Toward 1D Transport in 3D Materials: SOC-Induced Charge-Transport Anisotropy in Sm3ZrBi5.

1D charge transport offers great insight into strongly correlated physics, such as Luttinger liquids, electronic instabilities, and superconductivity. Although 1D charge transport is observed in nanomaterials and quantum wires, examples in bulk crystalline solids remain elusive. In this work, it is demonstrated that spin-orbit coupling (SOC) can act as a mechanism to induce quasi-1D charge transport in the Ln3MPn5 (Ln = lanthanide; M = transition metal; Pn = Pnictide) family. From three example compounds, La3ZrSb5, La3ZrBi5, and Sm3ZrBi5, density functional theory calculations with SOC included show a quasi-1D Fermi surface in the bismuthide compounds, but an anisotropic 3D Fermi surface in the antimonide structure. By performing anisotropic charge transport measurements on La3ZrSb5, La3ZrBi5, and Sm3ZrBi5, it is demonstrated that SOC starkly affects their anisotropic resistivity ratios (ARR) at low temperatures, with an ARR of ≈4 in the antimonide compared to ≈9.5 and ≈22 (≈32 after magnetic ordering) in La3ZrBi5 and Sm3ZrBi5, respectively. This report demonstrates the utility of spin-orbit coupling to induce quasi-low-dimensional Fermi surfaces in anisotropic crystal structures, and provides a template for examining other systems.

Chemical Bonding Induces One-Dimensional Physics in Bulk Crystal BiIr4Se8.

One-dimensional (1D) systems persist as some of the most interesting because of the rich physics that emerges from constrained degrees of freedom. A desirable route to harness the properties therein is to grow bulk single crystals of a physically three-dimensional (3D) but electronically 1D compound. Most bulk compounds which approach the electronic 1D limit still field interactions across the other two crystallographic directions and, consequently, deviate from the 1D models. In this paper, we lay out chemical concepts to realize the physics of 1D models in 3D crystals. These are based on both structural and electronic arguments. We present BiIr4Se8, a bulk crystal consisting of linear Bi2+ chains within a scaffolding of IrSe6 octahedra, as a prime example. Through crystal structure analysis, density functional theory calculations, X-ray diffraction, and physical property measurements, we demonstrate the unique 1D electronic configuration in BiIr4Se8. This configuration at ambient temperature is a gapped Su-Schriefer-Heeger system, generated by way of a canonical Peierls distortion involving Bi dimerization that relieves instabilities in a 1D metallic state. At 190 K, an additional 1D charge density wave distortion emerges, which affects the Peierls distortion. The experimental evidence validates our design principles and distinguishes BiIr4Se8 among other quasi-1D bulk compounds. We thus show that it is possible to realize unique electronically 1D materials applying chemical concepts.

Chemical exfoliation of 1-dimensional antiferromagnetic nanoribbons from a non-van der Waals material.

As the demand for increasingly varied types of 1-dimensional (1D) materials grows, there is a greater need for new methods to synthesize these types of materials in a simple and scalable way. Chemical exfoliation is commonly used to make 2-dimensional (2D) materials, often in a way that is both straightforward and suitable for making larger quantities, yet this method has thus far been underutilized for synthesizing 1D materials. In the few instances when chemical exfoliation has been used to make 1D materials, the starting compound has been a van der Waals material, thus excluding any structures without these weak bonds inherently present. We demonstrate here that ionically bonded crystals can also be chemically exfoliated to 1D structures by choosing KFeS2 as an example. Using chemical exfoliation, antiferromagnetic 1D nanoribbons can be yielded in a single step. The nanoribbons are crystalline and closely resemble the parent compound both in structure and in intrinsic antiferromagnetism. The facile chemical exfoliation of an ionically bonded crystal shown in this work opens up opportunities for the synthesis of both magnetic and non-magnetic 1D nanomaterials from a greater variety of starting structures.

Evidence for two dimensional anisotropic Luttinger liquids at millikelvin temperatures.

