Incommensurate Charge Density Wave Phase Research Articles

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.

Elastoresistivity in the incommensurate charge density wave phase of BaNi2(As1−xPx)2

AbstractElectronic nematicity, the breaking of the crystal lattice rotational symmetry by the electronic fluid, is a fascinating quantum state of matter. In this work, using electronic transport under strain we investigate the electronic nematicity of BaNi2(As1−xPx)2, a candidate system for charge-induced nematicity. We report a large B1g elastoresistance coefficient that is maximized at the tetragonal-to-orthorhombic transition temperature, that slightly precedes the first-order triclinic transition. An hysteretic behavior is observed in the resistance versus strain sweeps and interpreted as the pinning of orthorhombic domains. Remarkably, the elastoresistance only onsets together with a strong enhancement of the incommensurate charge density wave of the material, strongly suggesting that this electronic instability is uniaxial in nature and drive the orthorhombic transition. The absence of sizeable elastoresistance above this electronic phase clearly contrasts dynamic and static electronic nematicity. Finally, the elastoresistance temperature dependence that strongly differs from the Curie-Weiss form of iron-based superconductors reveals major differences for the respective coupling of electronic nematicity to the lattice. Our results uncover an extremely strain-sensitive platform to study electronic anisotropy induced by a charge-density-wave instability.

Observation of multiple charge density wave phases in epitaxial monolayer 1T-VSe2 film

As a special order of electronic correlation induced by spatial modulation, the charge density wave (CDW) phenomena in condensed matters attract enormous research interests. Here, using scanning–tunneling microscopy in various temperatures, we discover a hidden incommensurate stripe-like CDW order besides the () CDW phase at low-temperature of 4 K in the epitaxial monolayer 1T-VSe2 film. Combining the variable-temperature angle-resolved photoemission spectroscopic (ARPES) measurements, we discover a two-step transition of an anisotropic CDW gap structure that consists of two parts Δ 1 and Δ 2. The gap part Δ 1 that closes around ∼ 150 K is accompanied with the vanish of the () CDW phase. While another momentum-dependent gap part Δ 2 can survive up to ∼ 340 K, and is suggested to the result of the incommensurate CDW phase. This two-step transition with anisotropic gap opening and the resulted evolution in ARPES spectra are corroborated by our theoretical calculation based on a phenomenological form for the self-energy containing a two-gap structure Δ 1 + Δ 2, which suggests different forming mechanisms between the () and the incommensurate CDW phases. Our findings provide significant information and deep understandings on the CDW phases in monolayer 1T-VSe2 film as a two-dimensional (2D) material.

Photoinduced intragap excitations in the incommensurate charge density wave phase of Rb0.3MoO3

Using time- and angle-resolved photoemission spectroscopy, we investigate the photoexcited electron dynamics in a prototypical charge density wave (CDW) material, Rb0.3MoO3. We observe a pronounced slow relaxation component within the CDW-gap energies. This anomalously slow dynamics is independent of the wave number, and cannot be explained by the presence of impurities. We propose that phase-coherent domains are temporarily established after a transient closure of the CDW gap, and that the intragap excitations are attributed to relaxation of the domain boundaries.

Second harmonic generation as a probe of broken mirror symmetry

The notion of spontaneous symmetry breaking has been used to describe phase transitions in a variety of physical systems. In crystalline solids, the breaking of certain symmetries, such as mirror symmetry, is difficult to detect unambiguously. Using 1$T$-TaS$_2$, we demonstrate here that rotational-anisotropy second harmonic generation (RA-SHG) is not only a sensitive technique for the detection of broken mirror symmetry, but also that it can differentiate between mirror symmetry-broken structures of opposite planar chirality. We also show that our analysis is applicable to a wide class of different materials with mirror symmetry-breaking transitions. Lastly, we find evidence for bulk mirror symmetry-breaking in the incommensurate charge density wave phase of 1$T$-TaS$_2$. Our results pave the way for RA-SHG to probe candidate materials where broken mirror symmetry may play a pivotal role.

