Charge Density Wave Gap 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.

Imaging momentum-space Cooper pair formation and its competition with the charge density wave gap in a kagome superconductor

Imaging momentum-space Cooper pair formation and its competition with the charge density wave gap in a kagome superconductor

Plasmon Excitations across the Charge-Density-Wave Transition in Single-Layer TiSe2.

1T-TiSe2 is believed to possess a soft electronic mode, i.e., plasmon or exciton, that might be responsible for the exciton condensation and charge-density-wave (CDW) transition. Here, we explore collective electronic excitations in single-layer 1T-TiSe2 by using the ab initio electromagnetic linear response and unveil intricate scattering pathways of the two-dimensional (2D) plasmon mode near the CDW phase. We found the dominant role of plasmon-phonon scattering, which in combination with the CDW gap excitations leads to the anomalous temperature dependence of the plasmon line width across the CDW transition. Below the transition temperature TCDW a strong hybridization between the 2D plasmon and CDW excitations is obtained. These optical features are highly tunable due to temperature-dependent CDW-related modifications of electronic structure and electron-phonon coupling and make CDW-bearing systems potentially interesting for applications in optoelectronics and low-loss plasmonics.

Coexistence of Interacting Charge Density Waves in a Layered Semiconductor.

Coexisting orders are key features of strongly correlated materials and underlie many intriguing phenomena from unconventional superconductivity to topological orders. Here, we report the coexistence of two interacting charge-density-wave (CDW) orders in EuTe_{4}, a layered crystal that has drawn considerable attention owing to its anomalous thermal hysteresis and a semiconducting CDW state despite the absence of perfect Fermi surface nesting. By accessing unoccupied conduction bands with time- and angle-resolved photoemission measurements, we find that monolayers and bilayers of Te in the unit cell host different CDWs that are associated with distinct energy gaps. The two gaps display dichotomous evolutions following photoexcitation, where the larger bilayer CDW gap exhibits less renormalization and faster recovery. Surprisingly, the CDW in the Te monolayer displays an additional momentum-dependent gap renormalization that cannot be captured by density-functional theory calculations. This phenomenon is attributed to interlayer interactions between the two CDW orders, which account for the semiconducting nature of the equilibrium state. Our findings not only offer microscopic insights into the correlated ground state of EuTe_{4} but also provide a general nonequilibrium approach to understand coexisting, layer-dependent orders in a complex system.

Dual quantum spin Hall insulator by density-tuned correlations in TaIrTe4.

The convergence of topology and correlations represents a highly coveted realm in the pursuit of new quantum states of matter1. Introducing electron correlations to a quantum spin Hall (QSH) insulator can lead to the emergence of a fractional topological insulator and other exotic time-reversal-symmetric topological order2-8, not possible in quantum Hall and Chern insulator systems. Here we report a new dual QSH insulator within the intrinsic monolayer crystal of TaIrTe4, arising from the interplay of its single-particle topology and density-tuned electron correlations. At charge neutrality, monolayer TaIrTe4 demonstrates the QSH insulator, manifesting enhanced nonlocal transport and quantized helical edge conductance. After introducing electrons from charge neutrality, TaIrTe4 shows metallic behaviour in onlya small range of charge densities but quickly goes into a new insulating state, entirely unexpected on the basis of the single-particle band structure of TaIrTe4. This insulating state could arise from a strong electronic instability near the van Hove singularities, probably leading to a charge density wave (CDW). Remarkably, within this correlated insulating gap, we observe a resurgence of the QSH state. The observation of helical edge conduction in a CDW gap could bridge spin physics and charge orders. The discovery of a dual QSH insulator introduces a new method for creating topological flat minibands through CDW superlattices, which offer a promising platform for exploring time-reversal-symmetric fractional phases and electromagnetism2-4,9,10.

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.

Melting of Unidirectional Charge Density Waves across Twin Domain Boundaries in GdTe3.

Solids undergoing a transition from order to disorder experience a proliferation of topological defects. The melting process generates transient quantum states. However, their dynamic nature with a femtosecond lifetime hinders exploration with atomic precision. Here, we suggest an alternative approach to the dynamic melting process by focusing on the interface created by competing degenerate quantum states. We use a scanning tunneling microscope (STM) to visualize the unidirectional charge density wave (CDW) and its spatial progression ("static melting") across a twin domain boundary (TDB) in the layered material GdTe3. Combining the STM with a spatial lock-in technique, we reveal that the order parameter amplitude attenuates with the formation of dislocations and thus two different unidirectional CDWs coexist near the TDB, reducing the CDW anisotropy. Notably, we discovered a correlation between this anisotropy and the CDW gap. Our study provides valuable insight into the behavior of topological defects and transient quantum states.