Interacting electrons in one dimension (1D) are governed by the Luttinger liquid (LL) theory in which excitations are fractionalized. Can a LL-like state emerge in a 2D system as a stable zero-temperature phase? This question is crucial in the study of non-Fermi liquids. A recent experiment identified twisted bilayer tungsten ditelluride (tWTe2) as a 2D host of LL-like physics at a few kelvins. Here we report evidence for a 2D anisotropic LL state down to 50 mK, spontaneously formed in tWTe2 with a twist angle of ~ 3o. While the system is metallic-like and nearly isotropic above 2 K, a dramatically enhanced electronic anisotropy develops in the millikelvin regime. In the anisotropic phase, we observe characteristics of a 2D LL phase including a power-law across-wire conductance and a zero-bias dip in the along-wire differential resistance. Our results represent a step forward in the search for stable LL physics beyond 1D.

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 micrometer-sized two-dimensional van der Waals materials and devices. We demonstrate its performance by implementing photocurrent-based Fourier transform infrared spectroscopy on a monolayer WTe2 device and a multilayer 1T-TaS2 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.

Colossal magnetoresistance in the multiple wave vector charge density wave regime of an antiferromagnetic Dirac semimetal.

Colossal negative magnetoresistance 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. In contrast, topological semimetals show large but positive magnetoresistance, originated from the high-mobility charge carriers. Here, we show that in the highly electron-doped region, the Dirac semimetal CeSbTe demonstrates similar properties as the manganites. CeSb0.11Te1.90 hosts multiple charge density wave 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 magnetoresistance. Moreover, signatures of the coupling between the charge density wave and a spin modulation are observed in resistivity. This spin modulation also produces a giant anomalous Hall response.

Atomic Resolution Imaging of Highly Air-Sensitive Monolayer and Twisted-Bilayer WTe2.

Bulk Td-WTe2 is a semimetal, while its monolayer counterpart is a two-dimensional (2D) topological insulator. Recently, electronic transport resembling a Luttinger liquid state was found in twisted-bilayer WTe2 (tWTe2) with a twist angle of ∼5°. Despite the strong interest in 2D WTe2 systems, little experimental information is available about their intrinsic microstructure, leaving obstacles in modeling their physical properties. The monolayer, and consequently tWTe2, are highly air-sensitive, and therefore, probing their atomic structures is difficult. In this study, we develop a robust method for atomic-resolution visualization of monolayers and tWTe2 obtained through mechanical exfoliation and fabrication. We confirm the high crystalline quality of mechanically exfoliated WTe2 samples and observe that tWTe2 with twist angles of ∼5 and ∼2° retains its pristine moiré structure without substantial deformations or reconstructions. The results provide a structural foundation for future electronic modeling of monolayer and tWTe2 moiré lattices.

Synthesis of an aqueous, air-stable, superconducting 1T'-WS2 monolayer ink.

Liquid-phase chemical exfoliation can achieve industry-scale production of two-dimensional (2D) materials for a wide range of applications. However, many 2D materials with potential applications in quantum technologies often fail to leave the laboratory setting because of their air sensitivity and depreciation of physical performance after chemical processing. We report a simple chemical exfoliation method to create a stable, aqueous, surfactant-free, superconducting ink containing phase-pure 1T'-WS2 monolayers that are isostructural to the air-sensitive topological insulator 1T'-WTe2. The printed film is metallic at room temperature and superconducting below 7.3 kelvin, shows strong anisotropic unconventional superconducting behavior with an in-plane and out-of-plane upper critical magnetic field of 30.1 and 5.3 tesla, and is stable at ambient conditions for at least 30 days. Our results show that chemical processing can make nontrivial 2D materials that were formerly only studied in laboratories commercially accessible.

