arXiv subjects

Leslie M. Schoop

Publications and source records attributed to Leslie M. Schoop.

At least 37 records · Page 2Linked to original sources

arXiv2025

Clustering-Enhanced Time- and Angle-Resolved Photoemission Study of LaTe$_3$: Absence of a Photoinduced Secondary CDW in the Electronic Structure

Optical control offers a compelling route for tailoring material properties on an ultrafast time scale. Ordered states such as charge density waves (CDWs) can be transiently melted by an ultrafast light excitation. This is also the case for the rare-earth tritelluride LaTe$_3$, a prototypical CDW compound. For this material it has recently been reported that the suppression of the primary CDW allows the transient formation of a second CDW, whose wave vector is orthogonal to the primary one. This creates the intriguing scenario where light enables switching between two distinct ordered phases of the material. While the second CDW has so far been observed by structural techniques, it remains an open question how the interplay of the two CDW phases is reflected in the material's electronic structure. We investigate this via time- and angle-resolved photoemission measurements of LaTe$_3$. The complex Fermi contour is probed using a FeSuMa analyzer, which records the photoemission intensity of the entire Fermi contour at once. The dynamics revealed by the FeSuMa analyzer are complemented by measurements using a conventional hemispherical electron analyzer. We combine conventional data analysis with $k$-means clustering, an unsupervised machine learning technique, demonstrating its strong potential for disentangling large datasets. While we do not find any features that cannot be explained by the melting and re-establishment of the primary CDW, distinct dynamics and coherent oscillations are observed in the different branches of the Fermi contour.

cond-mat.str-el↗

arXiv2025

Successive orthorhombic distortions in kagome metals by molecular orbital formation

The kagome lattice, with its inherent frustration, hosts a plethora of exotic phenomena, including the emergence of $3\mathbf{q}$ charge density wave order. The high rotational symmetry, required to realize such an unconventional charge order, is broken in many kagome materials by orthorhombic distortions at high temperature, the origin of which is much less discussed despite their ubiquity. In this study, synchrotron X-ray diffraction reveals a structural phase transition from a parent hexagonal phase to an orthorhombic ground state, mediated by a critical regime of diffuse scattering in the prototypical kagome metals $R$Ru$_3$Si$_2$ ($R$=rare-earth). Structural analysis uncovers an interlayer dimerization of kagome atoms in the low-temperature phase. Accordingly, a dimer model with one-dimensional disorder on kagome layers successfully reproduces the diffuse scattering. The observations point to molecular orbital formation between kagome $4d_{z^2}$ orbitals as the driving force behind the transition, consistent with \textit{ab initio} calculations. A framework based on electronegativity and atomic radii is proposed to evaluate the stability of the hexagonal phase in kagome metals, guiding the design of highly symmetric materials.

cond-mat.str-el↗

arXiv2025

Chemical enhancement of superconductivity in LaRu3Si2 with mode-selective coupling between kagome phonons and flat bands

In kagome metals, flat electronic bands induced by frustrated hopping are a platform for strong electron correlations. In particular, a selective coupling of flat band states to certain kagome phonon modes is proposed as a universal origin of superconductivity in this material class. Here, we investigate the superconductivity in the kagome system LaRu$_3$(Si$_{1-x}$Ge$_x$)$_2$ by chemical pressure tuning while preserving the Ru-$4d$ states that constitute the kagome flat bands. We observe a sizable enhancement in the density of states up to $x = 0.07$, as determined by the specific heat, with a concomitant increase in the superconducting transition temperature $T_\mathrm{c}$. Ge-dopants induce a uniaxial lattice expansion along the $c$-axis. Our first-principles calculations suggest that this mitigates the detrimental effect of hybridization between kagome layers and reduces the dispersion of the Ru-$4d_{x^2-y^2}$ flat band. The calculated chemical potential moves closer to the maximum in the energy-dependent density of states. Our result is consistent with a theoretical prediction of tunable flat band superconductivity in LaRu$_3$Si$_2$ by mode-selective coupling between specific kagome phonons and the Ru-$d_{x^2-y^2}$ orbitals.

cond-mat.supr-con↗

arXiv2025

One-dimensional conduction channels in the correlated Mott NiS2 arising from obstructed Wannier charges

