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The metallic delafossites host ultra-high mobility carriers in the bulk, while at their polar surfaces, intrinsic electronic reconstructions stabilise markedly distinct electronic phases, from charge-disproportionated insulators, to Rashba-split heavy-hole gases and ferromagnetic metals. The understanding of these phases has been strongly informed by surface spectroscopic measurements, but previous studies have been complicated by the presence of spatially varying terminations of the material surface. Here, we demonstrate the potential of microscopic-area angle-resolved photoemission to overcome these challenges. Our measurements of the model compound PdCoO$_2$ yield extremely high-quality spectra of the electronic structure, which allows us to place new experimental constraints on the weak electron-phonon coupling in the bulk of PdCoO$_2$, while revealing much stronger interactions at its surfaces. While the CoO$_2$-terminated surface exhibits a conventional weak-coupling behavior, our measurements reveal surprising spectroscopic signatures of polaron formation at the Pd-terminated surface, despite its pronounced metallicity. Together, our findings reveal how mode and symmetry-selective couplings can markedly tune the electron-phonon interactions in a single host material, here opening routes to stabilise surprisingly persistent polaronic quasiparticles., Comment: 17 pages including supplementary information

The stability of the double-layered antiferromagnets and their magnonic properties are investigated by considering two model systems, the linear chain (LC) and more complex chain of railroad trestle (RT) geometry, and a real example of chromium nitride CrN. The spin-paired order ($\cdots{+}{+}{-}{-}\cdots$) in LC requires an alternation of the ferromagnetic and antiferromagnetic (AFM) interactions, while analogous spin-paired order in RT can be stable even for all magnetic exchange interactions being AFM. The rock-salt structure of CrN evokes clear magnetic frustration since Cr atoms in face-centered cubic lattice form links to twelve nearest neighbors all equivalent and AFM. Nonetheless, the magnetostructural transition to an orthorhombically distorted phase below $T_\text{N} = 287~\text{K}$ leads to a diversification of Cr-Cr links, which suppresses the frustration and allows for stable double-layered AFM order of CrN. Based on $\textit{ab initio}$ calculated exchange parameters, the magnon spectra and temperature evolution of ordered magnetic moments are derived., Comment: 7 pages, 8 figures

We present a detailed theoretical study of the electronic structure of hafnium tin HfSn crystallizing in a B$20$ structure, renowned for the diversity of physical and peculiar topological properties. The chiral crystal structure of these materials protects multifold band crossings located at high symmetry points. We employ density functional methods to reveal basic features of the band structure and Fermi surface topology of HfSn, on top of which an effective tight-binding model is built. The compound exhibits a fourfold band crossing pinned at the ${\Gamma}$ point. We investigate routes that can shift such crossings towards the Fermi level, offering a unique way to possibly tune the compound`s properties. Specifically, we show that the energy position of the fourfold crossing can be easily manipulated via external perturbations such as strain and pressure. Considering that this point carries a topological charge larger than one, such tuning is of great importance. We anticipate that the approach presented in the current study can be utilized to investigate symmetry protected crossings in a wide class of materials.

Based on our first detailed $^{181}$Ta nuclear quadrupole resonance (NQR) studies from 2017 on the Weyl semimetal TaP, we now extended our NQR studies to another Ta-based monopnictide TaAs. In the present work, we have determined the temperature-dependent $^{181}$Ta-NQR spectra, the spin-lattice relaxation time $T_{1}$, and the spin-spin relaxation time $T_{2}$. We found the following characteristic features that showed great contrast to what was found in TaP: (1) The quadrupole coupling constant and asymmetry parameter of EFG, extracted from three NQR frequencies, have a strong temperature dependence above $\sim$80 K that cannot be explained by the density functional theory calculation incorporating the thermal expansion of the lattice. (2) The temperature dependence of the spin-lattice relaxation rate, $1/T_{1} T$, shows a $T^{4}$ power law behavior above $\sim$30 K. This is a great contrast with the $1/T_{1} T \propto T^{2}$ behavior found in TaP, which was ascribed to the magnetic excitations at the Weyl nodes with a temperature-dependent orbital hyperfine coupling. (3) Regarding the nuclear spin-spin interaction, we found the spin-echo signal decays with the pulse separation simply by a Lorentzian function in TaAs, but we have observed spin-echo modulations in TaP that is most likely due to the indirect nuclear spin-spin coupling via virtually excited Weyl fermions. From our experimental findings, we conclude that the present NQR results do not show dominant contributions from Weyl fermion excitations in TaAs., Comment: 8 pages, 10 figures

