Charge Density Wave Transition Research Articles

Tuning charge density wave of kagome metal ScV6Sn6

Compounds with a kagome lattice exhibit intriguing properties and the charge density wave (CDW) adds an additional layer of interest to research on them. In this study, we investigate the temperature and magnetic field dependent electrical properties under a chemical substitution and hydrostatic pressure of ScV6Sn6, a non-magnetic CDW compound. Substituting 5% Cr at the V site or applying 1.5 GPa of pressure shifts the CDW from 92 K to ∼ 50 K. This shift is attributed to the movement of the imaginary phonon band, as revealed by the phonon dispersion relation. The longitudinal and Hall resistivities respond differently under these stimuli. The magnetoresistance (MR) retains its quasilinear behavior under pressure, but it becomes quadratic after Cr substitution. The anomalous Hall-like behavior of the parent compound persists up to the respective CDW transition under pressure, after which it decreases sharply. In contrast, the longitudinal and Hall resistivities of Cr substituted compounds follow a two-band model and originate from the multi carrier effect. These results clearly highlight the role of phonon contributions in the CDW transition and call for further investigation into the origin of the anomalous Hall-like behavior in the parent compound.

The competition between charge density wave and superconductivity in the kagome metal CsV3(Sb1-xPbx)5 single crystals

Kagome metal AV3Sb5 (A = K, Rb, Cs) has garnered considerable attention for its abundant exotic quantum phenomena and the special competitive relationship between charge density wave (CDW) and superconductivity (SC). In this work we explore the unconventional coupling between charge density wave and superconductivity by means of the substitutional doping of Pb atoms with Sb atoms. Microscopic characterization and performance tests provide valuable phase diagram information for CsV3(Sb1-xPbx)5. Upon Pb doping, a pronounced competition between the charge density wave transition temperature TCDW and the superconducting temperature Tc was observed. Analysis of changes in Debye temperature ΘD and lattice constant, it is shown that Pb doping affects atomic bonding and may strengthen the coupling between adjacent kagome layers to some extent. Furthermore, the small angular shift of the diffraction peak and increased full width at half maximum (FWHM) indicate that the doping causes crystal defects and distorts the crystal structure, which will change the charge density in the local area and may affect the superconductivity. This result further reveals a close correlation between the superconductivity of the system and the electronic structure of the kagome plane in the CsV3Sb5 system. Overall, our results suggest that the observed competition arises from the complex interplay of multiple factors.

Charge density waves tuned by biaxial tensile stress.

The precise arrangement and nature of atoms drive electronic phase transitions in condensed matter. To explore this tenuous link, we developed a true biaxial mechanical deformation device working at cryogenic temperatures, compatible with x-ray diffraction and transport measurements, well adapted to layered samples. Here we show that a slight deformation of TbTe3 can have a dramatic influence on its Charge Density Wave (CDW), with an orientational transition from c to a driven by the a/c parameter, a tiny coexistence region near a = c, and without space group change. The CDW transition temperature Tc displays a linear dependence with while the gap saturates out of the coexistence region. This behaviour is well accounted for within a tight-binding model. Our results question the relationship between gap and Tc in RTe3 systems. This method opens a new route towards the study of coexisting or competing electronic orders in condensed matter.

An advanced high-rate capability sodium-ion anode: Few-layered NbSe2 with a mechanism of parallel running intercalation and conversion

