme magnetoresistance might be less clear than previously thought.

The family of binary Lanthanum monopnictides, LaBi and LaSb, have attracted a great deal of attention as they display an unusual extreme magnetoresistance (XMR) that is not well understood. Two classes of explanations have been raised for this: the presence of non-trivial topology, and the compensation between electron and hole densities. Here, by synthesizing a new member of the family, LaAs, and performing transport measurements, Angle Resolved Photoemission Spectroscopy (ARPES), and Density Functional Theory (DFT) calculations, we show that (a) LaAs retains all qualitative features characteristic of the XMR effect but with a siginificant reduction in magnitude compared to LaSb and LaBi, (b) the absence of a band inversion or a Dirac cone in LaAs indicates that topology is insignificant to XMR, (c) the equal number of electron and hole carriers indicates that compensation is necessary for XMR but does not explain its magnitude, and (d) the ratio of electron and hole mobilities is much different in LaAs compared to LaSb and LaBi. We argue that the compensation is responsible for the XMR profile and the mobility mismatch constrains the magnitude of XMR., 8 pages, 4 figures

Magnetic van der Waals (vdW) materials are the centerpiece of atomically thin devices with spintronic and optoelectronic functions. Exploring new chemistry paths to tune their magnetic and optical properties enables significant progress in fabricating heterostructures and ultracompact devices by mechanical exfoliation. The key parameter to sustain ferromagnetism in 2D is magnetic anisotropy-a tendency of spins to align in a certain crystallographic direction known as easy-axis. In layered materials, two limits of easy-axis are in-plane (XY) and out-of-plane (Ising). Light polarization and the helicity of topological states can couple to magnetic anisotropy with promising photoluminescence or spin-orbitronic functions. Here, a unique experiment is designed to control the easy-axis, the magnetic transition temperature, and the optical gap simultaneously in a series of CrCl

A series of transport experiments on lanthanum antimonide reveal a plateau in its resistivity and an extremely large magnetoresistance that are consistent with topologically protected electronic states.

We report the observation of an extreme magnetoresistance (XMR) in HoBi with a large magnetic moment from Ho f-electrons. Neutron scattering is used to determine the magnetic wave vectors across several metamagnetic (MM) transitions on the phase diagram of HoBi. Unlike other magnetic rare-earth monopnictides, the field dependence of resistivity in HoBi is non-monotonic and reveals clear signatures of every metamagnetic transition in the low-temperature and low-field regime, at T < 2 K and H < 2.3 T. The XMR appears at H > 2.3 T after all the metamagnetic transitions are complete and the system is spin-polarized by the external magnetic field. The existence of an onset field for XMR and the intimate connection between magnetism and transport in HoBi are unprecedented among the magnetic rare-earth monopnictides. Therefore, HoBi provides a unique opportunity to understand the electrical transport in magnetic XMR semimetals., 6 pages, 4 figures

International audience; This work presents an integrated approach to study the crystal chemistry and phonon heat capacity of complex layered oxides. Two quaternary delafossites are synthesized from ternary parent compounds and copper monohalides via a topochemical exchange reaction that preserves the honeycomb ordering of the parent structures. For each compound, Rietveld refinement of the powder X-ray diffraction patterns is examined in both monoclinic C2/c and rhombohedral R (3) over barm space groups. Honeycomb ordering occurs only in the monoclinic space group. Bragg peaks associated with honeycomb ordering acquire an asymmetric broadening known as the Warren line shape that is commonly observed in layered structures with stacking disorder. Detailed TEM analysis confirms honeycomb ordering within each layer in both title compounds and establishes a twinning between the adjacent layers instead of the more conventional shifting or skipping stacking faults. The structural model is then used to calculate phonon dispersions and heat capacity from first principles. In both compounds, the calculated heat capacity accurately describes the experimental data. The integrated approach presented here offers a platform to carefully analyze the phonon heat capacity in complex oxides where the crystal structure can produce magnetic frustration. Isolating phonon contribution from total heat capacity is a necessary and challenging step toward a quantitative study of spin liquid materials with exotic magnetic excitations such as spinons and Majorana fermions. A quantitative understanding of phonon density of states based on crystal chemistry as presented here also paves the way toward higher efficiency thermoelectric materials.

We present the first copper iridium binary metal oxide with the chemical formula Cu