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We explore, through a combination of x-ray diffraction and elastoresistivity measurements, the effect of disorder on the strain-tuned charge density wave and associated multicriticality in Pd$_x$ErTe$_3$ (x = 0, 0.01, 0.02 and 0.026). We focus particularly on the behavior near the strain-tuned bicritical point that occurs in pristine ErTe$_3$ (x=0). Our study reveals that while Pd intercalation somewhat broadens the signatures of the CDW phase transitions, the line of first-order transitions at which the CDW reorients as a function of applied strain persists in the presence of disorder and still seemingly terminates at a critical point. The critical point occurs at a lower temperature and a lower strain compared to pristine ErTe$_3$. Similarly, the nematic elastoresistance of Pd$_x$ErTe$_3$, though suppressed in magnitude and broadened relative to that of ErTe$_3$, has a markedly more symmetric response around the critical point. These observations point to disorder driving a reduction in the system's electronic orthorhombicity even while the material remains irrevocably orthorhombic due to the presence of a glide plane in the crystal structure. Disorder, it would appear, reinforces the emergence of a "pseudo-tetragonal" electronic response in this fundamentally orthorhombic material.

In the electromagnetic multipole expansion, magnetic octupoles are the subsequent order of magnetic multipoles allowed in centrosymmetric systems, following the more commonly observed magnetic dipoles. As order parameters in condensed matter systems, magnetic octupoles have been experimentally elusive. In particular, the lack of simple external fields that directly couple to them makes their experimental detection challenging. Here, we demonstrate a methodology for probing the magnetic octupole susceptibility using a product of magnetic field $H_i$ and shear strain $\epsilon_{jk}$ to couple to the octupolar fluctuations, while using an adiabatic elastocaloric effect to probe the response to this composite effective field. We observe a Curie-Weiss behavior in the obtained octupolar susceptibility of \ce{PrV2Al20} up to temperatures approximately forty times the putative octupole ordering temperature. Our results demonstrate the presence of magnetic octupole fluctuations in the particular material system, and more broadly highlight how anisotropic strain can be combined with magnetic fields to formulate a versatile probe to observe otherwise elusive emergent `hidden' electronic orders., Comment: 7 pages, 3 figures

$GdTe_{3}$ is a layered antiferromagnet which has attracted attention due to its exceptionally high mobility, distinctive unidirectional incommensurate charge density wave (CDW), superconductivity under pressure, and a cascade of magnetic transitions between 7 and 12 K, with as yet unknown order parameters. Here, we use spin-polarized scanning tunneling microscopy to directly image the charge and magnetic orders in $GdTe_{3}$. Below 7 K, we find a striped antiferromagnetic phase with twice the periodicity of the Gd lattice and perpendicular to the CDW. As we heat the sample, we discover a spin density wave with the same periodicity as the CDW between 7 and 12 K; the viability of this phase is supported by our Landau free energy model. Our work reveals the order parameters of the magnetic phases in $GdTe_{3}$ and shows how the interplay between charge and spin can generate a cascade of magnetic orders., Comment: 46 pgs.; 4 main figures, 20 supplementary figures

Symmetry plays a key role in determining the physical properties of materials. By Neumann's principle, the properties of a material are invariant under the symmetry operations of the space group to which the material belongs. Continuous phase transitions are associated with a spontaneous reduction in symmetry. (For example, the onset of ferromagnetism spontaneously breaks time reversal symmetry.) Much less common are examples where proximity to a continuous phase transition leads to an increase in symmetry. Here, we find an emergent tetragonal symmetry close to an apparent charge density wave (CDW) bicritical point in a fundamentally orthorhombic material, ErTe$_3$, for which the CDW phase transitions are tuned via anisotropic strain. The underlying structure of the material remains orthorhombic for all applied strains, including at the bicritical point, due to a glide plane symmetry in the crystal structure. Nevertheless, the observation of a divergence in the anisotropy of the in-plane elastoresistivity reveals an emergent electronic tetragonality near the bicritical point.