The unique superconductivity and charge density wave transition characteristics of NbSe2 make it worthy of exploring its electrochemical performance and potential applications in the field of batteries. Herein, the bulk NbSe2 was successfully exfoliated into few-layered NbSe2 nanostructures by wet grinding exfoliation approach, which solved the issues of its long activation period and poor cycle stability. The strong Nb-Se bond in the plane and weak van der Waals force between the adjacent layers could render the fast Na+ diffusion, provide abundant reaction sites and multi-directional migration paths, thus accelerate the ionic conductivity. The theoretical calculations verified the high Na+ adsorption tendency between the NbSe2 interlayers stemming from the continuous region of charge accumulation. Thanks to the unique electronic and two-dimensional few-layered structures, the exfoliated NbSe2 exhibited a high cyclic stability with a capacity of 502 mA h g−1 over 2800 cycles at 10 A/g. In addition, the reaction mechanism was studied by in-situ X-ray diffraction and other tests, indicating a reaction mechanism containing of simultaneous intercalation (NbSe2↔NaxNbSe2↔NaNbSe2↔Na1+xNbSe2) and conversion processes in NbSe2. This parallelly running mechanism not only alleviates the volume change but also ensures a high specific capacity. Additionally, different lattice planes of the NaNbSe2 intermediate in the intercalation process experience varying degrees of contraction and expanding in d-spacing due to the influence of Coulombic force.

Anharmonic strong-coupling effects at the origin of the charge density wave in CsV3Sb5

The formation of charge density waves is a long-standing open problem, particularly in dimensions higher than one. Various observations in the vanadium antimonides discovered recently further underpin this notion. Here, we study the Kagome metal CsV3Sb5 using polarized inelastic light scattering and density functional theory calculations. We observe a significant gap anisotropy with 2Δmax/kBTCDW≈20\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$2{\\Delta }_{\\max }/{k}_{{{{{{{{\\rm{B}}}}}}}}}{T}_{{{{{{{{\\rm{CDW}}}}}}}}}\\, \\approx \\, 20$$\\end{document}, far beyond the prediction of mean-field theory. The analysis of the A1g and E2g phonons, including those emerging below TCDW, indicates strong phonon-phonon coupling, presumably mediated by a strong electron-phonon interaction. Similarly, the asymmetric Fano-type lineshape of the A1g amplitude mode suggests strong electron-phonon coupling below TCDW. The large electronic gap, the enhanced anharmonic phonon-phonon coupling, and the Fano shape of the amplitude mode combined are more supportive of a strong-coupling phonon-driven charge density wave transition than of a Fermi surface instability or an exotic mechanism in CsV3Sb5.

NMR study of charge density wave phase in the kagome metal RbV3Sb5

The mechanism of charge-density-wave (CDW) phase in one-dimensional lattices can be well described in theory. Whether similar mechanism works in two-dimensional systems is still a mystery. In this work, we employed 51V solid-state nuclear magnetic resonance (NMR) spectroscopy combined with first-principles computations to probe atomic structure and electronic properties at V sites in a quasi-two-dimensional crystal RbV3Sb5. Clear evidence of the CDW phase transition was observed from the temperature-dependent 51V NMR measurements. The sharp transition of 51V Knight shifts and electric field gradients (EFG) across the CDW transition supports the view that energy gap is formed by the nesting of partial Fermi surface in accompany with the superlattice formation. The calculated EFG parameters were also compared with our experiments, and the results suggest that the charge modulation of the CDW order is inverse Star-of-David pattern.

Ab initio electron-lattice downfolding: Potential energy landscapes, anharmonicity, and molecular dynamics in charge density wave materials

The interplay of electronic and nuclear degrees of freedom presents an outstanding problem in condensed matter physics and chemistry. Computational challenges arise especially for large systems, long time scales, in nonequilibrium, or in systems with strong correlations. In this work, we show how downfolding approaches facilitate complexity reduction on the electronic side and thereby boost the simulation of electronic properties and nuclear motion-in particular molecular dynamics (MD) simulations. Three different downfolding strategies based on constraining, unscreening, and combinations thereof are benchmarked against full density functional calculations for selected charge density wave (CDW) systems, namely 1H-TaS_22, 1T-TiSe_22, 1H-NbS_22, and a one-dimensional carbon chain. We find that the downfolded models can reproduce potential energy surfaces on supercells accurately and facilitate computational speedup in MD simulations by about five orders of magnitude in comparison to purely ab initio calculations. For monolayer 1H-TaS_22 we report classical and path integral replica exchange MD simulations, revealing the impact of thermal and quantum fluctuations on the CDW transition.

