Charge Density Wave Materials Research Articles

Intriguing Low-Temperature Phase in the Antiferromagnetic Kagome Metal FeGe.

The properties of kagome metals are governed by the interdependence of band topology and electronic correlations resulting in remarkably rich phase diagrams. Here, we study the temperature evolution of the bulk electronic structure of the antiferromagnetic kagome metal FeGe using infrared spectroscopy. We uncover drastic changes in the low-energy interband absorption at the 100K structural phase transition that has been linked to a charge-density-wave (CDW) instability. We explain this effect by the minuscule Fe displacement in the kagome plane, which results in parallel bands in the vicinity of the Fermi level. In contrast to conventional CDW materials, however, the spectral weight shifts to low energies, ruling out the opening of a CDW gap in FeGe.

Origin of Distinct Insulating Domains in the Layered Charge Density Wave Material 1T-TaS2.

Vertical charge order shapes the electronic properties in layered charge density wave (CDW) materials. Various stacking orders inevitably create nanoscale domains with distinct electronic structures inaccessible to bulk probes. Here, the stacking characteristics of bulk 1T-TaS2 are analyzed using scanning tunneling spectroscopy (STS) and density functional theory (DFT) calculations. It is observed that Mott-insulating domains undergo a transition to band-insulating domains restoring vertical dimerization of the CDWs. Furthermore, STS measurements covering a wide terrace reveal two distinct band insulating domains differentiated by band edge broadening. These DFT calculations reveal that the Mott insulating layers preferably reside on the subsurface, forming broader band edges in the neighboring band insulating layers. Ultimately, buried Mott insulating layers believed to harbor the quantum spin liquid phase are identified. These results resolve persistent issues regarding vertical charge order in 1T-TaS2, providing a new perspective for investigating emergent quantum phenomena in layered CDWmaterials.

Ultrafast creation of a light-induced semimetallic state in strongly excited 1T-TiSe2.

Screening, a ubiquitous phenomenon associated with the shielding of electric fields by surrounding charges, has been widely adopted as a means to modify a material's properties. While most studies have relied on static changes of screening through doping or gating thus far, here we demonstrate that screening can also drive the onset of distinct quantum states on the ultrafast timescale. By using time- and angle-resolved photoemission spectroscopy, we show that intense optical excitation can drive 1T-TiSe2, a prototypical charge density wave material, almost instantly from a gapped into a semimetallic state. By systematically comparing changes in band structure over time and excitation strength with theoretical calculations, we find that the appearance of this state is likely caused by a dramatic reduction of the screening length. In summary, this work showcases how optical excitation enables the screening-driven design of a nonequilibrium semimetallic phase in TiSe2, possibly providing a general pathway into highly screened phases in other strongly correlated materials.

Photodoping-Modified Charge Density Wave Phase Transition in WS2/1T-TaS2 Heterostructure

Controlling collective electronic states hold great promise for development of innovative devices. Here, we experimentally detect the modification of the charge density wave (CDW) phase transition within a 1T-TaS2 layer in a WS2/1T-TaS2 heterostructure using time-resolved ultrafast spectroscopy. Laser-induced charge transfer doping strongly suppresses the commensurate CDW phase, which results in a significant decrease in both the phase transition temperature (T c) and phase transition stiffness. We interpret the phenomenon that photo-induced hole doping, when surpassing a critical threshold value of ∼ 1018 cm−3, sharply decreases the phase transition energy barrier. Our results provide new insights into controlling the CDW phase transition, paving the way for optical-controlled novel devices based on CDW materials.

An exactly solvable model of randomly pinned charge density waves in two dimensions

The nature of the interplay between fluctuations and quenched random disorder is a long-standing open problem, particularly in systems with a continuous order parameter. This lack of a full theoretical treatment has been underscored by recent advances in experiments on charge density wave materials. To address this problem, we formulate an exactly solvable model of a two-dimensional randomly pinned incommensurate charge density wave, and use the large-N technique to map out the phase diagram and order parameter correlations. Our approach captures the physics of the Berezinskii–Kosterlitz–Thouless phase transition in the clean limit at large N. We pay particular attention to the roles of thermal fluctuations and quenched random field disorder in destroying long-range order, finding a novel crossover between weakly- and strongly-disordered regimes.