NiS2, a compound characterized by its pyrite structure, uniquely bridges the realms of strong correlation physics and topology. While bulk NiS2 is known to be a Mott or charge-transfer insulator, its surface displays anomalous metallic behavior and finite conductivity. Using high-resolution neutron scattering data and symmetry analysis, we propose a refined description of NiS2's magnetic phases by introducing a novel model for its ground state. Combined with high-resolution scanning tunneling microscopy and spectroscopy (STM/STS), we unveil the presence of edge states in both Ni- and S-terminated surfaces, which exhibit remarkable resilience to external magnetic fields. Although both types of edge states exhibit similar properties, only the edge states at the Ni termination populate the vicinity of the Fermi level and, therefore contribute to the surface conductivity. Utilizing ab initio methods combined with a topological quantum chemistry analysis, we attribute these edge states to obstructed atomic charges originating from bulk topology. Overall, this work not only deepens our understanding of NiS2 but also lays a robust experimental and theoretical foundation for further exploration of the interplay between one-dimensional step-edge states and the Wannier obstruction in correlated materials.

cond-mat.str-el↗

arXiv2025

A Recipe for Flat Bands in Pyrochlore Materials: A Chemist's Perspective

Materials in which atoms are arranged in a pyrochlore lattice have found renewed interest, as, at least theoretically, orbitals on those lattices can form flat bands. However, real materials often do not behave according to theoretical models, which is why there has been a dearth of pyrochlore materials exhibiting flat band physics. Here we examine the conditions under which ideal 'pyrochlore bands' can exist in real materials and how to have those close to the Fermi level. We find that the simple model used in the literature does not apply to the bands at the Fermi level in real pyrochlore materials. However, surprisingly, certain oxide compounds which have oxygen orbitals inside the pyrochlore tetrahedra do exhibit near-ideal pyrochlore bands near the Fermi level. We explain this observation by a generalized tight-binding model including the oxygen orbitals. We further classify all known pyrochlore materials based on their crystal structure, band structure, and chemical characteristics and propose materials to study in future experiments.

cond-mat.mtrl-sci↗

arXiv2025

Unconventional Superconducting Phase Diagram of Monolayer WTe2

The existence of a quantum critical point (QCP) and fluctuations around it are believed to be important for understanding the phase diagram in unconventional superconductors such as cuprates, iron pnictides, and heavy fermion superconductors. However, the QCP is usually buried deep within the superconducting dome and is difficult to investigate. The connection between quantum critical fluctuations and superconductivity remains an outstanding problem in condensed matter. Here combining both electrical transport and Nernst experiments, we explicitly demonstrate the onset of superconductivity at an unconventional QCP in gate-tuned monolayer tungsten ditelluride (WTe2), with features incompatible with the conventional Bardeen-Cooper-Schrieffer (BCS) scenario. The results lead to a novel superconducting phase diagram that is distinguished from other known superconductors. Two distinct gate-tuned quantum phase transitions are observed at the ends of the superconducting dome. We find that quantum fluctuations around the QCP of the underdoped regime are essential for understanding how the monolayer superconductivity is established. The unconventional phase diagram we report here illustrates a previously unknown relation between superconductivity and QCP.

cond-mat.mes-hall↗

arXiv2024

A New Moiré Platform Based on M-Point Twisting

We introduce a new class of moiré systems and materials based on monolayers with triangular lattices and low-energy states at the M points of the Brillouin zone. These M-point moiré materials are fundamentally distinct from those derived from $Γ$- or K-point monolayers, featuring three time-reversal-preserving valleys related by three-fold rotational symmetry. We propose twisted bilayers of experimentally exfoliable 1T-SnSe$_2$ and 1T-ZrS$_2$ as realizations of this new class. Using extensive ab initio simulations, we develop quantitative continuum models and analytically show that the corresponding M-point moiré Hamiltonians exhibit emergent momentum-space non-symmorphic symmetries and a kagome plane-wave lattice in momentum space. This represents the first experimentally viable realization of a projective representation of crystalline space groups in a non-magnetic system. With interactions, these materials represent six-flavor Hubbard simulators with Mott physics, as can be seen by their flat Wilson loops. Furthermore, the presence of a non-symmorphic momentum-space in-plane mirror symmetry makes some of the M-point moiré Hamiltonians quasi-one-dimensional in each valley, suggesting the possibility of realizing Luttinger liquid physics. We predict the twist angles at which a series of (conduction) flat bands appear, provide a faithful continuum Hamiltonian, analyze its topology and charge density and briefly discuss several aspects of the physics of this new platform.

cond-mat.str-el↗

arXiv2024

Uncovering the Hidden Ferroaxial Density Wave as the Origin of the Axial Higgs Mode in RTe$_3$