Resonant x-ray diffraction measurements in charge ordered kagome superconductors KV3Sb5 and RbV3Sb5

We report on (resonant) x-ray diffraction experiments on the normal state properties of kagome-lattice superconductors KV3Sb5 and RbV3Sb5. We have confirmed previous reports indicating that the charge density wave (CDW) phase is characterized by a doubling of the unit cell in all three crystallographic directions. By monitoring the temperature dependence of Bragg peaks associated with the CDW phase, we ascertained that it develops gradually over several degrees, as opposed to CsV3Sb5, where the CDW peak intensity saturates promptly just below the CDW transition temperature. Analysis of symmetry modes indicates that this behavior arises due to lattice distortions linked to the formation of CDWs. These distortions occur abruptly in CsV3Sb5, while they progress more gradually in RbV3Sb5 and KV3Sb5. In contrast, the amplitude of the mode leading to the crystallographic symmetry breaking from P6/mmm to Fmmm appears to develop more gradually in CsV3Sb5 as well. Diffraction measurements close to the V K edge and the Sb L1 edge show no sensitivity to inversion- or time-symmetry breaking, which are claimed to be associated with the onset of the CDW phase. The azimuthal angle dependence of the resonant diffraction intensity observed at the Sb L1 edge is associated with the difference in the population of unoccupied states and the anisotropy of the electron density of certain Sb ions.

Predicted multiple charge density wave phases in monolayer 1T-NbO2

Layered transition-metal dichalcogenides, such as NbSe2, have been extensively studied for almost half a century due to their intriguing properties, such as charge density wave (CDW) and superconductivity. Can the layered transition-metal dioxide, such as NbO2, be stable and exhibit CDW, given that it has the same crystal structure and electronic configuration as NbSe2? Here, we use first-principles calculations to predict that 1T-NbO2 is possibly stable at high temperatures, but it would undergo two CDW transitions with 12×12 and 13×13 periodicities at low temperatures. Both CDW transitions are accompanied by a metal-semiconductor transition. Notably, the 13×13 CDW phase of NbO2 possesses localized magnetic moments and hosts a Mott insulating state. This work offers a fresh outlook on studying CDW and Mott transition in low-dimensional oxide materials.

Experimental Investigation of Superconductivity in PdSSe Under High Pressure

AbstractAnalysis of the superconducting properties of transition metal dichalcogenides (TMDs) under high pressures offers valuable insights to guide the design and synthesis of high‐performance superconducting materials. Herein, the effect of pressure is investigated on the superconductivity of a typical van der Waals layered TMDs material, PdSSe, by measuring its transport properties. After initially increased pressure, superconductivity emerges at 10.2 GPa, with a critical superconducting temperature (Tc) of ≈5.1 K, accompanied by the diminishing charge density wave (CDW) that is originally strengthening. Then, the Tc gradually increases with increasing pressure, reaching 12.1 K at the maximum pressure. The study provides experimental evidence for the superconductivity of PdSSe, and to the best of the knowledge, this is the first report on the observation of amplified CDW phenomena under increasing pressure in nonmagnetic TMDs. The abnormal enhancement of CDW transition temperature at low pressure is consistent with the upward trend of resistance, which is related to the electron–electron interaction. Moreover, synchrotron X‐ray diffraction experiments reveal two additional structural phase transitions.