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 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). Scanning transmission electron microscopy reveals that this internal interface is a (001) twin plane which connects two enantiomeric counterparts at an atomically sharp interface with inversion twinning. Ab initio calculations show localized internal Fermi arcs at the (001) twin plane that can be clearly distinguished from both external Fermi arcs and bulk states. These merohedrally twinned CoSi NWs provide an ideal platform to explore topological properties associated with internal interfaces in WSMs.

Unlocking High Capacity and Fast Na+ Diffusion of Hx CrS2 by Proton-Exchange Pretreatment.

This study presents a new material, "Hx CrS2 " (denotes approximate composition) formed by proton-exchange of NaCrS2 which has a measured capacity of 728 mAh g-1 with significant improvements to capacity retention, sustaining over 700 mAh g-1 during cycling experiments. This is the highest reported capacity for a transition metal sulfide electrode and outperforms the most promising proposed sodium anodes to date. Hx CrS2 exhibits a biphasic structure featuring alternating crystalline and amorphous lamella on the scale of a few nanometers. This unique structural motif enables reversible access to Cr redox in the material resulting in higher capacities than seen in the parent structure which features only S redox. Pretreatment by proton-exchange offers a route to materials such as Hx CrS2 which provide fast diffusion and high capacities for sodium-ion batteries.

Chemical Exfoliation toward Magnetic 2D VOCl Monolayers.

The diversification of magnetic two-dimensional (2D) materials holds the key to the further development of advanced technologies, such as spintronic devices and efficient data storage. However, the search for intrinsic magnetism down to the 2D limit is severely limited by the ability to reliably exfoliate large, air-stable nanosheets. Chemical exfoliation, a relatively underutilized method for delamination, offers many advantages, including a high degree of adaptability and higher yields of uniformly exfoliated materials. van der Waals (vdW) materials, in particular the family of transition-metal oxyhalides, are ideal candidates for chemical exfoliation due to their large interlayer spacing and the wide variety of interesting magnetic properties they exhibit. In this study, we employ a chemical exfoliation method to delaminate the layered antiferromagnet vanadium oxychloride (VOCl) down to the monolayer limit. The resulting nansoheets have lateral sizes of up to 20 µm, are air-stable, and can be easily isolated. Magnetic characterization was performed throughout the exfoliation process, tracking the changes in magnetic behavior among bulk VOCl, its lithiated intercalate, and the restacked nanosheet pellet. The results from this work demonstrate the potential of chemical exfoliation, along with illustrating the effects of low dimensionality on magnetic properties.

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

When an electron is incident on a superconductor from a metal, it is reflected as a hole in a process called Andreev reflection. If the metal N is sandwiched between two superconductors S in an SNS junction, multiple Andreev reflections (MARs) occur. We have found that, in SNS junctions with high transparency ([Formula: see text]) based on the Dirac semimetal MoTe2, the MAR features are observed with exceptional resolution. By tuning the phase difference [Formula: see text] between the bracketing Al superconductors, we establish that the MARs coexist with a Josephson supercurrent [Formula: see text]. As we vary the junction voltage V, the supercurrent amplitude [Formula: see text] varies in step with the MAR order n, revealing a direct relation between them. Two successive Andreev reflections serve to shuttle a Cooper pair across the junction. If the pair is shuttled coherently, it contributes to [Formula: see text]. The experiment measures the fraction of pairs shuttled coherently vs. V. Surprisingly, superconductivity in MoTe2 does not affect the MAR features.

Simple Chemical Rules for Predicting Band Structures of Kagome Materials.

Compounds featuring a kagome lattice are studied for a wide range of properties, from localized magnetism to massless and massive Dirac Fermions. These properties come from the symmetry of the kagome lattice, which gives rise to Dirac cones and flat bands. However, not all compounds with a kagome sublattice show properties related to it. We derive chemical rules predicting if the low-energy physics of a material is determined by the kagome sublattice and bands arising from it. After sorting out all known crystals with the kagome lattice into four groups, we use chemical heuristics and local symmetry to explain additional conditions that need to be met to have kagome bands near the Fermi level.