The recent discovery of an axial amplitude (Higgs) mode in the long-studied charge density wave (CDW) systems GdTe$_3$ and LaTe$_3$ suggests a heretofore unidentified hidden order. A theoretical study proposed that the axial Higgs results from a hidden ferroaxial component of the CDW, which could arise from non-trivial orbital texture. Here, we report extensive experimental studies on ErTe$_3$ and HoTe$_3$ that possess a high-temperature CDW similar to other RTe$_3$ (R = rare earth), along with an additional low-temperature CDW with an orthogonal ordering vector. Combining Raman spectroscopy with large-angle convergent beam electron diffraction (LACBED), rotational anisotropy second-harmonic generation (RA-SHG), and muon-spin relaxation ($μ$SR), we provide unambiguous evidence that the high-temperature CDW breaks translation, rotation, and all vertical and diagonal mirror symmetries, but not time-reversal or inversion. In contrast, the low-temperature CDW only additionally breaks translation symmetry. Simultaneously, Raman scattering shows the high-temperature CDW produces an axial Higgs mode while the low-temperature mode is scalar. The weak monoclinic structural distortion and clear axial response in Raman and SHG are consistent with a ferroaxial phase in RTe$_3$ driven by coupled orbital and charge orders. Thus, our study provides a new standard for uncovering unconventional orders and confirms the power of Higgs modes to reveal them.

cond-mat.str-el↗

arXiv2024

Charge-Neutral Electronic Excitations in Quantum Insulators

Experiments on quantum materials have uncovered many interesting quantum phases ranging from superconductivity to a variety of topological quantum matter including the recently observed fractional quantum anomalous Hall insulators. The findings have come in parallel with the development of approaches to probe the rich excitations inherent in such systems. In contrast to observing electrically charged excitations, the detection of charge-neutral electronic excitations in condensed matter remains difficult, though they are essential to understanding a large class of strongly correlated phases. Low-energy neutral excitations are especially important in characterizing unconventional phases featuring electron fractionalization, such as quantum spin liquids, spin ices, and insulators with neutral Fermi surfaces. In this perspective, we discuss searches for neutral fermionic, bosonic, or anyonic excitations in unconventional insulators, highlighting theoretical and experimental progress in probing excitonic insulators, new quantum spin liquid candidates and emergent correlated insulators based on two-dimensional layered crystals and moiré materials. We outline the promises and challenges in probing and utilizing quantum insulators, and discuss exciting new opportunities for future advancements offered by ideas rooted in next-generation quantum materials, devices, and experimental schemes.

cond-mat.str-el↗

arXiv2024

Bonding Interactions Can Drive Topological Phase Transitions in a Zintl Antiferromagnetic Insulator

While $\sim$30% of materials are reported to be topological, topological insulators are rare. Magnetic topological insulators (MTI) are even harder to find. Identifying crystallographic features that can host the coexistence of a topological insulating phase with magnetic order is vital for finding intrinsic MTI materials. Thus far, most materials that are investigated for the determination of an MTI are some combination of known topological insulators with a magnetic ion such as MnBi$_2$Te$_4$. Motivated by the recent success of EuIn$_{2}$As$_{2}$, we investigate the role of chemical pressure on topologically trivial insulator, Eu$_5$In$_2$Sb$_6$ via Ga substitution. Eu$_5$Ga$_2$Sb$_6$ is predicted to be topological but is synthetically difficult to stabilize. We look into the intermediate compositions between Eu$_5$In$_2$Sb$_6$ and Eu$_5$Ga$_2$Sb$_6$ through theoretical works to explore a topological phase transition and band inversion mechanism. We attribute the band inversion mechanism to changes in Eu-Sb hybridization as Ga is substituted for In due to chemical pressure. We also synthesize Eu$_{5}$In$_{4/3}$Ga$_{2/3}$Sb$_{6}$, the highest Ga concentration in Eu$_{5}$In$_{2-x}$Ga$_{x}$Sb$_{6}$, and report the thermodynamic, magnetic, transport, and Hall properties. Overall, our work paints a picture of a possible MTI via band engineering and explains why Eu-based Zintl compounds are suitable for the co-existence of magnetism and topology.

cond-mat.mtrl-sci↗

arXiv2024

Atomic-Scale Visualization of a Cascade of Magnetic Orders in the Layered Antiferromagnet $GdTe_{3}$

$GdTe_{3}$ 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.

