Charge Density Wave Phase Research Articles

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.

Nontrivial topological properties in two-dimensional half-Heusler compounds

With the experimental synthesis of two-dimensional (2D) half-Heusler compounds, the need for comprehensive investigations of their material properties is rising. Using exhaustive materials search through first-principles computations, we explore the structural stability, electronic, and topological properties of 60 monolayer half-Heusler compounds with a chemical formula of ABX (A = Li, Na, K, Rb, or Cs; B = Be, Mg, Ca, Sr, Ba, or Zn; X = Sb or Bi) under the P4/nmm crystal structure. Regarding stability, three structural configurations were examined, namely pristine (d0), one-sided distortion (d1), and two-sided distortion (d2). Interestingly, 6 compounds exhibit nontrivial topological properties as confirmed by the calculated Z2 invariant under the hybrid functional approach, with RbBeBi having the largest system bandgap of 0.217 eV. Orbital analyses show that the band inversion along the Γ-point was driven by the s-orbital of the B element and the px+py-orbital of the X element. The calculated edge states also manifest gapless states, thus further confirming the topological insulating phase. Additionally, we conjecture that the monolayer RbBeBi may exhibit the charge density wave (CDW) phase as a consequence of periodic lattice distortion. Our research identifies a new 2D material family derived from the bulk half-Heusler possessing various stable distortions for the development of 2D topological materials platforms, paving the way for discovering 2D topological materials for future technological applications.

A hybrid quantum-classical method for electron-phonon systems

Interactions between electrons and phonons play a crucial role in quantum materials. Yet, there is no universal method that would simultaneously accurately account for strong electron-phonon interactions and electronic correlations. By combining methods of the variational quantum eigensolver and the variational non-Gaussian solver, we develop a hybrid quantum-classical algorithm suitable for this type of correlated systems. This hybrid method tackles systems with arbitrarily strong electron-phonon coupling without increasing the number of required qubits and quantum gates, as compared to purely electronic models. We benchmark our method by applying it to the paradigmatic Hubbard-Holstein model at half filling, and show that it correctly captures the competition between charge density wave and antiferromagnetic phases, quantitatively consistent with exact diagonalization.

Chiral-Flux-Phase-Based Topological Superconductivity in Kagome Systems with Mixed Edge Chiralities.

Recent studies have attracted intense attention on the quasi-2D kagome superconductors AV_{3}Sb_{5} (A=K, Rb, and Cs) where the unexpected chiral flux phase (CFP) associates with the spontaneous time-reversal symmetry breaking in charge density wave states. Here, commencing from the 2-by-2 charge density wave phases, we bridge the gap between topological superconductivity and time-reversal asymmetric CFP in kagome systems. Several chiral topological superconductor (TSC) states featuring distinct Chern numbers emerge for an s-wave or a d-wave superconducting pairing symmetry. Importantly, these CFP-based TSC phases possess unique gapless edge modes with mixed chiralities (i.e., both positive and negative chiralities), but with the net chiralities consistent with the Bogoliubov-de Gennes Chern numbers. We further study the transport properties of a two-terminal junction, using Chern insulator or normal metal leads via atomic Green's function method with Landauer-Büttiker formalism. In both cases, the normal electron tunneling and the crossed Andreev reflection oscillate as the chemical potential changes, but together contribute to plateau transmissions (1 and 3/2, respectively) that exhibit robustness against disorder. These behaviors can be regarded as the signature of a TSC hosting edge states with mixed chiralities.