In operando cryo-STEM of pulse-induced charge density wave switching in TaS2

The charge density wave material 1T-TaS2 exhibits a pulse-induced insulator-to-metal transition, which shows promise for next-generation electronics such as memristive memory and neuromorphic hardware. However, the rational design of TaS2 devices is hindered by a poor understanding of the switching mechanism, the pulse-induced phase, and the influence of material defects. Here, we operate a 2-terminal TaS2 device within a scanning transmission electron microscope at cryogenic temperature, and directly visualize the changing charge density wave structure with nanoscale spatial resolution and down to 300 μs temporal resolution. We show that the pulse-induced transition is driven by Joule heating, and that the pulse-induced state corresponds to the nearly commensurate and incommensurate charge density wave phases, depending on the applied voltage amplitude. With our in operando cryogenic electron microscopy experiments, we directly correlate the charge density wave structure with the device resistance, and show that dislocations significantly impact device performance. This work resolves fundamental questions of resistive switching in TaS2 devices, critical for engineering reliable and scalable TaS2 electronics.

Observation of momentum-dependent charge density wave gap in a layered antiferromagnet {textrm{Gd}}{textrm{Te}}_{3}

Charge density wave (CDW) ordering has been an important topic of study for a long time owing to its connection with other exotic phases such as superconductivity and magnetism. The R{textrm{Te}}_{3} (R = rare-earth elements) family of materials provides a fertile ground to study the dynamics of CDW in van der Waals layered materials, and the presence of magnetism in these materials allows to explore the interplay among CDW and long range magnetic ordering. Here, we have carried out a high-resolution angle-resolved photoemission spectroscopy (ARPES) study of a CDW material {textrm{Gd}}{textrm{Te}}_{3}, which is antiferromagnetic below sim mathrm {12~K}, along with thermodynamic, electrical transport, magnetic, and Raman measurements. Our ARPES data show a two-fold symmetric Fermi surface with both gapped and ungapped regions indicative of the partial nesting. The gap is momentum dependent, maximum along {overline{Gamma }}-mathrm{overline{Z}} and gradually decreases going towards {overline{Gamma }}-mathrm{overline{X}}. Our study provides a platform to study the dynamics of CDW and its interaction with other physical orders in two- and three-dimensions.

Cavity-mediated thermal control of metal-to-insulator transition in 1T-TaS2.

Placing quantum materials into optical cavities provides a unique platform for controlling quantum cooperative properties of matter, by both weak and strong light-matter coupling1,2. Here we report experimental evidence of reversible cavity control of a metal-to-insulator phase transition in a correlated solid-state material. We embed the charge density wave material 1T-TaS2 into cryogenic tunable terahertz cavities3 and show that a switch between conductive and insulating behaviours, associated with a large change in the sample temperature, is obtained by mechanically tuning the distance between the cavity mirrors and their alignment. The large thermal modification observed is indicative of a Purcell-like scenario in which the spectral profile of the cavity modifies the energy exchange between the material and the external electromagnetic field. Our findings provide opportunities for controlling the thermodynamics and macroscopic transport properties of quantum materials by engineering their electromagnetic environment.

Optically Induced Symmetry Breaking Due to Nonequilibrium Steady State Formation in Charge Density Wave Material 1T-TiSe2.

The strongly correlated charge density wave (CDW) phase of 1T-TiSe2 is of interest to verify the claims of a chiral order parameter. Characterization of the symmetries of 1T-TiSe2 is critical to understand the origin of its intriguing properties. Here we use very low-power, continuous wave laser excitation to probe the symmetries of 1T-TiSe2 by using the circular photogalvanic effect. We observe that the ground state of the CDW phase (D3d) is achiral. However, laser excitation above a threshold intensity transforms 1T-TiSe2 into a nonequilibrium chiral phase (C3), which changes the electronic correlations in the material. The inherent sensitivity of the photogalvanic technique to structural symmetries provides evidence of the different optically driven phase of 1T-TiSe2, which allows us to assign symmetry groups to these states. Our work demonstrates that optically induced phase change can occur at extremely low optical intensities in strongly correlated materials, providing a pathway to engineer new phases using light.