We thank G.P. Mikitik and Yu.V. Sharlai for contributing this note and the cordial exchange about it. First and foremost, we note that the aim of our paper is to report a methodology to diagnose topological (semi)metals using magnetic quantum oscillations. Thus far, such diagnosis has been based on the phase offset of quantum oscillations, which is extracted from a "Landau fan plot". A thorough analysis of the Onsager-Lifshitz-Roth quantization rules has shown that the famous $\pi$-phase shift can equally well arise from orbital- or spin magnetic moments in topologically trivial systems with strong spin-orbit coupling or small effective masses. Therefore, the "Landau fan plot" does not by itself constitute a proof of a topologically nontrivial Fermi surface. In the paper at hand, we report an improved analysis method that exploits the strong energy-dependence of the effective mass in linearly dispersing bands. This leads to a characteristic temperature dependence of the oscillation frequency which is a strong indicator of nontrivial topology, even for multi-band metals with complex Fermi surfaces. Three materials, Cd$_3$As$_2$, Bi$_2$O$_2$Se and LaRhIn$_5$ served as test cases for this method. Linear band dispersions were detected for Cd$_3$As$_2$, as well as the $F$ $\approx$ 7 T pocket in LaRhIn$_5$., Comment: Response to Matter arising for Nature Communications 12, 6213 (2021)

The adiabatic elastocaloric effect measures the temperature change of given systems with strain and probes the entropic landscape in the temperature-strain space. In this study we demonstrate that the DC bias strain-dependence of AC elastocaloric effect can be used to decompose the latter into contributions from symmetric (rotation-symmetry-preserving) and antisymmetric (rotation-symmetry-breaking) strains, using a tetragonal f-electron system DyB2C2--whose antiferroquadrupolar order locally breaks four-fold rotational site symmetries while globally remaining tetragonal--as a showcase example. We capture the strain evolution of the quadrupolar and magnetic phase transitions in the system using both singularities in the elastocaloric coefficient and its jump at the transitions, and the latter we show follows a modified Ehrenfest relation. We find that antisymmetric strain couples to the underlying order parameter in a bi-quadratic manner in the antiferroquadrupolar (AFQ) phase but in a linear-quadratic manner in the canted antiferromagnetic (CAFM) phase; the contrast is attributed to a preserved (broken) tetragonal symmetry in the AFQ (CAFM) phase, respectively. The broken tetragonal symmetry in the CAFM phase is further supported by elastocaloric strain-hysteresis and observation of two sets of domains with mutually perpendicular principal axes in optical birefringence. Additionally, when the quadrupolar moments are ordered in a staggered fashion, we uncover an elastocaloric response that reflects a quadratic increase of entropy with antisymmetric strain, analogous to the role magnetic field plays for Ising antiferromagnets by promoting pseudospin flips. Our results show that AC elastocaloric effect is a compact and incisive thermodynamic probe into the coupling between electronic degrees of freedom and strain, which can potentially be applied to broader classes of quantum materials., Comment: 10 pages, 7 figures

Superconductor/metal interfaces are usually fabricated in heterostructures that join these dissimilar materials. A conceptually different approach has recently exploited the strain sensitivity of heavy-fermion superconductors, selectively transforming regions of the crystal into the metallic state by strain gradients. The strain is generated by differential thermal contraction between the sample and the substrate. Here, we present an improved finite-element model that reliably predicts the superconducting transition temperature in CeIrIn$_5$ even in complex structures. Different substrates are employed to tailor the strain field into the desired shapes. Using this approach, both highly complex and strained as well as strain-free microstructures are fabricated to validate the model. This enables full control over the microscopic strain fields, and forms the basis for more advanced structuring of superconductors as in Josephson junctions., Comment: 8 pages, 4 figures