Comparison of tunneling spectra for normal and charge density wave states in 1T-TiSe2

The tunneling spectrum of 1T-TiSe2 in the charge density wave (CDW) state shows a dip structure below the Fermi level, and it is unclear whether this dip is a CDW gap. Answering this question is important because information regarding the CDW gap estimated from the dip is referred in discussions of the driving mechanism of this CDW. Therefore, we used scanning tunneling microscopy/scanning tunneling spectroscopy to acquire tunneling spectra for the normal and CDW states in TiSe2 and compared the spectra. Specifically, we measured pure TiSe2 at 293 K (>TCDW) and 4.2 K (<TCDW) and annealed TiSe2, in which the CDW is suppressed. As a result, we found that the tunneling spectra for the normal states exhibit a dip below the Fermi level similar to the spectrum for the CDW state. These results indicate that the dip itself is not a CDW gap.

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.

Electronic correlations and evolution of the charge density wave in the kagome metals AV3Sb5 (A=K,Rb,Cs)

The kagome metals $A$V$_{3}$Sb$_{5}$ ($A$ = K, Rb, Cs) have attracted enormous interest as they exhibit intertwined charge-density wave (CDW) and superconductivity. The alkali-metal dependence of these characteristics contains pivotal information about the CDW and its interplay with superconductivity. Here, we report optical studies of $A$V$_{3}$Sb$_{5}$ across the whole family. With increasing alkali-metal atom radius from K to Cs, the CDW gap increases monotonically, whereas $T_{\text{CDW}}$ first rises and then drops, at variance with conventional CDW. While the Fermi surface gapped by the CDW grows, $T_{c}$ is elevated in CsV$_{3}$Sb$_{5}$, indicating that the interplay between the CDW and superconductivity is not simply a competition for the density of states near \EF. More importantly, we observe an enhancement of electronic correlations in CsV$_{3}$Sb$_{5}$, which suppresses the CDW but enhances superconductivity, thus accounting for the above peculiar observations. Our results suggest electronic correlations as an important factor in manipulating the CDW and its entanglement with superconductivity in $A$V$_{3}$Sb$_{5}$.

Decisive role of electron-phonon coupling for phonon and electron instabilities in transition metal dichalcogenides

The origin of the charge density wave (CDW) in transition metal dichalcogenides has been hotly debated, and no conclusive agreement has been reached. Here, we propose an ab initio framework for an accurate description of both Fermi surface nesting and electron-phonon coupling (EPC) and systematically investigate their roles in the formation of the CDW. Using monolayer $1H\text{\ensuremath{-}}{\mathrm{NbSe}}_{2}$ and $1T\text{\ensuremath{-}}{\mathrm{VTe}}_{2}$ as representative examples, we show that it is the momentum-dependent EPC that softens the phonon frequencies, which become imaginary (phonon instabilities) at CDW vectors (indicating CDW formation). In addition, the distribution of the CDW gap opening (electron instabilities) can be correctly predicted only if EPC is included in the mean-field model. These results emphasize the decisive role of EPC in the CDW formation. Our analytical process is general and can be applied to other CDW systems.

Flat band in hole-doped transition metal dichalcogenide observed by angle-resolved photoemission spectroscopy

Layered transition metal dichalcogenides (TMDCs) gained widespread attention because of their electron-correlation-related physics, such as charge density wave (CDW), superconductivity, etc. In this paper, we report the high-resolution angle-resolved photoemission spectroscopy (ARPES) studies on the electronic structure of Ti-doped 1T-Ti x Ta1–x S2 with different doping levels. We observe a flat band that originates from the formation of the star of David super-cell at the x = 5% sample at the low temperature. With the increasing Ti doping levels, the flat band vanishes in the x = 8% sample due to the extra hole carrier. We also find the band shift and variation of the CDW gap caused by the Ti-doping. Meanwhile, the band folding positions and the CDW vector q CDW are intact. Our ARPES results suggest that the localized flat band and the correlation effect in the 1T-TMDCs could be tuned by changing the filling factor through the doping electron or hole carriers. The Ti-doped 1T-Ti x Ta1–x S2 provides a platform to fine-tune the electronic structure evolution and a new insight into the strongly correlated physics in the TMDC materials.