Progress in magnetoelectric materials is hindered by apparently contradictory requirements for time-reversal symmetry broken and polar ferroelectric electronic structure in common ferromagnets and antiferromagnets. Alternative routes could be provided by recent discoveries of a time-reversal symmetry breaking anomalous Hall effect in noncollinear magnets and altermagnets, but hitherto reported bulk materials are not polar. Here, we report the observation of a spontaneous anomalous Hall effect in doped AgCrSe$_2$, a layered polar semiconductor with an antiferromagnetic coupling between Cr spins in adjacent layers. The anomalous Hall resistivity 3 $\mu\Omega$ cm is comparable to the largest observed in compensated magnetic systems to date, and is rapidly switched off when the angle of an applied magnetic field is rotated to $\sim 80^{\circ}$ from the crystalline $c$-axis. Our ionic gating experiments show that the anomalous Hall conductivity magnitude can be enhanced by modulating the $p$-type carrier density. We also present theoretical results that suggest the anomalous Hall effect is driven by Berry curvature due to noncollinear antiferromagnetic correlations among Cr spins, which are consistent with the previously suggested magnetic ordering in AgCrSe$_2$. Our results open the possibility to study the interplay of magnetic and ferroelectric-like responses in this fascinating class of materials., Comment: 8 pages, 5 figures

The layered delafossite metal PdCrO$_2$ is a natural heterostructure of highly conductive Pd layers Kondo coupled to localized spins in the adjacent Mott insulating CrO$_2$ layers. At high temperatures $T$ it has a $T$-linear resistivity which is not seen in the isostructural but non-magnetic PdCoO$_2$. The strength of the Kondo coupling is known, as-grown crystals are extremely high purity and the Fermi surface is both very simple and experimentally known. It is therefore an ideal material platform in which to investigate 'Planckian metal' physics. We do this by means of controlled introduction of point disorder, measurement of the thermal conductivity and Lorenz ratio and studying the sources of its high temperature entropy. The $T$-linear resistivity is seen to be due mainly to elastic scattering and to arise from a sum of several scattering mechanisms. Remarkably, this sum leads to a scattering rate within 10$\%$ of the Planckian value of $k_BT/$$\hbar$.

Spatial inversion symmetry in crystal structures is closely related to the superconducting (SC) and magnetic properties of materials. Recently, several theoretical proposals that predict various interesting phenomena caused by the breaking of the local inversion symmetry have been presented. However, experimental validation has not yet progressed owing to the lack of model materials. Here we present evidence for antiferromagnetic (AFM) order in CeRh$_{2}$As$_{2}$ (SC transition temperature $T_{\rm SC} \sim 0.37$~K), wherein the Ce site breaks the local inversion symmetry. The evidence is based on the observation of different extents of broadening of the nuclear quadrupole resonance spectrum at two crystallographically inequivalent As sites. This AFM ordering breaks the inversion symmetry of this system, resulting in the activation of an odd-parity magnetic multipole. Moreover, the onset of antiferromagnetism $T_{\rm N}$ within an SC phase, with $T_{\rm N} < T_{\rm SC}$, is quite unusual in systems wherein superconductivity coexists or competes with magnetism. Our observations show that CeRh$_{2}$As$_{2}$ is a promising system to study how the absence of local inversion symmetry induces or influences unconventional magnetic and SC states, as well as their interaction., Comment: 6 pages, 3 figures, to be published in PRL