Q-dependent electron-phonon coupling induced phonon softening and non-conventional critical behavior in the CDW superconductor LaPt2Si2

This paper reports the first experimental observation of phonons and their softening on single crystalline LaPt2Si2 via inelastic neutron scattering. From the temperature dependence of the phonon frequency in close proximity to the charge density wave (CDW) q-vector, we obtain a CDW transition temperature of TCDW = 230 K and a critical exponent β = 0.28 ± 0.03. This value is suggestive of a non-conventional critical behavior for the CDW phase transition in LaPt2Si2, compatible with a scenario of CDW discommensuration (DC). The DC would be caused by the existence of two CDWs in this material, propagating separately in the non equivalent (Si1–Pt2–Si1) and (Pt1–Si2–Pt1) layers, respectively, with transition temperatures TCDW−1 = 230 K and TCDW−2 = 110 K. A strong q-dependence of the electron-phonon coupling has been identified as the driving mechanism for the CDW transition at TCDW−1 = 230 K while a CDW with 3-dimensional character, and Fermi surface quasi-nesting as a driving mechanism, is suggested for the transition at TCDW−2 = 110 K. Our results clarify some aspects of the CDW transition in LaPt2Si2 which have been so far misinterpreted by both theoretical predictions and experimental observations and give direct insight into its actual temperature dependence.

Alternative Structure Model of Correlated Charge Density Wave in Monolayer 1T-Nb(Ta)Se2.

The putative Mott charge density wave (CDW) phases of monolayer 1T-NbSe2 and 1T-TaSe2 have attracted a lot of recent interest due to the unexpected orbital texture of their Mott-Hubbard states and the superstructure related to an exotic possibility of a quantum spin liquid with a spinon Fermi surface. The origins of the orbital texture and the superstructure have been, however, elusive. We find by using density functional theory calculations that these CDW phases can have an alternative metastable structure, an anion (Se) centered cluster, in contrast to the prevailing model of a cation (Nb or Ta) centered David star cluster. This structure can be stabilized by the charge transfer from the bilayer graphene/SiC substrate used commonly in the experiments. The anion-centered structure has a similar electronic band structure of a charge transfer insulator to that of DS clusters but naturally explains the orbital texture of the upper Hubbard band from simply its atomic structure. Moreover, this band structure exhibits a Fermi surface nesting to possibly break the symmetry spontaneously into a -R30° superstructure observed experimentally. The resulting ground state of the superstructure is shown to be a trivial band insulator, in contrast to exotic proposals. This result emphasizes the huge structural flexibility of these heteroexpitaxial monolayers, for which careful studies on atomic structures and interactions with substrates are highly requested.

Emergent topological quantum orbits in the charge density wave phase of kagome metal CsV3Sb5

The recently discovered kagome materials AV3Sb5 (A = K, Rb, Cs) attract intense research interest in intertwined topology, superconductivity, and charge density waves (CDW). Although the in-plane 2 × 2 CDW is well studied, its out-of-plane structural correlation with the Fermi surface properties is less understood. In this work, we advance the theoretical description of quantum oscillations and investigate the Fermi surface properties in the three-dimensional CDW phase of CsV3Sb5. We derived Fermi-energy-resolved and layer-resolved quantum orbits that agree quantitatively with recent experiments in the fundamental frequency, cyclotron mass, and topology. We reveal a complex Dirac nodal network that would lead to a π Berry phase of a quantum orbit in the spinless case. However, the phase shift of topological quantum orbits is contributed by the orbital moment and Zeeman effect besides the Berry phase in the presence of spin-orbital coupling (SOC). Therefore, we can observe topological quantum orbits with a π phase shift in otherwise trivial orbits without SOC, contrary to common perception. Our work reveals the rich topological nature of kagome materials and paves a path to resolve different topological origins of quantum orbits.

Electronic dispersion, correlations and stacking in the photoexcited state of 1T-TaS2

Here we perform angle and time-resolved photoelectron spectroscopy on the commensurate charge density wave (CDW) phase of 1T-TaS2. Data with different probe pulse polarization are employed to map the dispersion of electronic states below and above the chemical potential. Upon photoexcitation, the fluctuations of CDW order erase the band dispersion and squeeze the electronic states near to the chemical potential. This transient phase sets within half a period of the coherent lattice motion and is favored by strong electronic correlations. The experimental results are compared to density-functional theory calculations with a self-consistent evaluation of the Coulomb repulsion. Our simulations indicate that the screening of Coulomb repulsion depends on the stacking order of the TaS2 layers. The entanglement of such degrees of freedom suggest that both the structural order and electronic repulsion are locally modified by the photoinduced CDW fluctuations.