Charge-density wave mediated quasi-one-dimensional Kondo lattice in stripe-phase monolayer 1T-NbSe2

The heavy fermion physics is dictated by subtle competing exchange interactions, posing a challenge to their understanding. One-dimensional (1D) Kondo lattice model has attracted special attention in theory, because of its exact solvability and expected unusual quantum criticality. However, such experimental material systems are extremely rare. Here, we demonstrate the realization of quasi-1D Kondo lattice behavior in a monolayer van der Waals crystal NbSe2, that is driven into a stripe phase via Se-deficient line defects. Spectroscopic imaging scanning tunneling microscopy measurements and first-principles calculations indicate that the stripe-phase NbSe2 undergoes a novel charge-density wave transition, creating a matrix of local magnetic moments. The Kondo lattice behavior is manifested as a Fano resonance at the Fermi energy that prevails the entire film with a high Kondo temperature. Importantly, coherent Kondo screening occurs only in the direction of the stripes. Upon approaching defects, the Fano resonance exhibits prominent spatial 1D oscillations along the stripe direction, reminiscent of Kondo holes in a quasi-1D Kondo lattice. Our findings provide a platform for exploring anisotropic Kondo lattice behavior in the monolayer limit.

Polymorphism in the Ruddlesden-Popper Nickelate La3Ni2O7: Discovery of a Hidden Phase with Distinctive Layer Stacking.

We report the discovery of a novel form of Ruddlesden-Popper (RP) nickelate that stands as the first example of long-range, coherent polymorphism in this class of inorganic solids. Rather than the well-known, uniform stacking of perovskite blocks ubiquitously found in RP phases, this newly discovered polymorph of the bilayer RP phase La3Ni2O7 adopts a novel stacking sequence in which single-layer and trilayer blocks of NiO6 octahedra alternate in a "1313" sequence. Crystals of this new polymorph are described in space group Cmmm, although we note evidence for a competing Imam variant. Transport measurements at ambient pressure reveal metallic character with evidence of a charge density wave transition with an onset at T ≈ 134 K. The discovery of such polymorphism could reverberate to the expansive range of science and applications that rely on RP materials, particularly the recently reported signatures of superconductivity in bilayer La3Ni2O7 with Tc as high as 80 K above 14 GPa.

Chirality manipulation of ultrafast phase switches in a correlated CDW-Weyl semimetal

Light engineering of correlated states in topological materials provides a new avenue of achieving exotic topological phases inaccessible by conventional tuning methods. Here we demonstrate a light control of correlation gaps in a model charge-density-wave (CDW) and polaron insulator (TaSe4)2I recently predicted to be an axion insulator. Our ultrafast terahertz photocurrent spectroscopy reveals a two-step, non-thermal melting of polarons and electronic CDW gap via the fluence dependence of a longitudinal circular photogalvanic current. This helicity-dependent photocurrent reveals continuous ultrafast phase switches from the polaronic state to the CDW (axion) phase, and finally to a hidden Weyl phase as the pump fluence increases. Additional distinctive attributes aligning with the light-induced switches include: the mode-selective coupling of coherent phonons to the polaron and CDW modulation, and the emergence of a non-thermal chiral photocurrent above the pump threshold of CDW-related phonons. The demonstrated ultrafast chirality control of correlated topological states here holds large potentials for realizing axion electrodynamics and advancing quantum-computing applications.

Alloying effect of rare-earth tritellurides on the charge density wave and magnetic properties

Among many van der Waals materials rare-earth tritellurides (RTe3) allow studying several phenomena like magnetic, superconducting, and charge density wave (CDW). These studies show the effect of cationic alloying of antiferromagnetic RTe3 for fully tunable near room-temperature CDW properties. DyxGd1−xTe3 and DyxTb1−xTe3 alloys were synthesized through a chemical vapor transport technique, and the rare-earth element composition was controlled by changing the ratio of rare-earth metal reagents. The results show that the lattice parameters can be continuously tuned with the composition of the rare-earth cations leading to the variation of the internal chemical pressure. Temperature-dependent Raman spectroscopy and electric transport measurement show that the CDW transition temperature (TCDW) of RTe3 alloys varies with lattice parameters/chemical pressure spanning across 300–380 K. Additional magnetism studies offer the first insights into the magnetic ordering in RTe3 alloys. The emergence of multiple magnetic transitions implies complex magnetic interactions that arise from interactions between different rare-earth elements. Overall findings introduce ways to control the CDW behavior and provide valuable insights into the magnetic ordering in RTe3 alloys, contributing to further investigation and a better understanding of their properties.