Intense work studying the ballistic regime of electron transport in two dimensional systems based on semiconductors and graphene had been thought to have established most of the key experimental facts of the field. In recent years, however, new forms of ballistic transport have become accessible in the quasi-two-dimensional delafossite metals, whose Fermi wavelength is a factor of 100 shorter than those typically studied in the previous work, and whose Fermi surfaces are nearly hexagonal in shape, and therefore strongly faceted. This has some profound consequences for results obtained from the classic ballistic transport experiment of studying bend and Hall resistances in mesoscopic squares fabricated from delafossite single crystals. We observe pronounced anisotropies in bend resistances and even a Hall voltage that is strongly asymmetric in magnetic field. Although some of our observations are non-intuitive at first sight, we show that they can be understood within a non-local Landauer-B\"uttiker analysis tailored to the symmetries of the square/hexagonal geometries of our combined device/Fermi surface system. Signatures of non-local transport can be resolved for squares of linear dimension of nearly 100 $\mu$m, approximately a factor of 15 larger than the bulk mean free path of the crystal from which the device was fabricated., Comment: 23 pages, 9 figures (including supplementary information)

In photoelectron spectroscopy, the measured electron momentum range is intrinsically related to the excitation photon energy. Low photon energies $<10$ eV are commonly encountered in laser-based photoemission and lead to a momentum range that is smaller than the Brillouin zones of most materials. This can become a limiting factor when studying condensed matter with laser-based photoemission. An additional restriction is introduced by widely used hemispherical analyzers that record only electrons photoemitted in a solid angle set by the aperture size at the analyzer entrance. Here, we present an upgrade to increase the effective solid angle that is measured with a hemispherical analyzer. We achieve this by accelerating the photoelectrons towards the analyzer with an electric field that is generated by a bias voltage on the sample. Our experimental geometry is comparable to a parallel plate capacitor and, therefore, we approximate the electric field to be uniform along the photoelectron trajectory. With this assumption, we developed an analytic, parameter-free model that relates the measured angles to the electron momenta in the solid and verify its validity by comparing with experimental results on the charge density wave material TbTe$_3$. By providing a larger field of view in momentum space, our approach using a bias potential considerably expands the flexibility of laser-based photoemission setups., Comment: 11 pages, 7 figures

The quest to improve transparent conductors balances two key goals: increasing electrical conductivity and increasing optical transparency. To improve both simultaneously is hindered by the physical limitation that good metals with high electrical conductivity have large carrier densities that push the plasma edge into the ultra-violet range. Transparent conductors are compromises between electrical conductivity, requiring mobile electrons, and optical transparency based on immobile charges to avoid screening of visible light. Technological solutions reflect this trade-off, achieving the desired transparencies by reducing the conductor thickness or carrier density at the expense of a lower conductance. Here we demonstrate that highly anisotropic crystalline conductors offer an alternative solution, avoiding this compromise by separating the directions of conduction and transmission. Materials with a quasi-two-dimensional electronic structure have a plasma edge well below the range of visible light while maintaining excellent in-plane conductivity. We demonstrate that slabs of the layered oxides Sr$_2$RuO$_4$ and Tl$_2$Ba$_2$CuO$_{6+\delta}$ are optically transparent even at macroscopic thicknesses >2$\mu$m for c-axis polarized light. Underlying this observation is the fabrication of out-of-plane slabs by focused ion beam milling. This work provides a glimpse into future technologies, such as highly polarized and addressable optical screens, that advancements in a-axis thin film growth will enable.

In an idealized infinite crystal, the material properties are constrained by the symmetries of its unit cell. Naturally, the point-group symmetry is broken by the sample shape of any finite crystal, yet this is commonly unobservable in macroscopic metals. To sense the shape-induced symmetry lowering in such metals, long-lived bulk states originating from anisotropic Fermi surfaces are needed. Here we show how strongly facetted Fermi surfaces and long quasiparticle mean free paths present in microstructures of PdCoO2 yield an in-plane resistivity anisotropy that is forbidden by symmetry on an infinite hexagonal lattice. Bar shaped transport devices narrower than the mean free path are carved from single crystals using focused ion beam (FIB) milling, such that the ballistic charge carriers at low temperatures frequently collide with both sidewalls defining a channel. Two symmetry-forbidden transport signatures appear: the in-plane resistivity anisotropy exceeds a factor of 2, and transverse voltages appear in zero magnetic field. We robustly identify the channel direction as the source of symmetry breaking via ballistic Monte- Carlo simulations and numerical solution of the Boltzmann equation.