Applying in-plane uniaxial pressure to strongly correlated low-dimensional systems has been shown to tune the electronic structure dramatically. For example, the unconventional superconductor Sr$_2$RuO$_4$ can be tuned through a single Van Hove singularity which results in a strong enhancement of both $T_\text{c}$ and $H_\text{c2}$. Out-of-plane ($c$ axis) uniaxial pressure is expected to tune the quasi-two-dimensional structure even more strongly, causing it to approach two Van Hove singularities simultaneously. Here we achieve a record value of $3.2$ GPa compression along the $c$ axis of Sr$_2$RuO$_4$. Although the rise in $H_\text{c2}$ shows that we are indeed approaching the van Hove points, $T_\text{c}$ is suppressed, a result that contradicts expectations based on simple two-dimensional models. As a first attempt to take the third dimension into account, we present three-dimensional calculations in the weak interaction limit, and discuss the extent to which they are consistent with observation. Our experimental results highlight the importance of out-of-plane effects in low-dimensional systems in general and provide new constraints on theories of the pairing interaction in Sr$_2$RuO$_4$.

The magnetic, thermal and transport properties as well as electronic band structure of MnPtSi are reported. MnPtSi is a metal that undergoes a ferromagnetic transition at $T_{\mathrm{C}}=340$(1) K and a spin-reorientation transition at $T_{\mathrm{N}}=326$(1) K to an antiferromagnetic phase. First-principles electronic structure calculations indicate a not-fully polarized spin state of Mn in a $d^5$ electron configuration with $J=S=3$/2, in agreement with the saturation magnetization of 3~$\mu_{\mathrm{B}}$ in the ordered state and the observed paramagnetic effective moment. A sizeable anomalous Hall effect in the antiferromagnetic phase alongside the computational study suggests that the antiferromagnetic structure is non-collinear. Based on thermodynamic and resistivity data we construct a magnetic phase diagram. Magnetization curves $M$($H$) at low temperatures reveal a metamagnetic transition of spin-flop type. The spin-flopped phase terminates at a critical point with $T_{\mathrm{cr}}\approx 300$ K and $H_{\mathrm{cr}}\approx 10$ kOe, near which a peak of the magnetocaloric entropy change is observed. Using Arrott plot analysis and magnetoresistivity data we argue that the metamagnetic transition is of a first-order type, whereas the strong field dependence of $T_{\mathrm{N}}$ and the linear relationship of the $T_{\mathrm{N}}$ with $M^2$ hint at its magnetoelastic nature.

We present inelastic neutron scattering data on the quantum paramagnet AgVOAsO4 that establish the system is a S=1/2 alternating spin chain compound and provide a direct measurement of the spin gap. We also present experimental evidence for two different types of field-induced magnetic order between mu_0H_c1 = 8.4T and mu_0H_c2 = 48.9T, which may be related to Bose-Einstein condensation (BEC) of triplons. Thermodynamic measurements in magnetic fields up to 60T and temperatures down to 0.1K reveal a H-T phase diagram consisting of a dome encapsulating two ordered phases with maximum ordering temperatures of 3.8K and 5.3K respectively. This complex phase diagram is not expected for a single-Q BEC system and therefore establishes AgVOAsO4 as a promising multi-Q BEC candidate capable of hosting exotic vortex phases.

We present a detailed study of the temperature evolution of the crystal structure, specific heat, magnetic susceptibility and resistivity of single crystals of the paradigmatic valence-fluctuating compound EuIr$_2$Si$_2$. A comparison to stable-valent isostructural compounds EuCo$_2$Si$_2$ (with Eu$^{3+}$), and EuRh$_2$Si$_2$, (with Eu$^{2+}$) reveals an anomalously large thermal expansion indicative of the lattice softening associated to valence fluctuations. A marked broad peak at temperatures around 65-75 K is observed in specific heat, susceptibility and the derivative of resistivity, as thermal energy becomes large enough to excite Eu into a divalent state, which localizes one f electron and increases scattering of conduction electrons. In addition, the intermediate valence at low temperatures manifests in a moderately renormalized electron mass, with enhanced values of the Sommerfeld coefficient in the specific heat and a Fermi-liquid-like dependence of resistivity at low temperatures. The high residual magnetic susceptibility is mainly ascribed to a Van Vleck contribution. Although the intermediate/fluctuating valence duality is to some extent represented in the interconfiguration fluctuation model commonly used to analyze data on valence-fluctuating systems, we show that this model cannot describe the different physical properties of EuIr$_2$Si$_2$ with a single set of parameters., Comment: 12 pages, 4 figures, 1 table