Pressure Dependence of the Structural and Superconducting Properties of the Bi-Based Superconductor Bi2Pd3Se2.

The structural and superconducting properties of the Bi-based compound Bi2Pd3Se2 were investigated over a wide pressure range. The prepared Bi2Pd3Se2 sample was a superconductor with a superconducting transition temperature, Tc, of approximately 3.0 K, which differed from a previous report (Tc of less than 1.0 K). At ambient pressure, the powder X-ray diffraction (XRD) pattern of the Bi2Pd3Se2 sample was consistent with that previously reported for Bi2Pd3Se2. The Rietveld method was used to refine the crystal structure, which had a space group of C2/m (No. 12), as reported previously. This compound showed no clear anomaly due to the charge-density-wave (CDW) transition, as seen from the temperature dependence of magnetic susceptibility. However, the temperature dependence of electrical resistivity indicated a clear anomaly, presumably because of the CDW transition in the low-pressure range; the CDW transition temperature was approximately 230 K. The XRD patterns of the Bi2Pd3Se2 sample were measured at 0.160-22.7 GPa, and the patterns were well analyzed by both the Le Bail and Rietveld refinement methods, showing no structural phase transitions in the above pressure range. The pressure dependence of Tc of Bi2Pd3Se2 was recorded based on the temperature dependence of the electrical resistance, which showed an almost constant Tc at 0-13.7 GPa, and the Tc-pressure (p) behavior was fully discussed.

Unconventional Charge-Density-Wave Gap in Monolayer NbS2.

Using scanning tunneling microscopy and spectroscopy, for a monolayer of transition metal dichalcogenide H-NbS2 grown by molecular beam epitaxy on graphene, we provide unambiguous evidence for a charge density wave (CDW) with a 3 × 3 superstructure, which is not present in bulk NbS2. Local spectroscopy displays a pronounced gap on the order of 20 meV at the Fermi level. Within the gap, low-energy features are present. The gap structure with its low-energy features is at variance with the expectation for a gap opening in the electronic band structure due to a CDW. Instead, comparison with ab initio calculations indicates that the observed gap structure must be attributed to combined electron-phonon quasiparticles. The phonons in question are the elusive amplitude and phase collective modes of the CDW transition. Our findings advance the understanding of CDW mechanisms in 2D materials and their spectroscopic signatures.

Controlling the Charge Density Wave Transition in Single-Layer TiTe2xSe2(1-x) Alloys by Band Gap Engineering.

Closing the band gap of a semiconductor into a semimetallic state gives a powerful potential route to tune the electronic energy gains that drive collective phases like charge density waves (CDWs) and excitonic insulator states. We explore this approach for the controversial CDW material monolayer (ML) TiSe2 by engineering its narrow band gap to the semimetallic limit of ML-TiTe2. Using molecular beam epitaxy, we demonstrate the growth of ML-TiTe2xSe2(1-x) alloys across the entire compositional range and unveil how the (2 × 2) CDW instability evolves through the normal state semiconductor-semimetal transition via in situ angle-resolved photoemission spectroscopy. Through model electronic structure calculations, we identify how this tunes the relative strength of excitonic and Peierls-like coupling, demonstrating band gap engineering as a powerful method for controlling the microscopic mechanisms underpinning the formation of collective states in two-dimensional materials.