cond-mat.str-el↗

arXiv2023

Materials Expert-Artificial Intelligence for Materials Discovery

The advent of material databases provides an unprecedented opportunity to uncover predictive descriptors for emergent material properties from vast data space. However, common reliance on high-throughput ab initio data necessarily inherits limitations of such data: mismatch with experiments. On the other hand, experimental decisions are often guided by an expert's intuition honed from experiences that are rarely articulated. We propose using machine learning to "bottle" such operational intuition into quantifiable descriptors using expertly curated measurement-based data. We introduce "Materials Expert-Artificial Intelligence" (ME-AI) to encapsulate and articulate this human intuition. As a first step towards such a program, we focus on the topological semimetal (TSM) among square-net materials as the property inspired by the expert-identified descriptor based on structural information: the tolerance factor. We start by curating a dataset encompassing 12 primary features of 879 square-net materials, using experimental data whenever possible. We then use Dirichlet-based Gaussian process regression using a specialized kernel to reveal composite descriptors for square-net topological semimetals. The ME-AI learned descriptors independently reproduce expert intuition and expand upon it. Specifically, new descriptors point to hypervalency as a critical chemical feature predicting TSM within square-net compounds. Our success with a carefully defined problem points to the "machine bottling human insight" approach as promising for machine learning-aided material discovery.

cond-mat.mtrl-sci↗

arXiv2023

Strong and Fragile Topological Dirac Semimetals with Higher-Order Fermi Arcs

Dirac and Weyl semimetals both exhibit arc-like surface states. However, whereas the surface Fermi arcs in Weyl semimetals are topological consequences of the Weyl points themselves, the surface Fermi arcs in Dirac semimetals are not directly related to the bulk Dirac points, raising the question of whether there exists a topological bulk-boundary correspondence for Dirac semimetals. In this work, we discover that strong and fragile topological Dirac semimetals exhibit 1D higher-order hinge Fermi arcs (HOFAs) as universal, direct consequences of their bulk 3D Dirac points. To predict HOFAs coexisting with topological surface states in solid-state Dirac semimetals, we introduce and layer a spinful model of an $s-d$-hybridized quadrupole insulator (QI). We develop a rigorous nested Jackiw-Rebbi formulation of QIs and HOFA states. Employing $ab\ initio$ calculations, we demonstrate HOFAs in both the room- ($α$) and intermediate-temperature ($α''$) phases of Cd$_{3}$As$_2$, KMgBi, and rutile-structure ($β'$-) PtO$_2$.

cond-mat.mes-hall↗

arXiv2023

A Platform for Far-Infrared Spectroscopy of Quantum Materials at Millikelvin Temperatures

Optical spectroscopy of quantum materials at ultralow temperatures is rarely explored, yet it may provide critical characterizations of quantum phases not possible using other approaches. We describe the development of a novel experimental platform that enables optical spectroscopic studies, together with standard electronic transport, of materials at millikelvin temperatures inside a dilution refrigerator. The instrument is capable of measuring both bulk crystals and micron-sized two-dimensional van der Waals materials and devices. We demonstrate the performance by implementing photocurrent-based Fourier transform infrared spectroscopy on a monolayer WTe$_2$ device and a multilayer 1T-TaS$_2$ crystal, with a spectral range available from the near-infrared to the terahertz regime and in magnetic fields up to 5 T. In the far-infrared regime, we achieve spectroscopic measurements at a base temperature as low as ~ 43 mK and a sample electron temperature of ~ 450 mK. Possible experiments and potential future upgrades of this versatile instrumental platform are envisioned.

cond-mat.mes-hall↗

arXiv2023

Pb$_9$Cu(PO4)$_6$(OH)$_2$: Phonon bands, Localized Flat Band Magnetism, Models, and Chemical Analysis

In a series of recent reports, doped lead apatite (LK-99) has been proposed as a candidate ambient temperature and pressure superconductor. However, from both an experimental and theoretical perspective, these claims are largely unsubstantiated. To this end, our synthesis and subsequent analysis of an LK-99 sample reveals a multiphase material that does not exhibit high-temperature superconductivity. We study the structure of this phase with single-crystal X-ray diffraction (SXRD) and find a structure consistent with doped $\text{Pb}_{10}(\text{PO}_4)_6(\text{OH})_2$. However, the material is transparent which rules out a superconducting nature. From ab initio defect formation energy calculations, we find that the material likely hosts $\text{OH}^-$ anions, rather than divalent $\text{O}^{2-}$ anions, within the hexagonal channels and that Cu substitution is highly thermodynamically disfavored. Phonon spectra on the equilibrium structures reveal numerous unstable phonon modes. Together, these calculations suggest it is doubtful that Cu enters the structure in meaningful concentrations, despite initial attempts to model LK-99 in this way. However for the sake of completeness, we perform ab initio calculations of the topology, quantum geometry, and Wannier function localization in the Cu-dominated flat bands of four separate doped structures. In all cases, we find they are atomically localized by irreps, Wilson loops, and the Fubini-Study metric. It is unlikely that such bands can support strong superfluidity, and instead are susceptible to ferromagnetism (or out-of-plane antiferromagnetism) at low temperatures, which we find in ab initio studies. In sum, $\text{Pb}_{9}\text{Cu}(\text{PO}_4)_6(\text{OH})_2$ could more likely be a magnet, rather than an ambient temperature and pressure superconductor.