We report a scanning superconducting quantum interference device (SQUID) microscope in a cryogen-free dilution refrigerator with a base temperature at the sample stage of at least 30 mK. The microscope is rigidly mounted to the mixing chamber plate to optimize thermal anchoring of the sample. The microscope housing fits into the bore of a superconducting vector magnet, and our design accommodates a large number of wires connecting the sample and sensor. Through a combination of vibration isolation in the cryostat and a rigid microscope housing, we achieve relative vibrations between the SQUID and sample that allow us to image with micrometer resolution over a 150 $\mu$m range while the sample stage temperature remains at base temperature. To demonstrate the capabilities of our system, we show images acquired simultaneously of the static magnetic field, magnetic susceptibility, and magnetic fields produced by a current above a superconducting micrometer-scale device.

ErTe$_3$ is studied as a model system to explore thermal transport in a layered charge density wave (CDW) material. We present data from thermal diffusivity, resistivity, and specific heat measurements: There is a sharp decrease in thermal conductivity both parallel and perpendicular to the primary CDW at the CDW transition temperature. At the same time, the resistivity changes more gradually. Correspondingly, while well above and below $T_c$, a consistent description of the thermal transport applies with essentially independent electron and phonon contributions (estimated using the Wiedemann Franz law), in the critical regime no such description is possible; the observed behavior corresponds to a strongly coupled electron-phonon critical `soup.', Comment: Main text 7 pages and 7 figures, supplementary text 2 pages and 2 figures

In RuCl$_3$, inelastic neutron scattering and Raman spectroscopy reveal a continuum of non-spin-wave excitations that persists to high temperature, suggesting the presence of a spin liquid state on a honeycomb lattice. In the context of the Kitaev model, magnetic fields introduce finite interactions between the elementary excitations, and thus the effects of high magnetic fields - comparable to the spin exchange energy scale - must be explored. Here we report measurements of the magnetotropic coefficient - the second derivative of the free energy with respect to magnetic field orientation - over a wide range of magnetic fields and temperatures. We find that magnetic field and temperature compete to determine the magnetic response in a way that is independent of the large intrinsic exchange interaction energy. This emergent scale-invariant magnetic anisotropy provides evidence for a high degree of exchange frustration that favors the formation of a spin liquid state in RuCl$_3$., Comment: arXiv admin note: substantial text overlap with arXiv:1901.09245. Nature Physics

The phase offset of quantum oscillations is commonly used to experimentally diagnose topologically non-trivial Fermi surfaces. This methodology, however, is inconclusive for spin-orbit-coupled metals where $\pi$-phase-shifts can also arise from non-topological origins. Here, we show that the linear dispersion in topological metals leads to a $T^2$-temperature correction to the oscillation frequency that is absent for parabolic dispersions. We confirm this effect experimentally in the Dirac semi-metal Cd$_3$As$_2$ and the multiband Dirac metal LaRhIn$_5$. Both materials match a tuning-parameter-free theoretical prediction, emphasizing their unified origin. For topologically trivial Bi$_2$O$_2$Se, no frequency shift associated to linear bands is observed as expected. However, the $\pi$-phase shift in Bi$_2$O$_2$Se would lead to a false positive in a Landau-fan plot analysis. Our frequency-focused methodology does not require any input from ab-initio calculations, and hence is promising for identifying correlated topological materials.