We study the electronic structure of delafossite PtCoO$_2$ to elucidate its extremely small resistivity and high mobility. The band exhibits steep dispersion near the Fermi level despite the fact that it is formed mainly by Pt $d$ orbitals that are typically localized. We propose a picture based on two hidden kagome-lattice-like electronic structure: one originating from Pt $s+p_x/p_y$ orbitals, and the other from Pt $d_{3z^2-r^2}+d_{xy}/d_{x^2-y^2}$ orbitals, each placed on the bonds of the triangular lattice. In particular, we find that the underlying Pt $s+p_x/p_y$ bands actually determine the steepness of the original dispersion, so that the large Fermi velocity can be attributed to the large width of the Pt $s+p_x/p_y$ band. More importantly, the kagome-like electronic structure gives rise to "orbital-momentum locking" on the Fermi surface, which reduces the electron scattering by impurities. We conclude that the combination of the large Fermi velocity and the orbital-momentum locking is likely to be the origin of the extremely small resistivity in PtCoO$_2$., Comment: 9 pages, 14 figures

The two-dimensional (2D) metal PtCoO$_2$ is renowned for the lowest room temperature resistivity among all oxides, close to that of the top two materials Ag and Cu. In addition, we theoretically predict a strong intrinsic spin Hall effect. This originates from six strongly-tilted Dirac cones that we find in the electronic structure near the Fermi surface, where a gap is opened by large spin-orbit coupling (SOC). This is underpinned by rich topological properties; in particular, the phenomenology of a mirror Chern metal is realized not exactly, but very accurately, on account of an approximate crystalline symmetry. We expect that such 'vicinity topology' to be a feature of relevance well beyond this material. Our Wilson loop analysis indicates further elaborate features such as fragile topology. These findings highlight PtCoO$_2$ as a promising material for spintronic applications as well as a platform to study the interplay of symmetry and topology., Comment: 9 pages, 7 figures

The crystalline electric field (CEF) of Ce3+ in trigonal symmetry has recently become of some relevance, for instance, in the search of frustrated magnetic systems. Fortunately, it is one of the CEF case in which a manageable analytic solution can be obtained. Here, we present this solution for the general case, and use this result to determine the CEF scheme of the new compound CeIr3Ge7 with the help of T-dependent susceptibility and isothermal magnetization measurements. The resulting CEF parameters B20 = 34.4 K, B40 = 0.82 K and B43 = 67.3 K correspond to an exceptional large CEF splittings of the first and second excited levels, 374 K and 1398 K, and a large mixing between the +-|5/2> and the -+|1/2> states. This indicates a very strong easy plane anisotropy with an unusual small c-axis moment. Using the same general expressions, we show that the properties of the recently reported system CeCd3As3 can also be described by a similar CEF scheme, providing a much simpler explanation for its magnetic properties than the initial proposal. Moreover, a similar strong easy plane anisotropy has also been reported for the two compounds CeAuSn and CePdAl4Ge2, indicating that the CEF scheme elaborated here for CeIr3Ge7 corresponds to an exemplary case for Ce3+ in trigonal symmetry., Comment: 10 pages, 7 figures

We have studied magneto transport in the single-band, quasi-two-dimensional metals PdCoO2 and PtCoO2, which have extremely long mean free paths. We observer a strong temperature dependence of the Hall resistivity in small applied, fields, linked to a large violation of Kohler's rule in the magnetoresistance. We discuss the extent to which these observations can be accounted for by standard transport theory, and describe other possible, unconventional contributions to magnetotransport in very high purity metals.