Light-induced hexatic state in a layered quantum material

The tunability of materials properties by light promises a wealth of future applications in energy conversion and information technology. Strongly correlated materials such as transition metal dichalcogenides offer optical control of electronic phases, charge ordering and interlayer correlations by photodoping. Here, we find the emergence of a transient hexatic state during the laser-induced transformation between two charge-density wave phases in a thin-film transition metal dichalcogenide, 1T-type tantalum disulfide (1T-TaS2). Introducing tilt-series ultrafast nanobeam electron diffraction, we reconstruct charge-density wave rocking curves at high momentum resolution. An intermittent suppression of three-dimensional structural correlations promotes a loss of in-plane translational order caused by a high density of unbound topological defects, characteristic of a hexatic intermediate. Our results demonstrate the merit of tomographic ultrafast structural probing in tracing coupled order parameters, heralding universal nanoscale access to laser-induced dimensionality control in functional heterostructures and devices.

Excitation spectrum and momentum distribution of the ionic Bose–Hubbard model

We investigate the excitation spectrum and momentum distribution of the ionic Bose–Hubbard model by the standard basis operator method. We derive Green’s functions in the random phase approximation in Mott insulator, superfluid, charge density wave, and supersolid phases. The excitation spectrum has gapped modes and gapless Goldstone modes in the superfluid and supersolid phases. We show that the momentum distribution has a peak at the zone corner in the supersolid phase and the charge density wave phase close to the phase boundary. In addition, we demonstrate that the momentum distribution can be explained by the excitation spectrum and spectral weights of hole excitation modes.

Observation of Electronic Nematicity Driven by the Three-Dimensional Charge Density Wave in Kagome Lattice KV3Sb5.

Kagome superconductors AV3Sb5 (A = K, Rb, Cs) provide a fertile playground for studying intriguing phenomena, including nontrivial band topology, superconductivity, giant anomalous Hall effect, and charge density wave (CDW). Recently, a C2 symmetric nematic phase prior to the superconducting state in AV3Sb5 drew enormous attention due to its potential inheritance of the symmetry of the unusual superconductivity. However, direct evidence of the rotation symmetry breaking of the electronic structure in the CDW state from the reciprocal space is still rare, and the underlying mechanism remains ambiguous. The observation shows unconventional unidirectionality, indicative of rotation symmetry breaking from six-fold to two-fold. The interlayer coupling between adjacent planes with π-phase offset in the 2 × 2 × 2 CDW phase leads to the preferred two-fold symmetric electronic structure. These rarely observed unidirectional back-folded bands in KV3Sb5 may provide important insights into its peculiar charge order and superconductivity.

True First-Order Surface Phase Transition without Nanoscale Phase Separation.

Nanoscale phase separation is common in many materials ranging from correlated electron systems to semiconductor surfaces undergoing phase transitions. On solid surfaces, nanoscale phase separations are known to occur over an extended temperature range during temperature-driven first-order surface phase transitions, precluding the true first-order transitions in thermodynamics. Here, we report the case of a surface phase transition very close to a true first-order transition. An array of indium wires on Si(111) undergoes a first-order charge-density-wave (CDW) transition with surprisingly little or no phase separation when prepared free of indium adatom impurities. The lack of phase separation was attributed to the small difference in strain with the substrate between the two competing normal and CDW phases. Indium adatom impurities cause phase separation and blur the transition, making it gradual and incomplete. These experimental observations provide insight into the surface phase transition at the nanoscale level.