Dynamics and resilience of the unconventional charge density wave in ScV6Sn6 bilayer kagome metal

Long-range electronic ordering descending from a metallic parent state constitutes a rich playground to study the interplay of structural and electronic degrees of freedom. In this framework, kagome metals are in the most interesting regime where both phonon and electronically mediated couplings are significant. Several of these systems undergo a charge density wave transition. However, to date, the origin and the main driving force behind this charge order is elusive. Here, we use the kagome metal ScV6Sn6 as a platform to investigate this problem, since it features both a kagome-derived nested Fermi surface and van-Hove singularities near the Fermi level, and a charge-ordered phase that strongly affects its physical properties. By combining time-resolved reflectivity, first principles calculations and photo-emission experiments, we identify the structural degrees of freedom to play a fundamental role in the stabilization of charge order, indicating that ScV6Sn6 features an instance of charge order predominantly originating from phonons.

Deconfined criticalities and dualities between chiral spin liquid, topological superconductor and charge density wave Chern insulator

We propose bi-critical and tri-critical theories between chiral spin liquid (CSL), topological superconductor (SC) and charge density wave (CDW) ordered Chern insulator with Chern number C=2C=2 on square, triangular and Kagome lattices. The three CDW order parameters form a manifold of S^2S2 or S^1S1 depending on whether there is easy-plane anisotropy. The skyrmion defect of the CDW order carries physical charge 2e2e and its condensation leads to a topological superconductor. The CDW-SC transitions are in the same universality classes as the celebrated deconfined quantum critical points (DQCP) between Neel order and valence bond solid order on square lattice. Both SC and CDW order can be accessed from the CSL phase through a continuous phase transition. At the CSL-SC transition, there is still CDW order fluctuations although CDW is absent in both sides. We propose three different theories for the CSL-SC transition (and CSL to easy-plane CDW transition): a U(1)U(1) theory with two bosons, a U(1)U(1) theory with two Dirac fermions, and an SU(2)SU(2) theory with two bosons. Our construction offers a derivation of the duality between these three theories as well as a promising physical realization. The SU(2)SU(2) theory offers a unified framework for a series of fixed points with explicit SO(5), O(4)SO(5),O(4) or SO(3)× O(2)SO(3)×O(2) symmetry. There is also a transparent duality transformation mapping SC order to easy-plane CDW order. The CSL-SC-CDW tri-critical points are invariant under this duality mapping and have an enlarged SO(5)SO(5) or O(4)O(4) symmetry. The DQCPs between CDW and SC inherit the enlarged symmetry, emergent anomaly, and self-duality from the tri-critical point. Our analysis unifies the well-studied DQCP between symmetry breaking phases into a larger framework where they are proximate to a topologically ordered phase. Experimentally the theory demonstrates the possibility of a rich phase diagram and criticality through closing the Mott gap of a quantum spin liquid with projective symmetry group.

Surface properties of 1T-TaS2 and contrasting its electron-phonon coupling with TlBiTe2 from helium atom scattering.

We present a detailed helium atom scattering study of the charge-density wave (CDW) system and transition metal dichalcogenide 1T-TaS2. In terms of energy dissipation, we determine the electron-phonon (e-ph) coupling, a quantity that is at the heart of conventional superconductivity and may even "drive" phase transitions such as CDWs. The e-ph coupling of TaS2 in the commensurate CDW phase (λ = 0.59 ± 0.12) is compared with measurements of the topo-logical insulator TlBiTe2 (λ = 0.09 ± 0.01). Furthermore, by means of elastic He diffraction and resonance/interference effects in He scattering, the thermal expansion of the surface lattice, the surface step height, and the three-dimensional atom-surface interaction potential are determined including the electronic corrugation of 1T-TaS2. The linear thermal expansion coefficient is similar to that of other transition-metal dichalcogenides. The He-TaS2 interaction is best described by a corrugated Morse potential with a relatively large well depth and supports a large number of bound states, comparable to the surface of Bi2Se3, and the surface electronic corrugation of 1T-TaS2 is similar to the ones found for semimetal surfaces.