arXiv subjects

Leslie M. Schoop

Publications and source records attributed to Leslie M. Schoop.

At least 55 records · Page 3Linked to original sources

arXiv2023

Ultrafast Dynamics of the Topological Semimetal GdSb$_{x}$Te$_{2-x-δ}$ In the Presence and Absence of a Charge Density Wave

Time-resolved dynamics in charge-density-wave materials have revealed interesting out-of-equilibrium electronic responses. However these are typically only performed in a single material possessing a CDW. As such, it is challenging to separate subtle effects originating from the CDW. Here, we report on the ultrafast dynamics of the GdSb$_{x}$Te$_{2-x-δ}$ series of materials where E$_{F}$ can be tuned, resulting in a change from an undistorted tetraganal phase to a CDW with a wavevector that depends on $x$. Using mid-infrared, near-infrared, and visible excitation, we find the dynamics are sensitive to both E$_{F}$ and the presence of the CDW. Specifically, as the Sb content of the compounds increases, transient spectral features shift to higher probe energies. In addition, we observe an enhanced lifetime and change in the sign of the transient signal upon removing the CDW with high Sb concentrations. Finally, we reveal fluence- and temperature-dependent photo-induced responses of the differential reflectivity, which provide evidence of transient charge density wave suppression in related telluride materials. Taken together our results provide a blueprint for future ultrafast studies of CDW systems.

cond-mat.mtrl-sci↗

arXiv2023

Charge density wave-templated spin cycloid in topological semimetal $NdSb_{x}Te_{2-x-δ}$

Magnetic topological semimetals present open questions regarding the interplay of crystal symmetry, magnetism, band topology, and electron correlations. $LnSb_{x}Te_{2-x-δ}$ (Ln= lanthanide) is a family of square-net-derived topological semimetals that allows compositional control of band filling, and access to different topological states via an evolving charge density wave (CDW) distortion. Previously studied Gd and Ce members containing a CDW have shown complex magnetic phase diagrams, which implied that spins localized on Ln interact with the CDW, but to this date, no magnetic structures have been solved within the CDW regime of this family of compounds. Here, we report on the interplay of the CDW with magnetism in $NdSb_{x}Te_{2-x-δ}$, by comparing the undistorted square net member $NdSb_{0.94}Te_{0.92}$ with the CDW-distorted phase $NdSb_{0.48}Te_{1.37}$, via single-crystal x-ray diffraction, magnetometry, heat capacity, and neutron powder diffraction. $NdSb_{0.94}Te_{0.92}$ is a collinear antiferromagnet with $T_N$ $\sim$ 2.7 K, where spins align antiparallel to each other, but parallel to the square net of the nuclear structure. $NdSb_{0.48}Te_{1.37}$ exhibits a nearly five-fold modulated CDW ($q_{CDW}=0.18b^*$), isostructural to other $LnSb_{x}Te_{2-x-δ}$ at similar x. $NdSb_{0.48}Te_{1.37}$ displays more complex magnetism with $T_N = 2.3 K$, additional metamagnetic transitions, and an elliptical cycloid magnetic structure with $q_{mag}=-0.41b^*$.The magnitudes of $q_{CDW}$ and $q_{mag}$ exhibit a integer relationship, $1+2q_{mag}=q_{CDW}$, implying a coupling between the CDW and magnetic structure. Given that the CDW is localized within the nonmagnetic distorted square net, we propose that conduction electrons "template" the spin modulation via the Ruderman-Kittel-Kasuya-Yosida interaction.

cond-mat.mtrl-sci↗

arXiv2022

Atomically Sharp Internal Interface in a Chiral Weyl Semimetal Nanowire

Internal interfaces in Weyl semimetals (WSMs) are predicted to host distinct topological features that are different from the commonly studied external interfaces (crystal-to-vacuum boundaries). However, the lack of atomically sharp and crystallographically oriented internal interfaces in WSMs makes it difficult to experimentally investigate hidden topological states buried inside the material. Here, we study a unique internal interface known as merohedral twin boundary in chemically synthesized single-crystal nanowires (NWs) of CoSi, a chiral WSM of space group P213 (No. 198). High resolution scanning transmission electron microscopy reveals that this internal interface is (001) twin plane and connects two enantiomeric counterparts at an atomically sharp interface with inversion twinning. Ab-initio calculations show localized internal Fermi arcs at the (001) twin boundary that can be clearly distinguished from both external Fermi arcs and bulk states. These merohedrally twinned CoSi NWs provide an ideal material system to probe unexplored topological properties associated with internal interfaces in WSMs.