Phonon-induced instabilities in correlated electron Hamiltonians

Studies of Hamiltonians modeling the coupling between electrons as well as to local phonon excitations have been fundamental in capturing the novel ordering seen in many quasi-one dimensional condensed matter systems. Extending studies of such Hamiltonians to quasi-two dimensional systems is of great current interest, as electron-phonon couplings are predicted to play a major role in the stabilization or enhancement of novel phases in 2D material systems. In this work, we study model systems that describe the interplay between the Hubbard coupling and the phonon modes in the Holstein (H) and Su-Schrieffer-Heeger (SSH) Hamiltonians using the functional renormalization group (fRG). For both types of electron phonon couplings, we find the predicted charge density wave phases in competition with anti-ferromagnetic ($AF$) ordering. As the system is doped, the transition shifts, with both orders showing incommensurate peaks. We compare the evolution of the quasiparticle weight for the Holstein model with that of the SSH model as the systems transition from antiferromagnetic to charge-ordered ground states. Finally, we calculate the self-energy of the phonon and capture the impact of charge ordering on the phonon modes.

Controllable Synthesis and Charge Density Wave Phase Transitions of Two-Dimensional 1T-TaS2 Crystals.

1T-TaS2 has attracted much attention recently due to its abundant charge density wave phases. In this work, high-quality two-dimensional 1T-TaS2 crystals were successfully synthesized by a chemical vapor deposition method with controllable layer numbers, confirmed by the structural characterization. Based on the as-grown samples, their thickness-dependency nearly commensurate charge density wave/commensurate charge density wave phase transitions was revealed by the combination of the temperature-dependent resistance measurements and Raman spectra. The phase transition temperature increased with increasing thickness, but no apparent phase transition was found on the 2~3 nm thick crystals from temperature-dependent Raman spectra. The transition hysteresis loops due to temperature-dependent resistance changes of 1T-TaS2 can be used for memory devices and oscillators, making 1T-TaS2 a promising material for various electronic applications.

Doping evolution of superconductivity, charge order, and band topology in hole-doped topological kagome superconductors Cs(V1−xTix)3Sb5

The newly discovered kagome superconductors $A{\mathrm{V}}_{3}{\mathrm{Sb}}_{5}$ ($A=\mathrm{K}$, Rb, Cs) exhibit superconductivity, charge order, and band topology simultaneously. To explore the intricate interplay between the superconducting and charge-density-wave (CDW) orders, we investigate the doping evolution of underlying electronic structures in doped topological kagome superconductors $\mathrm{Cs}{({\mathrm{V}}_{1\ensuremath{-}x}{\mathrm{Ti}}_{x})}_{3}{\mathrm{Sb}}_{5}$ where the Ti dopant introduces hole-like charge carriers. Despite the absence of the CDW phase transition in doped compounds even for the lowest doping level of $x=0.047$, the superconductivity survives in all doped samples with enhanced critical temperatures. The high-resolution angle-resolved photoemission spectroscopy (ARPES) measurements reveal that the Ti dopant in the kagome plane lowers the chemical potential, pushing the van Hove singularity (VHS) at $M$ point above the Fermi level. First-principle simulations corroborate the doping evolution of the band structure observed in ARPES, and affirm that the CDW instability does not occur once the VHS moves above the Fermi level, explaining the absence of the CDW ordering in our doped samples $\mathrm{Cs}{({\mathrm{V}}_{1\ensuremath{-}x}{\mathrm{Ti}}_{x})}_{3}{\mathrm{Sb}}_{5}$. Our results also demonstrate a competition between the CDW and superconducting orders in the kagome-metal superconductor ${\mathrm{CsV}}_{3}{\mathrm{Sb}}_{5}$, although the superconductivity is likely inconsequential of the CDW order.

Carrier-Density Control of the Quantum-Confined 1T-TiSe_{2} Charge Density Wave.