Charge‐Density‐Wave Resistive Switching and Voltage Oscillations in Ternary Chalcogenide BaTiS3

AbstractPhase change materials, which show different electrical characteristics across the phase transitions, have attracted considerable research attention for their potential electronic device applications. Materials with metal‐to‐insulator or charge density wave (CDW) transitions such as VO2 and 1T‐TaS2 have demonstrated voltage oscillations due to their robust bi‐state resistive switching behavior with some basic neuronal characteristics. BaTiS3 is a small bandgap ternary chalcogenide that has recently reported the emergence of CDW order below 245 K. Here, the discovery of DC voltage / current‐induced reversible threshold switching in BaTiS3 devices between a CDW phase and a room temperature semiconducting phase is reported. The resistive switching behavior is consistent with a Joule heating scheme and sustained voltage oscillations with a frequency of up to 1 kHz are demonstrated by leveraging the CDW phase transition and the associated negative differential resistance. Strategies of reducing channel sizes and improving thermal management may further improve the device's performance. The findings establish BaTiS3 as a promising CDW material for future electronic device applications, especially for energy‐efficient neuromorphic computing.

Orbital-selective charge-density wave in TaTe4

TaTe4, a metallic charge-density wave (CDW) material discovered decades ago, has attracted renewed attention due to its rich interesting properties, such as pressure-induced superconductivity and candidate nontrivial topological phase. Here, using high-resolution angle-resolved photoemission spectroscopy and ab initio calculation, we systematically investigate the electronic structure of TaTe4. At 26 K, we observe a CDW gap as large as 290 meV, which persists up to 500 K. The CDW-modulated band structure shows a complex reconstruction that closely correlates with the lattice distortion. Inside the CDW gap, there exist highly dispersive energy bands contributing to the remnant Fermi surface and metallic behavior in the CDW state. Interestingly, our ab initio calculation reveals that the large CDW gap mainly opens in the electronic states with out-of-plane orbital components, while the in-gap metallic states originate from in-plane orbitals, suggesting an orbital texture that couples with the CDW order. Our results shed light on the interplay between electron, lattice, and orbital in quasi-one-dimensional CDW materials.

Hybrid Quantum Systems for Higher Temperature Quantum Information Processing

The ability to operate superconducting quantum computers at higher temperatures would greatly expand their utility and range of applications. This could be achieved by increasing resonance frequencies and/or utilizing collective modes that are less noisy and more robust against decoherence. We discuss several nonlinear resonator concepts in which the roles of linear and nonlinear elements are reversed vs. the transmon. The simplest version is a nonlinear <italic xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">LC</i> resonator with a linear superconducting inductor and a nonlinear capacitor employing a nonlinear dielectric material. Due to progress in tunable dielectrics for 6G, some ferroelectric composites may enable operation of a nonlinear dielectric – superconductor qubit at hundreds of gigahertz. Other nonlinear dielectric materials include quantum paraelectrics and charge density wave materials. These are of interest due to robust collective modes resulting from macroscopically occupied states. Other proposed nonlinear resonators employing nonlinear dielectrics include quarter- and half-wavelength resonators. Voltage tunability is a potential feature of the proposed concepts.

Pressure effect of the charge density wave transition on Raman spectra and transport properties of 2H−NbSe2

Charge density wave (CDW) order is widely existing and fundamentally important in solid-state physics. However, several critical issues regarding the vibrational and electronic subsystems and their coupling still need to be better understood. Here, we tune the electrical transport and collective vibrational excitation, i.e., phonon and amplitude mode, by pressure in a prototype charge density wave material, $2H\text{\ensuremath{-}}{\mathrm{NbSe}}_{2}$. A complete pressure-temperature phase diagram is revisited. The anomaly in Hall and magnetoresistivity at CDW critical temperature, ${T}_{\mathrm{CDW}}$, was suppressed by the pressure. In the Raman spectroscopy measurements, the appearance of CDW amplitude mode is accompanied by the freezing of the two-phonon mode. The frequency of CDW amplitude mode under pressure follows modified mean-field theory with power-law scaling $(\ensuremath{\beta}=0.18)$. The renormalization of the Raman phonon across the CDW transition and the mean-field temperature dependence of CDW amplitude mode emphasized the importance of electron-phonon coupling in the formation of CDW state in $2H\text{\ensuremath{-}}{\mathrm{NbSe}}_{2}$. Our work clarifies the complex vibrational and electronic subsystems and sheds light on the mechanism of the charge density state in $2H\text{\ensuremath{-}}{\mathrm{NbSe}}_{2}$.