In the Ca$_{1-x}$La$_x$FeAs$_2$ (112) family of pnictide superconductors, we have investigated a highly overdoped composition (x = 0.56), prepared by high-pressure, high-temperature synthesis. Magnetic measurements show an antiferromagnetic transition at TN = 120K, well above the one at lower doping (0.15 < x < 0.27). Below the onset of long-range magnetic order at TN, the electrical resistivity is strongly reduced and is dominated by electron-electron interactions, as evident from its temperature dependence. The Seebeck coefficient shows a clear metallic behavior as in narrow band conductors. The temperature dependence of the Hall coefficient and the violation of Kohler's rule agree with the multiband character of the material. No superconductivity was observed down to 1.8 K. The success of the high-pressure synthesis encourages further investigations of the so far only partially explored phase diagram in this family of Iron-based high temperature superconductors.

Transport of electrons in a bulk metal is usually well captured by their particle-like aspects, while their wave-like nature is commonly harder to observe. Microstructures can be are fully designed to reveal the quantum phase, for example mesoscopic metal rings resembling interferometers. Here we report a new type of phase coherent oscillation of the out-of-plane magnetoresistance in the layered delafossites PdCoO$_2$ and PtCoO$_2$. The oscillation period is equivalent to that determined by the magnetic flux quantum, $h/e$, threading an area defined by the atomic interlayer separation and the sample width. The phase of the electron wave function in these crystals appears remarkably robust over macroscopic length scales exceeding 10$\mu$m and persisting up to elevated temperatures of $T$>50K. We show that, while the experimental signal cannot be explained in a standard Aharonov-Bohm analysis, it arises due to periodic field-modulation of the out-of-plane hopping. These results demonstrate extraordinary single-particle quantum coherence lengths in the delafossites, and identify a new form of quantum interference in solids.

Geometric electron optics may be implemented in solid state when transport is ballistic on the length scale of a device. Currently, this is realized mainly in 2D materials characterized by circular Fermi surfaces. Here we demonstrate that the nearly perfectly hexagonal Fermi surface of PdCoO2 gives rise to highly directional ballistic transport. We probe this directional ballistic regime in a single crystal of PdCoO2 by use of focused ion beam (FIB) micro-machining, defining crystalline ballistic circuits with features as small as 250nm. The peculiar hexagonal Fermi surface naturally leads to electron self-focusing effects in a magnetic field, well below the geometric limit associated with a circular Fermi surface. This super-geometric focusing can be quantitatively predicted for arbitrary device geometry, based on the hexagonal cyclotron orbits appearing in this material. These results suggest a novel class of ballistic electronic devices exploiting the unique transport characteristics of strongly faceted Fermi surfaces.

In RuCl$_3$, inelastic neutron scattering and Raman spectroscopy reveal a continuum of non-spin-wave excitations that persists to high temperature, suggesting the presence of a spin liquid state on a honeycomb lattice. In the context of the Kitaev model, magnetic fields introduce finite interactions between the elementary excitations, and thus the effects of high magnetic fields - comparable to the spin exchange energy scale - must be explored. Here we report measurements of the magnetotropic coefficient - the second derivative of the free energy with respect to magnetic field orientation - over a wide range of magnetic fields and temperatures. We find that magnetic field and temperature compete to determine the magnetic response in a way that is independent of the large intrinsic exchange interaction energy. This emergent scale-invariant magnetic anisotropy provides evidence for a high degree of exchange frustration that favors the formation of a spin liquid state in RuCl$_3$., Comment: superseded by arXiv:2005.04228

The Ce(Co,Rh,Ir)In$_5$ family of ``Ce-115'' materials hosts an abundance of correlated electron behavior, including heavy-fermion physics, magnetism, superconductivity and nematicity. The complicated behavior of these entangled phenomena leads to a variety of exotic physical properties, which, despite the seemingly simple crystal structure of these compounds, remain poorly understood. It is generally accepted that the interplay between the itinerant and local character of Ce-$4f$ electrons is the key to their exotic behavior. Here, we report theoretical evidence that the Ce-115 materials are also topological semi-metals, with Dirac fermions around well-separated nodes. Dirac nodes in each compound are present on the $\Gamma-Z$ plane close to the Fermi level. As the Dirac bands are derived from In-orbitals, they occur in all family members irrespective of the transition metal (Co,Rh,Ir). We present the expected Fermi-arc surface state patterns and show the close proximity of a topological Lifshitz transition, which possibly explains the high field physics of Ce-115 materials. Experimentally, we highlight the surprising similarity of Ce(Co,Rh,Ir)In$_5$ in high magnetic fields, despite the distinctly different states of the Ce-$4f$ electrons. These results raise questions about the role Dirac fermions play in exotic transport behavior, and we propose this class of materials as a prime candidate for unconventional topological superconductivity.