Using angle-resolved photoemission spectroscopy, combined with first principle and coupled self-consistent Poisson-Schrödinger calculations, we demonstrate that potassium (K) atoms adsorbed on the low-temperature phase of 1T-TiSe_{2} induce the creation of a two-dimensional electron gas (2DEG) and quantum confinement of its charge-density wave (CDW) at the surface. By further changing the K coverage, we tune the carrier density within the 2DEG that allows us to nullify, at the surface, the electronic energy gain due to exciton condensation in the CDW phase while preserving a long-range structural order. Our Letter constitutes a prime example of a controlled exciton-related many-body quantum state in reduced dimensionality by alkali-metal dosing.

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.

Phase-resolved frequency-domain analysis of the photoemission spectra for photoexcited 1T-TaS2 in the Mott insulating charge density wave state

We investigate the nonequilibrium electronic structure of 1T-TaS2 by time- and angle-resolved photoemission spectroscopy. We observe that strong photoexcitation induces the collapse of the Mott gap, leading to the photo-induced metallic phase. It is also found that the oscillation of photoemission intensity occurs as a result of the excitations of coherent phonons corresponding to the amplitude mode of the charge density wave (CDW). To study the dynamical change in the band dispersions modulated by the CDW amplitude mode, we perform analyses by using frequency-domain angle-resolved photoemission spectroscopy (FDARPES). We find that two different peak structures exhibit anti-phase oscillation with respect to each other by retrieving the amplitude and phase parts of the FDARPES spectra. They are attributed to the minimum and maximum band positions in energy, where the single band is oscillating between them synchronizing with the CDW amplitude mode. We further find that the flatband constructed as a result of CDW band folding survives during the oscillation while the Mott gap is significantly reduced. Our results suggest the CDW phase is robust, and the lattice modulation corresponding to the CDW amplitude mode dynamically modulates the Mott gap.

Impact of Sb degrees of freedom on the charge density wave phase diagram of the kagome metal CsV3Sb5

Elucidating the microscopic mechanisms responsible for the charge density wave (CDW) instability of the AV$_3$Sb$_5$ (A=Cs, K, Rb) family of kagome metals is critical for understanding their unique properties, including superconductivity. In these compounds, distinct CDW phases with wave-vectors at the $M$ and $L$ points are energetically favorable, opening the possibility of tuning the type of CDW order by appropriate external parameters. Here, we shed light on the CDW landscape of CsV$_3$Sb$_5$ via a combination of first-principles calculations and phenomenology, which consists of extracting the coefficients of the CDW Landau free-energy expansion from density functional theory. We find that while the main structural distortions of the kagome lattice in the staggered tri-hexagonal CDW phase are along the nearest-neighbor V-V bonds, distortions associated with the Sb ions play a defining role in the energy gain in this and all other CDW states. Moreover, the coupling between ionic displacements from different unit cells is small, thus explaining the existence of multiple CDW instabilities with different modulations along the c-axis. We also investigate how pressure and temperature impact the CDW phase of CsV$_3$Sb$_5$. Increasing pressure does not change the staggered tri-hexagonal CDW ground state, even though the $M$-point CDW instability disappears before the $L$-point one, a behavior that we attribute to the large nonlinear coupling between the order parameters. Upon changing the temperature, we find a narrow regime in which another transition can take place, toward a tri-hexagonal Star-of-David CDW phase. We discuss the implications of our results by comparing them with experiments on this compound.

Structure of the kagome superconductor CsV3Sb5 in the charge density wave state

The structure of charge density wave states in AV$_3$Sb$_5$ (A = K, Rb, Cs) kagome superconductors remains elusive, with three possible $2a\times2a\times2c$ candidates: tri-hexagonal, star-of-David, and their mixture. In this study, we conducted a systematic first-principles investigation of the nuclear quadrupole resonance (NQR) and nuclear magnetic resonance (NMR) spectra for the $2a\times2a\times2c$ CsV$_3$Sb$_5$ structures. By comparing our simulations with experimental data, we have concluded that the NQR spectrum indicates the tri-hexagonal structure as the proper structure for CsV$_3$Sb$_5$ after its charge density wave phase transition. The NMR calculation results obtained from the tri-hexagonal structure are also consistent with the experimental data.