Electron-Exciton Coupling in 1T-TiSe2 Bilayer

Excitons in solid state are bosons generated by electron-hole pairs as the Coulomb screening is sufficiently reduced. The exciton condensation can result in exotic physics such as super-fluidity and insulating state. In charge density wave (CDW) state, 1T-TiSe2 is one of the candidates that may host the exciton condensation. However, to envision its excitonic effect is still challenging, particularly at the two-dimensional limit, which is applicable to future devices. Here, we realize the epitaxial 1T-TiSe2 bilayer, the two-dimensional limit for its 2 × 2 × 2 CDW order, to explore the exciton-associated effect. By means of high-resolution scanning tunneling spectroscopy and quasiparticle interference, we discover an unexpected state residing below the conduction band and right within the CDW gap region. As corroborated by our theoretical analysis, this mysterious phenomenon is in good agreement with the electron-exciton coupling. Our study provides a material platform to explore exciton-based electronics and opto-electronics.

Thermal hysteretic behavior and negative magnetoresistance in the charge density wave material EuTe4

EuTe4 is a newly-discovered van der Waals material exhibiting a novel charge-density wave (CDW) with a large thermal hysteresis in the resistivity and CDW gap. In this work, we systematically study the electronic structure and transport properties of EuTe4 using high-resolution angle-resolved photoemission spectroscopy (ARPES), magnetoresistance measurements, and scanning tunneling microscopy (STM). We observe a CDW gap of about 200 meV at low temperatures that persists up to 400 K, suggesting that the CDW transition occurs at a much higher temperature. We observe a large thermal hysteretic behavior of the ARPES intensity near the Fermi level, consistent with the resistivity measurement. The hysteresis in the resistivity measurement does not change under a magnetic field up to 7 T, excluding the thermal magnetic hysteresis mechanism. Instead, the surface topography measured with STM shows surface domains with different CDW trimerization directions, which may be important for the thermal hysteretic behavior of EuTe4. Interestingly, we observe a large negative magnetoresistance at low temperatures that can be associated with the canting of magnetically ordered Eu spins. Our work shed light on the understanding of magnetic, transport, and electronic properties of EuTe4.

Effects of niobium doping on the charge density wave and electronic correlations in the kagome metal Cs(V1−xNbx)3Sb5

The transport and optical properties of the Nb-doped Cs(V$_{1-x}$Nb$_{x}$)$_{3}$Sb$_{5}$ with x = 0.03 and 0.07 have been investigated and compared with those of the undoped CsV$_{3}$Sb$_{5}$. Upon Nb doping, the charge-density wave (CDW) transition temperature $T_{\text{CDW}}$ is suppressed, and the superconducting temperature $T_{c}$ rises. The residual resistivity ratio decreases with Nb doping, suggesting an increase of disorder. For all compounds, the optical conductivity in the pristine phase reveals two Drude components (D1 and D2). The substitution of Nb causes an increase of D1 alongside a reduction of D2 in weight, which implies a change of the Fermi surface. The total Drude weight is reduced with increasing Nb content, signifying an enhancement of electronic correlations. Below $T_{\text{CDW}}$, while the optical conductivity clearly manifests the CDW gap in all materials, the gapped portion of the Fermi surface shrinks as the Nb content grows. A comprehensive analysis indicates that the change of the Fermi surface, the enhancement of electronic correlations, the shrinkage of the removed Fermi surface by the CDW gap, and the increase of disorder may all have a considerable impact on the interplay between the CDW and superconductivity in Cs(V$_{1-x}$Nb$_{x}$)$_{3}$Sb$_{5}$.

Electrically controlled superconductor-to-failed insulator transition and giant anomalous Hall effect in kagome metal CsV3Sb5 nanoflakes

The electronic correlations (e.g. unconventional superconductivity (SC), chiral charge order and nematic order) and giant anomalous Hall effect (AHE) in topological kagome metals AV3Sb5 (A = K, Rb, and Cs) have attracted great interest. Electrical control of those correlated electronic states and AHE allows us to resolve their own nature and origin and to discover new quantum phenomena. Here, we show that electrically controlled proton intercalation has significant impacts on striking quantum phenomena in CsV3Sb5 nanodevices mainly through inducing disorders in thinner nanoflakes and carrier density modulation in thicker ones. Specifically, in disordered thin nanoflakes (below 25 nm), we achieve a quantum phase transition from a superconductor to a “failed insulator” with a large saturated sheet resistance for T → 0 K. Meanwhile, the carrier density modulation in thicker nanoflakes shifts the Fermi level across the charge density wave (CDW) gap and gives rise to an extrinsic-intrinsic transition of AHE. With the first-principles calculations, the extrinsic skew scattering of holes in the nearly flat bands with finite Berry curvature by multiple impurities would account for the giant AHE. Our work uncovers a distinct disorder-driven bosonic superconductor-insulator transition (SIT), outlines a global picture of the giant AHE and reveals its correlation with the unconventional CDW in the AV3Sb5 family.