cond-mat.mtrl-sci↗

arXiv2022

Charge density wave-generated Fermi surfaces in NdTe$_3$

The electronic structure of NdTe$_3$ in the charge density wave phase (CDW) is investigated by angle-resolved photoemission spectroscopy. The combination of high-quality crystals and careful surface preparation reveals subtle and previously unobserved details in the Fermi surface topology, allowing an interpretation of the rich and unexplained quantum oscillations in the rare earth tritellurides RTe$_3$. In particular, several closed Fermi surface elements can be observed that are related to CDW-induced replicas of the original bands, leading to the curious situation in which a CDW does not only remove Fermi surface elements but creates new ones that are observable in transport experiments. Moreover, a large residual Fermi surface is found in the CDW gap, very close to the position of the gapped normal-state Fermi surface. Its area agrees very well with high-frequency quantum oscillations in NdTe$_3$ and its presence is explained by strong electron-phonon coupling combined with the quasi one-dimensional character of the CDW. Finally, we identify the origin of the low-frequency $α$ quantum oscillations ubiquitous for the lighter R elements in the RTe$_3$ family and responsible for the high mobility in these compounds.

cond-mat.str-el↗

arXiv2022

Colossal negative magnetoresistance in the complex charge density wave regime of an antiferromagnetic Dirac semimetal

Colossal magnetoresistance (MR) is a well-known phenomenon, notably observed in hole-doped ferromagnetic manganites. It remains a major research topic due to its potential in technological applications. Though topological semimetals also show large MR, its origin and nature are completely different. Here, we show that in the highly electron doped region, the Dirac semimetal CeSbTe demonstrates similar properties as the manganites. CeSb$_{0.11}$Te$_{1.90}$ hosts multiple charge density wave (CDW) modulation-vectors and has a complex magnetic phase diagram. We confirm that this compound is an antiferromagnetic Dirac semimetal. Despite having a metallic Fermi surface, the electronic transport properties are semiconductor-like and deviate from known theoretical models. An external magnetic field induces a semiconductor-metal-like transition, which results in a colossal negative MR. Moreover, signatures of the coupling between the CDW and a spin modulation are observed in resistivity. This spin modulation also produces a giant anomalous Hall response.

cond-mat.mtrl-sci↗

arXiv2022

Transport signatures of Fermi arcs at twin boundaries in Weyl materials

One of the most striking signatures of Weyl fermions is their surface Fermi arcs. Less known is that Fermi arcs can also be localized at internal twin boundaries where two Weyl materials of opposite chirality meet. In this work, we derive constraints on the topology and connectivity of these "internal Fermi arcs." We show that internal Fermi arcs can exhibit transport signatures and propose two probes: quantum oscillations and a quantized chiral magnetic current. We propose merohedrally twinned B20 materials as candidates to host internal Fermi arcs, verified through both model and ab initio calculations. Our theoretical investigation sheds lights on the topological features and motivates experimental studies into the intriguing physics of internal Fermi arcs.

cond-mat.mes-hall↗

arXiv2022

Catalogue of Flat-Band Stoichiometric Materials

Topological electronic flatten bands near or at the Fermi level are a promising avenue towards unconventional superconductivity and correlated insulating states. However, the related experiments are mostly limited to the engineered materials, such as moire systems. Here we present a catalogue of all the three-dimensional stoichiometric materials with flat bands around the Fermi level that exist in nature. We consider 55,206 materials from the Inorganic Crystal Structure Database catalogued using the Topological Quantum Chemistry website which provides their structural parameters, space group (SG), band structure, density of states and topological characterization. We combine several direct signatures and properties of band flatness to a high-throughput analysis of all crystal structures. In particular, we identify materials hosting line-graph or bipartite sublattices - either in two or three dimensions - likely leading to flat bands. From this trove of information, we create the Materials Flatband Database website, a powerful search engine for future theoretical and experimental studies. We use it to extract a curated list of 2,379 materials, with among them 345 promising candidates, potentially hosting flat bands whose charge centers are not strongly localized on the atomic sites. We showcase five representative materials: KAg[CN]2 in SG 163 $(P\bar{3}1c)$, Pb2Sb2O7 in SG 227 $(Fd\bar{3}m)$, Rb2CaH4 in SG 139 $(I4/mmm)$, Ca2NCl in SG 166 $(R\bar{3}m)$ and WO3 in SG 221 $(Pm\bar{3}m)$. We provide a theoretical explanation for the origin of their flat bands close to the Fermi energy using the $S$-matrix method introduced in a parallel work [Calugaru et al., Nature Physics 18, 185 (2022)].