The ability to spatially modulate the electronic properties of solids has led to landmark discoveries in condensed matter physics as well as new electronic applications. Although crystals of strongly correlated metals exhibit a diverse set of electronic ground states, few approaches to spatially modulating their properties exist. Here we demonstrate spatial control over the superconducting state in mesoscale samples of the canonical heavy-fermion superconductor CeIrIn5. We use a focused ion beam (FIB) to pattern crystals on the microscale, which tailors the strain induced by differential thermal contraction into specific areas of the device. The resulting non-uniform strain fields induce complex patterns of superconductivity due to the strong dependence of the transition temperature on the strength and direction of strain. Electrical transport and magnetic imaging of devices with different geometry show that the obtained spatial modulation of superconductivity agrees with predictions based on finite element simulations. These results present a generic approach to manipulating electronic order on micrometer length scales in strongly correlated matter., Comment: 29 pages, 14 figures

Unusual behavior of quantum materials commonly arises from their effective low-dimensional physics, which reflects the underlying anisotropy in the spin and charge degrees of freedom. Torque magnetometry is a highly sensitive technique to directly quantify the anisotropy in quantum materials, such as the layered high-T$_c$ superconductors, anisotropic quantum spin-liquids, and the surface states of topological insulators. Here we introduce the magnetotropic coefficient $k=\partial^2 F/\partial \theta^2$, the second derivative of the free energy F with respect to the angle $\theta$ between the sample and the applied magnetic field, and report a simple and effective method to experimentally detect it. A sub-$\mu$g crystallite is placed at the tip of a commercially available atomic force microscopy cantilever, and we show that $k$ can be quantitatively inferred from a shift in the resonant frequency under magnetic field. While related to the magnetic torque $\tau=\partial F/\partial \theta$, $k$ takes the role of torque susceptibility, and thus provides distinct insights into anisotropic materials akin to the difference between magnetization and magnetic susceptibility. The thermodynamic coefficient $k$ is discontinuous at second-order phase transitions and subject to Ehrenfest relations with the specific heat and magnetic susceptibility. We apply this simple yet quantitative method on the exemplary cases of the Weyl-semimetal NbP and the spin-liquid candidate RuCl$_3$, yet it is broadly applicable in quantum materials research., Comment: 7 pages including 6 figures and methods section

By introducing a superconducting gap in Weyl- or Dirac semi-metals, the superconducting state inherits the non-trivial topology of their electronic structure. As a result, Weyl superconductors are expected to host exotic phenomena such as non-zero-momentum pairing due to their chiral node structure, or zero- energy Majorana modes at the surface. These are of fundamental interest to improve our understanding of correlated topological systems, and moreover practical applications in phase coherent devices and quantum applications have been proposed. Proximity-induced superconductivity promises to allow such experiments on non-superconducting Weyl semi-metals. Here we show a new route to reliably fabricating superconducting microstructures from the non-superconducting Weyl semi-metal NbAs under ion irradiation. The significant difference in the surface binding energy of Nb and As leads to a natural enrichment of Nb at the surface during ion milling, forming a superconducting surface layer (Tc~3.5K). Being formed from the target crystal itself, the ideal contact between the superconductor and the bulk may enable an effective gapping of the Weyl nodes in the bulk due to the proximity effect. Simple ion irradiation may thus serve as a powerful tool to fabricating topological quantum devices from mono-arsenides, even on an industrial scale., Comment: accepted by Science Advances