We report on a combined study of the de Haas-van Alphen effect and angle resolved photoemission spectroscopy on single crystals of the metallic delafossite PdRhO$_2$ rounded off by \textit{ab initio} band structure calculations. A high sensitivity torque magnetometry setup with SQUID readout and synchrotron-based photoemission with a light spot size of $~50\,\mu\mathrm{m}$ enabled high resolution data to be obtained from samples as small as $150\times100\times20\,(\mu\mathrm{m})^3$. The Fermi surface shape is nearly cylindrical with a rounded hexagonal cross section enclosing a Luttinger volume of 1.00(1) electrons per formula unit.

We report on the electronic band structure, structural, magnetic and thermal properties of Ce$_2$Rh$_3$Sn$_5$. Ce $L_{\mathrm{III}}$-edge XAS spectra give direct evidence for an intermediate valence behaviour. Thermodynamic measurements reveal magnetic transitions at $T_{\mathrm{N1}}\approx$ 2.9 K and $T_{\mathrm{N2}}\approx$ 2.4 K. Electrical resistivity shows behaviour typical for Kondo lattices. The coexistence of magnetic order and valence fluctuations in a Kondo lattice system we attribute to a peculiar crystal structure in which Ce ions occupy two distinct lattice sites. Analysis of the structural features of Ce$_2$Rh$_3$Sn$_5$, together with results of electronic band structure calculations and thermodynamic data indicate that Ce2 ions are in an intermediate valence state with the ground state electronic configuration close to 4$f^0$, whereas Ce1 ions are trivalent (4$f^1$) and contribute to the low temperature magnetic ordering. Thus, our joined experimental and theoretical investigations classify Ce$_2$Rh$_3$Sn$_5$ as a multivalent charge-ordered system., Comment: 12 pages with 10 figures (main manuscript) and 2 pages with 2 figures (supplementary information)

In this joint experimental and theoretical work magnetic properties of the Cu$^{2+}$ mineral szenicsite Cu$_3$(MoO$_4$)(OH)$_4$ are investigated. This compound features isolated triple chains in its crystal structure, where the central chain involves an edge-sharing geometry of the CuO$_4$ plaquettes, while the two side chains feature a corner-sharing zig-zag geometry. The magnetism of the side chains can be described in terms of antiferromagnetic dimers with a coupling larger than 200 K. The central chain was found to be a realization of the frustrated antiferromagnetic $J_1$-$J_2$ chain model with $J_1\simeq 68$ K and a sizable second-neighbor coupling $J_2$. The central and side chains are nearly decoupled owing to interchain frustration. Therefore, the low-temperature behavior of szenicsite should be entirely determined by the physics of the central frustrated $J_1$-$J_2$ chain. Our heat-capacity measurements reveal an accumulation of entropy at low temperatures and suggest a proximity of the system to the Majumdar-Ghosh point of the antiferromagnetic $J_1$-$J_2$ spin chain, $J_2/J_1=0.5$.

Cuprate materials, like those hosting high temperature superconductivity, represent a famous class of materials where the correlations between the strongly entangled charges and spins produce complex phase diagrams. Several years ago the Zhang-Rice singlet was proposed as a natural quasiparticle in hole-doped cuprates. The occurance and binding energy of this quasiparticle, consisting of a pair of bound holes with antiparallel spins on the same CuO$_4$ plaquette, depends on the local electronic interactions, which are fundamental quantities for understanding the physics of the cuprates. Here, we employ state-of-the-art Resonant Inelastic X-ray Scattering (RIXS) to probe the correlated physics of the CuO$_4$ plaquettes in the quasi-one dimensional chain cuprate Li$_2$CuO$_2$. By tuning the incoming photon energy to the O $K$-edge, we populate bound states related to the Zhang-Rice quasiparticles in the RIXS process. Both intra- and interchain Zhang-Rice singlets are observed and their occurrence is shown to depend on the nearest-neighbor spin-spin correlations, which are readily probed in this experiment. We also extract the binding energy of the Zhang-Rice singlet and identify the Zhang-Rice triplet excitation in the RIXS spectra., Comment: 8 pages, 4 figures, accepted for publication in Physical Review B