cond-mat.str-el↗

arXiv2022

Synthesis of an aqueous, air-stable, superconducting 1T'-WS$_2$ monolayer-ink

Liquid-phase chemical exfoliation is ideal to achieve industry scale production of two-dimensional (2D) materials for a wide range of application such as printable electronics, catalysis and energy storage. However, many impactful 2D materials with potentials in quantum technologies can only be studied in lab settings due to their air-sensitivity, and loss of physical performance after chemical processing. Here, we report a simple chemical exfoliation method to create a stable, aqueous, surfactant-free, superconducting ink containing phase-pure 1T'-WS$_2$ monolayers that are isotructural to the air-sensitive topological insulator 1T'-WTe$_2$. We demonstrate that thin films can be cast on both hard and flexible substrates. The printed film is metallic at room temperature and superconducting below 7.3 K, shows strong anisotropic unconventional superconducting behavior with an in-plane and out-of-plane upper critical magnetic field of 30.1 T and 5.3 T, has a critical current of 44 mA, and is stable at ambient conditions for at least 30 days. Our results show that chemical processing can provide an engineering solution, which makes non-trivial 2D materials that used to be only studied in laboratories commercially accessible.

cond-mat.mtrl-sci↗

arXiv2022

A Class of Magnetic Topological Material Candidates with Hypervalent Bi Chains

The link between crystal and electronic structure is crucial for understanding structure-property relations in solid-state chemistry. In particular, it has been instrumental in understanding topological materials, where electrons behave differently than they would in conventional solids. Herein, we identify 1D Bi chains as a structural motif of interest for topological materials. We focus on Sm$_3$ZrBi$_5$, a new quasi-one-dimensional (1D) compound in the Ln$_3$MPn$_5$ (Ln = lanthanide; M = metal; Pn = pnictide) family that crystallizes in the P$6_{3}$/mcm space group. Density functional theory calculations indicate a complex, topologically non-trivial electronic structure that changes significantly in the presence of spin-orbit coupling. Magnetic measurements show a quasi-1D antiferromagnetic structure with two magnetic transitions at 11.7 and 10.7 K that are invariant to applied field up to 9 T, indicating magnetically frustrated spins. Heat capacity, electrical, and thermal transport measurements support this claim and suggest complex scattering behavior in Sm$_3$ZrBi$_5$. This work highlights 1D chains as an unexplored structural motif for identifying topological materials, as well as the potential for rich physical phenomena in the Ln$_3$MPn$_5$ family.

cond-mat.mtrl-sci↗

arXiv2022

Evidence for a Monolayer Excitonic Insulator

The interplay between topology and correlations can generate a variety of quantum phases, many of which remain to be explored. Recent advances have identified monolayer WTe2 as a promising material for doing so in a highly tunable fashion. The ground state of this two-dimensional (2D) crystal can be electrostatically tuned from a quantum spin Hall insulator (QSHI) to a superconductor. However, much remains unknown about the gap-opening mechanism of the insulating state. Here we report evidence that the QSHI is also an excitonic insulator (EI), arising from the spontaneous formation of electron-hole bound states (excitons). We reveal the presence of an intrinsic insulating state at the charge neutrality point (CNP) in clean samples and confirm the correlated nature of this charge-neutral insulator by tunneling spectroscopy. We provide evidence against alternative scenarios of a band insulator or a localized insulator and support the existence of an EI phase in the clean limit. These observations lay the foundation for understanding a new class of correlated insulators with nontrivial topology and identify monolayer WTe2 as a promising candidate for exploring quantum phases of ground-state excitons.

cond-mat.mes-hall↗

arXiv2021

One-Dimensional Luttinger Liquids in a Two-Dimensional Moiré Lattice

The Luttinger liquid (LL) model of one-dimensional (1D) electronic systems provides a powerful tool for understanding strongly correlated physics including phenomena such as spin-charge separation. Substantial theoretical efforts have attempted to extend the LL phenomenology to two dimensions (2D), especially in models of closely packed arrays of 1D quantum wires, each being described as a LL. Such coupled-wire models have been successfully used to construct 2D anisotropic non-Fermi liquids, quantum Hall states, topological phases, and quantum spin liquids. However, an experimental demonstration of high-quality arrays of 1D LLs suitable for realizing these models remains absent. Here we report the experimental realization of 2D arrays of 1D LLs with crystalline quality in a moiré superlattice made of twisted bilayer tungsten ditelluride (tWTe$_{2}$). Originating from the anisotropic lattice of the monolayer, the moiré pattern of tWTe$_{2}$ hosts identical, parallel 1D electronic channels, separated by a fixed nanoscale distance, which is tunable by the interlayer twist angle. At a twist angle of ~ 5 degrees, we find that hole-doped tWTe$_{2}$ exhibits exceptionally large transport anisotropy with a resistance ratio of ~ 1000 between two orthogonal in-plane directions. The across-wire conductance exhibits power-law scaling behaviors, consistent with the formation of a 2D anisotropic phase that resembles an array of LLs. Our results open the door for realizing a variety of correlated and topological quantum phases based on coupled-wire models and LL physics.