cond-mat.supr-con↗

arXiv2023

Evidence for Two Dimensional Anisotropic Luttinger Liquids at Millikelvin Temperatures

While Landau's Fermi liquid theory provides the standard description for two- and three-dimensional (2D/3D) conductors, the physics of interacting one-dimensional (1D) conductors is governed by the distinct Luttinger liquid (LL) theory. Can a LL-like state, in which electronic excitations are fractionalized modes, emerge in a 2D system as a stable zero-temperature phase? This long-standing question, first brought up by Anderson decades ago, is crucial in the study of non-Fermi liquids but remains unsettled. A recent experiment identified a moiré superlattice of twisted bilayer tungsten ditelluride (tWTe_2) with a small interlayer twist angle as a 2D host of the LL physics at temperatures of a few kelvins. Here we report experimental evidence for a 2D anisotropic LL state in a substantially reduced temperature regime, down to at least 50 mK, spontaneously formed in a tWTe_2 system with a twist angle of ~ 3 degree. While the system is metallic-like and nearly isotropic above 2 K, a dramatically enhanced electronic anisotropy develops in the millikelvin regime, featuring distinct transport behaviors along two orthogonal in-plane directions. In the strongly anisotropic phase, we observe transport characteristics of a 2D LL phase, i.e., the universal power law scaling behaviors in across-wire conductance and a zero-bias dip in the differential resistance along the wire direction. Our results represent a step forward in the search for stable LL physics beyond 1D and related unconventional quantum matter.

cond-mat.mes-hall↗

arXiv2023

Eavesdropping on competing condensates by the edge supercurrent in a Weyl superconductor

In a topological insulator the metallic surface states are easily distinguished from the insulating bulk states (FuKane07). By contrast, in a topological superconductor (FuKane08,Qi,FuBerg,Oppen), much less is known about the relationship between an edge supercurrent and the bulk pair condensate. Can we force their pairing symmetries to be incompatible? In the superconducting state of the Weyl semimetal MoTe$_2$, an edge supercurrent is observed as oscillations in the current-voltage (\emph{I-V}) curves induced by fluxoid quantization (Wang). We have found that the $s$-wave pairing potential of supercurrent injected from niobium contacts is incompatible with the intrinsic pair condensate in MoTe$_2$. The incompatibility leads to strong stochasticity in the switching current $I_c$ as well as other anomalous properties such as an unusual antihysteretic behavior of the ``wrong'' sign. Under supercurrent injection, the fluxoid-induced edge oscillations survive to much higher magnetic fields \emph{H}. Interestingly, the oscillations are either very noisy or noise-free depending on the pair potential that ends up dictating the edge pairing. Using the phase noise as a sensitive probe that eavesdrops on the competiting bulk states, we uncover an underlying blockade mechanism whereby the intrinsic condensate can pre-emptively block proximitization by the Nb pair potential depending on the history.

cond-mat.supr-con↗

arXiv2023

Unconventional Superconducting Quantum Criticality in Monolayer WTe2

The superconductor to insulator or metal transition in two dimensions (2D) provides a valuable platform for studying continuous quantum phase transitions (QPTs) and critical phenomena. Distinct theoretical models, including both fermionic and bosonic localization scenarios, have been developed, but many questions remain unsettled despite decades of research. Extending Nernst experiments down to millikelvin temperatures, we uncover anomalous quantum fluctuations and identify an unconventional superconducting quantum critical point (QCP) in a gate-tuned excitonic quantum spin Hall insulator (QSHI), the monolayer tungsten ditelluride (WTe2). The observed vortex Nernst effect reveals singular superconducting fluctuations in the resistive normal state induced by magnetic fields or temperature, even well above the transition. Near the doping-induced QCP, the Nernst signal driven by quantum fluctuations is exceptionally large in the millikelvin regime, with a coefficient of ~ 4,100 uV/KT at zero magnetic field, an indication of the proliferation of vortices. Surprisingly, the Nernst signal abruptly disappears when the doping falls below the critical value, in striking conflict with conventional expectations. This series of phenomena, which have no prior analogue, call for careful examinations of the mechanism of the QCP, including the possibility of a continuous QPT between two distinct ordered phases in the monolayer. Our experiments open a new avenue for studying unconventional QPTs and quantum critical matter.

cond-mat.mes-hall↗