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 (for example, dark matter) rely on further symmetry breaking, calling for an undiscovered axial Higgs mode1. The Higgs mode was also seen in magnetic, superconducting and charge density wave (CDW) systems2,3. Uncovering the vector properties of a low-energy mode is challenging, and requires 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 momenta4-6. As such, the Raman scattering tensor associated with the Higgs mode contains both symmetric and antisymmetric components, which are 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 behaviour of the Raman spectra is well captured by an appropriate tight-binding model, including an axial Higgs mode. Elucidation of the antisymmetric component is direct evidence that the Higgs mode contains an axial vector representation (that is, a pseudo-angular momentum) and hints that the CDW is unconventional. Thus, we provide a means for measuring quantum properties of collective modes without resorting to extreme experimental conditions.

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 separation1. Substantial theoretical efforts have attempted to extend the LL phenomenology to two dimensions, especially in models of closely packed arrays of 1D quantum wires2-13, each being described as a LL. Such coupled-wire models have been successfully used to construct two-dimensional (2D) anisotropic non-Fermi liquids2-6, quantum Hall states7-9, topological phases10,11 and quantum spin liquids12,13. 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 (tWTe2). Originating from the anisotropic lattice of the monolayer, the moiré pattern of tWTe2 hosts identical, parallel 1D electronic channels, separated by a fixed nanoscale distance, which is tuneable by the interlayer twist angle. At a twist angle of approximately 5 degrees, we find that hole-doped tWTe2 exhibits exceptionally large transport anisotropy with a resistance ratio of around 1,000 between two orthogonal in-plane directions. The across-wire conductance exhibits power-law scaling behaviours, 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.

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 Sm3ZrBi5, a new quasi-one-dimensional (1D) compound in the Ln3MPn5 (Ln = lanthanide; M = metal; Pn = pnictide) family that crystallizes in the P63/mcm space group. Density functional theory calculations indicate a complex, topologically nontrivial 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 thermoelectric measurements support this claim and suggest complex scattering behavior in Sm3ZrBi5. 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 Ln3MPn5 family.

Catalogue of flat-band stoichiometric materials.

Topological electronic flattened bands near or at the Fermi level are a promising route towards unconventional superconductivity and correlated insulating states. However, the related experiments are mostly limited to engineered materials, such as moiré systems1-3. Here we present a catalogue of the naturally occuring three-dimensional stoichiometric materials with flat bands around the Fermi level. We consider 55,206 materials from the Inorganic Crystal Structure Database catalogued using the Topological Quantum Chemistry website4,5, which provides their structural parameters, space group, band structure, density of states and topological characterization. We combine several direct signatures and properties of band flatness with a high-throughput analysis of all crystal structures. In particular, we identify materials hosting line-graph or bipartite sublattices-in either two or three dimensions-that probably lead 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 the database to extract a curated list of 2,379 high-quality flat-band materials, from which we identify 345 promising candidates that potentially host flat bands with charge centres that are not strongly localized on the atomic sites. We showcase five representative materials and 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 work6.

Square-Net Topological Semimetals: How Spectroscopy Furthers Understanding and Control.

Square-net materials are well positioned to lead optical spectroscopic explorations into the electronic structure, photoinduced dynamics, and phase transitions in topological semimetals. Hundreds of square-net topological semimetals can be prepared that have remarkably different electronic and optical properties despite having similar structures. Here we present what has been gleaned recently from these materials with the whole gamut of optical spectroscopies, ranging from steady-state reflectance and Raman investigations into topological band structures, electronic correlations, and equilibrium phase transitions to time-resolved techniques used to decipher ultrafast relaxation dynamics and nonequilibrium photoinduced phase transitions. We end with a discussion of some major remaining questions and possible future research directions.

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 is observed, which implies direct coupling between CDW and a collective spin-excitation. It is further shown that the CDW creates a robust idealized nonsymmorphic Dirac semimetal, thus providing access to topological systems with rich magnetism.