cond-mat.mes-hall↗

arXiv2021

Phase tuning of multiple Andreev reflections of Dirac fermions and the Josephson supercurrent in Al-MoTe2-Al junctions

When a normal metal $N$ is sandwiched between two superconductors, the energy gaps in the latter act as walls that confine electrons in $N$ in a square-well potential. If the voltage $V$ across $N$ is finite, an electron injected into the well undergoes multiple Andreev reflections (MAR) until it gains enough energy to overcome the energy barrier. Because each reflection converts an electron to a hole (or vice versa), while creating (or destroying) a Cooper pair, the MAR process shuttles a stream of pairs across the junction. An interesting question is, given a finite $V$, what percentage of the shuttled pairs end up as a Josephson supercurrent? This fraction does not seem to have been measured. Here we show that, in high-transparency junctions based on the type II Dirac semimetal MoTe$_2$, the MAR leads to a stair-case profile in the current-voltage ($I$-$V$) response, corresponding to pairs shuttled incoherently by the $n^{th}$-order process. By varying the phase $φ$ across the junction, we demonstrate that a Josephson supercurrent ${\bf J}_{\rm s}\sim \sinφ$ co-exists with the MAR steps, even at large $V$. The observed linear increase in the amplitude of ${\bf J}_{\rm s}$ with $n$ (for small $n$) implies that ${\bf J}_{\rm s}$ originates from the population of pairs that are coherently shuttled. We infer that the MAR steps and the supercurrent are complementary aspects of the Andreev process. The experiment yields the percentage of shuttled pairs that form the supercurrent. At large $V$, the coherent fraction is initially linear in $n$. However, as $V\to 0$ ($n\gg 1$), almost all the pairs end up as the observed Josephson supercurrent.

cond-mat.supr-con↗

arXiv2021

Axial Higgs Mode Detected by Quantum Pathway Interference in RTe3

The observation of the Higgs boson solidified the standard model of particle physics. However, explanations of anomalies (e.g. dark matter) rely on further symmetry breaking calling for an undiscovered axial Higgs mode. In condensed matter the Higgs was seen in magnetic, superconducting and charge density wave(CDW) systems. Uncovering a low energy mode's vector properties is challenging, requiring going beyond typical spectroscopic or scattering techniques. Here, we discover an axial Higgs mode in the CDW system RTe3 using the interference of quantum pathways. In RTe3 (R=La,Gd), the electronic ordering couples bands of equal or different angular momenta. As such, the Raman scattering tensor associated to the Higgs mode contains both symmetric and antisymmetric components, which can be excited via two distinct, but degenerate pathways. This leads to constructive or destructive interference of these pathways, depending on the choice of the incident and Raman scattered light polarization. The qualitative behavior of the Raman spectra is well-captured by an appropriate tight-binding model including an axial Higgs mode. The elucidation of the antisymmetric component provides direct evidence that the Higgs mode contains an axial vector representation (i.e. a pseudo-angular momentum) and hints the CDW in RTe3 is unconventional. Thus we provide a means for measuring collective modes quantum properties without resorting to extreme experimental conditions.

physics.optics↗

arXiv2021

TaCo$_{2}$Te$_{2}$: An air-stable, magnetic van der Waals material with high mobility

Van der Waals (vdW) materials are an indispensable part of functional device technology due to their versatile physical properties and ease of exfoliating to the low-dimensional limit. Among all the compounds investigated so far, the search for magnetic vdW materials has intensified in recent years, fueled by the realization of magnetism in two dimensions (2D). However, metallic magnetic vdW systems are still uncommon. In addition, they rarely host high-mobility charge carriers, which is an essential requirement for high-speed electronic applications. Another shortcoming of 2D magnets is that they are highly air sensitive. Using chemical reasoning, we introduce TaCo2Te2 as an air-stable, high-mobility, magnetic vdW material. It has a layered structure, which consists of Peierls distorted Co chains and a large vdW gap between the layers. We find that the bulk crystals can be easily exfoliated and the obtained thin flakes are robust to ambient conditions after four months of monitoring using an optical microscope. We also observe signatures of canted antiferromagntic behavior at low-temperature. TaCo2Te2 shows a metallic character and a large, non-saturating, anisotropic magnetoresistance. Furthermore, our Hall data and quantum oscillation measurements reveal the presence of both electron- and hole-type carriers and their high mobility.