Optical study of the topological materials LnSbTe (Ln=La, Ce, Sm, Gd)

The interaction among nontrivial topology, symmetry breaking orders, and strong electron correlation could generate many exotic physical phenomena. Recently, charge-density wave (CDW) orders and the Kondo effect are reported to occur in some of the $Ln\mathrm{Sb}\mathrm{Te}$ compounds, which are suggested to be either topological insulators or topological semimetals. Here we perform optical spectroscopic measurements on four of the $Ln\mathrm{Sb}\mathrm{Te}$ $(Ln=\mathrm{La}, \mathrm{Ce}, \mathrm{Sm}, \mathrm{Gd})$ compounds in order to investigate their exact electronic ground states. Metallic responses are commonly observed in all of the four compounds, despite their different transport behaviors. Furthermore, We observe some temperature-dependent excitations in the midinfrared region which are most likely to stem from CDW gaps. There is one such gap of about 452 meV in LaSbTe, one about 471 meV in CeSbTe, and two around 374 and 480 meV in GdSbTe, but none in SmSbTe, which is inconsistent with their highly similar electronic structures. Additionally, the presence of a Kondo hybridization gap is a bit too weak to be clearly revealed in our measured temperature range. Our results provide more detailed information on the $Ln\mathrm{Sb}\mathrm{Te}$ family, which helps to understand the underlying physics of these systems and inspires more related explorations.

Angle-resolved photoemission spectroscopy study of charge density wave order in the layered semiconductor EuTe4

Layered tellurides have been extensively studied as a platform for investigating the Fermi surface (FS) nesting-driven charge density wave (CDW) states. EuTe4, one of quasi-two-dimensional (quasi-2D) binary rare-earth tetratellurides CDW compounds, with unconventional hysteretic transition, is currently receiving much attention. Here, the CDW modulation vector, momentum and temperature dependence of CDW gaps in EuTe4 are investigated using angle-resolved photoemission spectroscopy. Our results reveal that (i) a FS nesting vector q ~ 0.67 b* drives the formation of CDW state, (ii) a large anisotropic CDW gap is fully open in the whole FS, and maintains a considerable size even at 300 K, leading to appearance of semiconductor properties, (iii) an abnormal non-monotonic increase of CDW gap in magnitude as a function of temperature, (iv) an extra, larger gap opens at a higher binding energy due to the interaction between the different orbits of the main bands.

Dramatic Plasmon Response to the Charge-Density-Wave Gap Development in 1T-TiSe_{2}.

1T-TiSe_{2} is one of the most studied charge density wave (CDW) systems, not only because of its peculiar properties related to the CDW transition, but also due to its status as a promising candidate of exciton insulator signaled by the proposed plasmon softening at the CDW wave vector. Using high-resolution electron energy loss spectroscopy, we report a systematic study of the temperature-dependent plasmon behaviors of 1T-TiSe_{2}. We unambiguously resolve the plasmon from phonon modes, revealing the existence of Landau damping to the plasmon at finite momentums, which does not support the plasmon softening picture for exciton condensation. Moreover, we discover that the plasmon lifetime at zero momentum responds dramatically to the band gap evolution associated with the CDW transition. The interband transitions near the Fermi energy in the normal phase are demonstrated to serve as a strong damping channel of plasmons, while such a channel in the CDW phase is suppressed due to the CDW gap opening, which results in the dramatic tunability of the plasmon in semimetals or small-gap semiconductors.

Optically induced changes in the band structure of the Weyl charge-density-wave compound

Collective modes are responsible for the emergence of novel quantum phases in topological materials. In the quasi-one dimensional (1D) Weyl semimetal , a charge density wave (CDW) opens band gaps at the Weyl points, thus turning the system into an axionic insulator. Melting the CDW would restore the Weyl phase, but 1D fluctuations extend the gapped regime far above the 3D transition temperature (T = 263 K), thus preventing the investigation of this topological phase transition with conventional spectroscopic methods.Here we use a non-equilibrium approach: we perturb the CDW phase by photoexcitation, and we monitor the dynamical evolution of the band structure by time- and angle-resolved photoelectron spectroscopy. We find that, upon optical excitation, electrons populate the linearly dispersing states at the Fermi level (E ), and fill the CDW gap. The dynamics of both the charge carrier population and the band gap renormalization (BGR) show a fast component with a characteristic time scale of a few hundreds femtoseconds. However, the BGR also exhibits a second slow component on the µs time scale. The combination of an ultrafast response and of persistent changes in the spectral weight at E , and the resulting sensitivity of the linearly dispersing states to optical excitations, may explain the high performances of as a material for broadband infrared photodetectors.