Two new ternary borides $TM$$_7$Fe$_3$B$_8$ ($TM$ = Nb, Ta) were synthesized by high-temperature thermal treatment of samples obtained by arc-melting. This new type of structure with space group $P$6/$mmm$, comprises $TM$ slabs containing isolated planar hexagonal [B$_6$] rings and iron centered $TM$ columns in a Kagome type of arrangement. Chemical bonding analysis in Nb$_7$Fe$_3$B$_8$ by means of the electron localizability approach reveals two-center interactions forming the Kagome net of Fe and embedded B, while weaker multicenter bonding present between this net and Nb atoms. Magnetic susceptibility measurements reveal antiferromagnetic order below $T_N$ = 240 K for Nb$_7$Fe$_3$B$_8$ and $T_N$ =265 K for Ta$_7$Fe$_3$B$_8$. Small remnant magnetization below 0.01 $\mu_B$/f.u. is observed in the antiferromagnetic state. The bulk nature of the magnetic transitions was confirmed by the hyperfine splitting of the M\"o{\ss}bauer spectra, the sizable anomalies in the specific heat capacity, and the kinks in the resistivity curves. The high-field paramagnetic susceptibilities fitted by the Curie-Weiss law show effective paramagnetic moments $\mu_{eff}$ about 3.1 $\mu_B$/Fe in both compounds. The temperature dependence of the electrical resistivity also reveals metallic character of both compounds. Density functional calculations corroborate the metallic behaviour of both compounds and demonstrate the formation of a sizable local magnetic moment on the Fe-sites. They indicate the presence of both antiferro- and ferromagnetic interactions., Comment: 11 pages, 11 figures

We report a combined experimental and theoretical study of the dependence of the superconductivity of the unconventional superconductor Sr$_2$RuO$_4$ on anisotropic strain. Novel piezoelectric apparatus is used to apply uniaxial pressures of up to $\sim$1~GPa along a $\langle 100 \rangle$ direction ($a$-axis) of the crystal lattice. $T_c$ increases from 1.5~K in unstrained material to 3.4~K at compression by $\approx$0.6\%, then falls steeply. The $c$-axis upper critical field for the strained $T_c$ = 3.4~K material is a factor of twenty larger than that of the unstrained crystal, whereas the in-plane ($a$-axis) critical field increases by only a factor of three. First-principles electronic structure calculations give evidence that the observed maximum $T_c$ occurs at or near a Lifshitz transition when the Fermi level passes through a van Hove singularity. Finally, we perform order parameter analyses using three-band renormalization group calculations. These, combined with the unexpectedly low in-plane critical field, open the possibility that the highly strained $T_c$=3.4~K Sr$_2$RuO$_4$ has an even- rather than an odd-parity order parameter. Potential implications such as a transition at nonzero strain between odd- and even-parity order parameters are discussed.

Magnetic and crystallographic properties of the mineral langite Cu$_4$(OH)$_6$SO$_4\cdot 2$H$_2$O are reported. Its layered crystal structure features a peculiar spatial arrangement of spin-$\frac12$ Cu$^{2+}$ ions that arises from a combination of corner- and edge-sharing chains. Experimentally, langite orders antiferromagnetically at $T_N\simeq 5.7$ K as revealed by magnetization and specific heat measurements. Despite this very low energy scale of the magnetic transition, langite features significantly stronger couplings on the order of 50-70 K. Half of the Cu$^{2+}$ spins are weakly coupled and saturate around 12T, where the magnetization reaches 0.5$\mu_B$/Cu. These findings are rationalized by density-functional band-structure calculations suggesting a complex interplay of frustrated exchange couplings in the magnetic planes. A simplified model of coupled magnetic sublattices explains the experimental features qualitatively. To start from reliable structural data, the crystal structure of langite in the 100-280 K temperature range has been determined by single-crystal x-ray diffraction, and the hydrogen positions were refined computationally.