cond-mat.mtrl-sci↗

arXiv2021

Real-space visualization of quasiparticle dephasing near the Planckian limit in the Dirac line node material ZrSiS

Dirac line node (DLN) materials are topological semimetals wherein a set of symmetry protected crossing points forms a one-dimensional (1D) line in reciprocal space. Not only are the linearly dispersing bands expected to give rise to exceptional electronic properties, but the weak screening of the Coulomb interaction near the line node may enhance electronic correlations, produce new many-body ground states, or influence the quasiparticle lifetime. We investigate the quasiparticle dynamics in the DLN material ZrSiS via spectroscopic imaging scanning tunneling microscopy (SI-STM). By studying the spatial decay of quasiparticle interference patterns (QPI) from point scatterers, we were able to directly and selectively extract the phase coherence length $l_{\textrm{QPI}}$ and lifetime $τ_{\textrm{QPI}}$ for the bulk DLN excitations, which are dominated by inelastic electron-electron scattering. We find that the experimental $τ_{\textrm{QPI}}(E)$ values below $-$40 meV are very short, likely due to the stronger Coulomb interactions, and lie at the Planckian limit $\hbar/|E|$. Our results corroborate a growing body of experimental reports demonstrating unusual electronic correlation effects near a DLN.

cond-mat.str-el↗

arXiv2021

Theoretical study of topological properties of ferromagnetic pyrite CoS$_2$

Since the discovery of the first topological material 15 years ago, the search for material realizations of novel topological phases has become the driving force of the field. While oftentimes we search for new materials, we forget that well established materials can also display very interesting topological properties. In this work, we revisit CoS$_2$ , a metallic ferromagnetic pyrite that has been extensively studied in the literature due to its magnetic properties. We study the topological features of its electronic band structure and identify Weyl nodes and Nodal lines, as well as a symmetry-protected 4-fold fermion close to the Fermi level. Looking at different surface cleavage planes, we observe both spin polarized Fermi arcs in the majority channel and drumhead states. These findings suggest that CoS$_2$ is a promising platform to study topological phenomena, as well as a good candidate for spintronic applications.

cond-mat.mtrl-sci↗

arXiv2021

Robust narrow-gap semiconducting behavior in square-net La$_{3}$Cd$_{2}$As$_{6}$

ABSTRACT: Narrow-gap semiconductors are sought-after materials due to their potential for long-wavelength detectors, thermoelectrics, and more recently non-trivial topology. Here we report the synthesis and characterization of a new family of narrow-gap semiconductors, $R$$_{3}$Cd$_{2}$As$_{6}$ ($R=$ La, Ce). Single crystal x-ray diffraction at room temperature reveals that the As square nets distort and Cd vacancies order in a monoclinic superstructure. A putative charge-density ordered state sets in at 279~K in La$_{3}$Cd$_{2}$As$_{6}$ and at 136~K in Ce$_{3}$Cd$_{2}$As$_{6}$ and is accompanied by a substantial increase in the electrical resistivity in both compounds. The resistivity of the La member increases by thirteen orders of magnitude on cooling, which points to a remarkably clean semiconducting ground state. Our results suggest that light square net materials within a $I4/mmm$ parent structure are promising clean narrow-gap semiconductors.

cond-mat.mtrl-sci↗

arXiv2021

Evolving Devil's staircase magnetization from tunable charge density waves in nonsymmorphic Dirac semimetals

While several magnetic topological semimetals have been discovered in recent years, their band structures are far from ideal, often obscured by trivial bands at the Fermi energy. Square-net materials with clean, linearly dispersing bands show potential to circumvent this issue. CeSbTe, a square-net material, features multiple magnetic field-controllable topological phases. Here, it is shown that in this material, even higher degrees of tunability can be achieved by changing the electron count at the square-net motif. Increased electron filling results in structural distortion and formation of charge density waves (CDWs). The modulation wave-vector evolves continuously leading to a region of multiple discrete CDWs and a corresponding complex "Devil's staircase" magnetic ground state. A series of fractionally quantized magnetization plateaus are observed, which implies direct coupling between CDW and a collective spin-excitation. It is further shown that the CDW creates a robust idealized non-symmorphic Dirac semimetal, thus providing access to topological systems with rich magnetism.

cond-mat.mtrl-sci↗