Ultrafast Switching from the Charge Density Wave Phase to a Metastable Metallic State in 1T-TiSe_{2}.

The ultrafast electronic structures of the charge density wave material 1T-TiSe_{2} were investigated by high-resolution time- and angle-resolved photoemission spectroscopy. We found that the quasiparticle populations drove ultrafast electronic phase transitions in 1T-TiSe_{2} within 100fs after photoexcitation, and a metastable metallic state, which was significantly different from the equilibrium normal phase, was evidenced far below the charge density wave transition temperature. Detailed time- and pump-fluence-dependent experiments revealed that the photoinduced metastable metallic state was a result of the halted motion of the atoms through the coherent electron-phonon coupling process, and the lifetime of this state was prolonged to picoseconds with the highest pump fluence used in this study. Ultrafast electronic dynamics were well captured by the time-dependent Ginzburg-Landau model. Our work demonstrates a mechanism for realizing novel electronic states by photoinducing coherent motion of atoms in the lattice.

The Influence of Dimensionality on the Charge‐Density‐Wave Transition and its Application on Mid‐Infrared Photodetection

Abstract2D charge density wave (CDW) materials receive much attention for high responsivity and broadband photodetection in recent years due to their collective electron transport and narrow bandgap. However, the high dark current density problem hinders their real application. Here, a sharp CDW transition in quasi‐1D (TaSe4)2I is reported and applied for broadband photodetection. Especially at mid‐infrared region, the device shows both high photo responsivity of 1.18 ×103 A W−1 and large light on/off ratio of 80, which is superior to 2D CDW TaS2 and most reported low‐dimensional materials. Such high performance relies on two aspects. One is the much lower dark current density resulting from the pseudo gap associated with 1D Luttinger liquid state, which is supported by finite size scaling of nonlinear I–V at variable temperatures and occurrence of 1D structural phase transition consolidated by in situ Raman spectroscopy. The other is the high photocurrent associated with the “Fröhlich superconductivity” state, manifested by an ultrasensitive switching, which can be only accessible in 1D CDW materials, in agreement with the authors’ density functional theory calculation. This work thus reveals the pivotal role of dimensionality in CDW phase transition and paves a way for implementing highly sensitive broadband photodetector.

Multiple Electronic Phases Coexisting under Inhomogeneous Strains in the Correlated Insulator.

Monolayer transition metal dichalcogenides (TMDs) can host exotic phenomena such as correlated insulating and charge-density-wave (CDW) phases. Such properties are strongly dependent on the precise atomic arrangements. Strain, as an effective tuning parameter in atomic arrangements, has been widely used for tailoring material's structures and related properties, yet to date, a convincing demonstration of strain-induced dedicate phase transition at nanometer scale in monolayer TMDs has been lacking. Here, a strain engineering technique is developed to controllably introduce out-of-plane atomic deformations in monolayer CDW material 1T-NbSe2 . The scanning tunneling microscopy and spectroscopy (STM and STS) measurements, accompanied by first-principles calculations, demonstrate that the CDW phase of 1T-NbSe2 can survive under both tensile and compressive strains even up to 5%. Moreover, significant strain-induced phase transitions are observed, i.e., tensile (compressive) strains can drive 1T-NbSe2 from an intrinsic-correlated insulator into a band insulator (metal). Furthermore, experimental evidence of the multiple electronic phase coexistence at the nanoscale is provided. The results shed new lights on the strain engineering of correlated insulator and useful for design and development of strain-related nanodevices.

Origin of Immediate Damping of Coherent Oscillations in Photoinduced Charge-Density-Wave Transition

In stark contrast to the conventional charge density wave (CDW) materials, the one-dimensional CDW on the In/Si(111) surface exhibits immediate damping of the CDW oscillation during the photoinduced phase transition. Here, we successfully reproduce the experimental observation of the photoinduced CDW transition on the In/Si(111) surface by performing real-time time-dependent density functional theory (rt-TDDFT) simulations. We show that photoexcitation promotes valence electrons from the Si substrate to the empty surface bands composed primarily of the covalent p-p bonding states of the long In-In bonds. Such photoexcitation generates interatomic forces to shorten the long In-In bonds and thus drives the structural transition. After the structural transition, these surface bands undergo a switch among different In-In bonds, causing a rotation of the interatomic forces by about π/6 and thus quickly damping the oscillations in feature CDW modes. These findings provide a deeper understanding of photoinduced phase transitions.

Experimental and Theoretical Studies of the Surface Oxidation Process of Rare‐Earth Tritellurides

AbstractRecent studies have established Van der Waals (vdW) layered and 2D rare‐earth tritellurides (RTe3) as superconductors and near room‐temperature charge density wave (CDW) materials. Their environmental stability raises natural concern owing to aging/stability effects observed in other tellurium‐based layered crystals. Here, the results establish the stability and environmental aging characteristics of these RTe3 systems involving a variety of metals such as La, Nd, Sm, Gd, Dy, and Ho. The atomic force microscopy (AFM) and scanning electron microscopy (SEM) results show that all the RTe3 sheets oxidize to form thin TeOx layers that are primarily confined to the surface, edges, and grain boundaries. Time‐resolved in situ Raman spectroscopy measurements are used to understand the kinetics of the oxidization process for different lanthanide metal cations and establish their relative stability/resilience to oxidization. Overall results indicate that the vdW layers show higher air stability as the 4f electron number decreases going from Ho to La, resulting in the most stable LaTe3 compared to the least stable HoTe3. Comprehensive quantum mechanical simulations reveal that environmental degradation originates from a strong oxidizing reaction with O2 molecules, while humidity (H2O) plays a negligible role unless Te vacancies are present. Moreover, the simulations explain the effects of 4f electrons on the work function and Te vacancies formation, which directly impact the aging characteristics of RTe3 layers. Interestingly, optical and electrical measurements show that the CDW response is still observed in aged RTe3 layers owing to the presence of underlying pristine/nonoxidized RTe3 layers, except CDW transition temperatures increase due to the thickness effect. Overall results offer the first in‐depth environmental aging studies on these materials, which can be applied to engineer and design their chemical stability, surface properties, and overall CDW characteristics.

Unveiling Electronic Behaviors in Heterochiral Charge-Density-Wave Twisted Stacking Materials with 1.25 nm Unit Dependence.

Layered charge-density-wave (CDW) materials have gained increasing interest due to their CDW stacking-dependent electronic properties for practical applications. Among the large family of CDW materials, those with star of David (SOD) patterns are very important due to the potentials for quantum spin liquid and related device applications. However, the spatial extension and the spin coupling information down to the nanoscale remain elusive. Here, we report the study of heterochiral CDW stackings in bilayer (BL) NbSe2 with high spatial resolution. We reveal that there exist well-defined heterochiral stackings, which have inhomogeneous electronic states among neighboring CDW units (star of David, SOD), significantly different from the homogeneous electronic states in the homochiral stackings. Intriguingly, the different electronic behaviors are spatially localized within each SOD with a unit size of 1.25 nm, and the gap sizes are determined by the different types of SOD stackings. Density functional theory (DFT) calculations match the experimental measurements well and reveal the SOD-stacking-dependent correlated electronic states and antiferromagnetic/ferromagnetic couplings. Our findings give a deep understanding of the spatial distribution of interlayer stacking and the delicate modulation of the spintronic states, which is very helpful for CDW-based nanoelectronic devices.

Superconductivity in single-crystalline ZrTe3-x (x ≤ 0.5) nanoplates.

Superconductivity with an unusual filamented character below 2 K has been reported in bulk ZrTe3 crystals, a well-known charge density wave (CDW) material, but still lacks in its nanostructures. Here, we systemically investigated the transport properties of controllable chemical vapor transport synthesized ZrTe3-x nanoplates. Intriguingly, superconducting behavior is found at T c = 3.4 K and can be understood by the suppression of CDW due to the atomic disorder formed by Te vacancies. Magnetic field and angle dependent upper critical field revealed that the superconductivity in the nanoplates exhibits a large anisotropy and two-dimensional character. This two-dimensional nature of superconductivity was further satisfactorily described using the Berezinsky-Kosterlitz-Thouless transition. Our results not only demonstrate the critical role of Te vacancies for superconductivity in ZrTe3-x nanoplates, but also provide a promising platform to explore the exotic physics in the nanostructure devices.