Temperature-filling phase diagram of the two-dimensional Holstein model in the thermodynamic limit by self-consistent Migdal approximation

We study the temperature-filling phase diagram of the single-band Holstein model in two dimensions using the self-consistent Migdal approximation, where both the electron and phonon self-energies are treated on an equal footing. By employing an efficient numerical algorithm utilizing fast Fourier transforms to evaluate momentum and Matsubara frequency summations, we determine the charge-density-wave (CDW) and superconducting transition temperatures in the thermodynamic limit using lattice sizes that are sufficient to eliminate significant finite size effects present at lower temperatures. We obtain the temperature-filling phase diagrams for a range of coupling strengths and phonon frequencies for the model defined on a square lattice with and without next-nearest neighbor hopping. We find the appearance of a superconducting dome with a critical temperature that decreases before reaching the $\mathbf{q}_{\text{max}} = (\pi,\pi)$ CDW phase boundary. For very low phonon frequencies, we also find an incommensurate CDW phase with the ordering vector $\mathbf{q}_{\text{max}} \approx (\pi,\pi)$ appearing between the commensurate CDW and superconducting phases. Our numerical implementation can be easily extended to treat momentum-dependent electron-phonon coupling, as well as dispersive phonon branches, and has been made available to the public.

Electronic structure of commensurate, nearly commensurate, and incommensurate phases of 1T−TaS2 by angle-resolved photoelectron spectroscopy, scanning tunneling spectroscopy, and density functional theory

The electronic structure of $1T\ensuremath{-}\mathrm{Ta}{\mathrm{S}}_{2}$ showing a metal-insulator transition and a sequence of different charge density wave (CDW) transformations was discussed in the frame of variable temperature angle-resolved photoelectron spectroscopy (ARPES), scanning tunneling spectroscopy (STS), and density functional theory (DFT) calculations. For the commensurate charge density wave phase (CCDW) the Mott gap was estimated to be 0.4 eV and energy gaps ${\mathrm{\ensuremath{\Delta}}}_{\text{CCDW},1},\phantom{\rule{0.16em}{0ex}}{\mathrm{\ensuremath{\Delta}}}_{\text{CCDW},2},\phantom{\rule{0.16em}{0ex}}{\mathrm{\ensuremath{\Delta}}}_{B3\ensuremath{-}\mathit{HHB}},\phantom{\rule{0.16em}{0ex}}{\mathrm{\ensuremath{\Delta}}}_{B4\ensuremath{-}B3}$ were observed. For the nearly commensurate charge density wave phase (NCCDW), the reminiscent of higher and lower Hubbard bands and a very pronounced electronic state associated with the parabolic band at the $\overline{\mathrm{\ensuremath{\Gamma}}}$ point in the Brillouin zone were identified. The incommensurate charge density wave phase (ICCDW) showed a high value of local density of states at the Fermi level and a very pronounced edge of the metallic surface state located in the range of 0.15--0.20 eV above the Fermi level. The obtained STS and ARPES results were consistent with our theoretical calculations performed within DFT formalism including spin-orbit coupling.

Chemical Growth of 1T-TaS2 Monolayer and Thin Films: Robust Charge Density Wave Transitions and High Bolometric Responsivity.

Ultrathin two-dimensional (2D) charge density wave (CDW) materials, with sharp resistance change at the phase-transition temperature, yet with ultrathin thickness, hold great potential for electrical device applications. However, chemical synthesis of high-quality samples and observation of the CDW states down to the monolayer limit is still of great challenge. Chemical vapor deposition of 1T-TaS2 sheets on hexagonal boron nitride (h-BN) with robust CDW states even down to the monolayer extreme is reported here. Further, based on the near commensurate CDW to incommensurate CDW phase transition with a high temperature coefficient of resistance (TCR), highly responsive room-temperature bolometers are fabricated by suspending the as-grown 1T-TaS2 sheets.

Influence of Domain Walls in the Incommensurate Charge Density Wave State of Cu Intercalated 1T-TiSe_{2}.

We report a low-temperature scanning tunneling microscopy study of the charge density wave (CDW) order in 1T-TiSe_{2} and Cu_{0.08}TiSe_{2}. In pristine 1T-TiSe_{2} we observe a long-range coherent commensurate CDW (CCDW) order. In contrast, Cu_{0.08}TiSe_{2} displays an incommensurate CDW (ICDW) phase with localized CCDW domains separated by domain walls. Density of states measurements indicate that the domain walls host an extra population of fermions near the Fermi level which may play a role in the emergence of superconductivity in this system. Fourier transform scanning tunneling spectroscopy studies suggest that the dominant mechanism for CDW formation in the ICDW phase may be electron-phonon coupling.

A charge-density-wave oscillator based on an integrated tantalum disulfide-boron nitride-graphene device operating at room temperature.

The charge-density-wave (CDW) phase is a macroscopic quantum state consisting of a periodic modulation of the electronic charge density accompanied by a periodic distortion of the atomic lattice in quasi-1D or layered 2D metallic crystals. Several layered transition metal dichalcogenides, including 1T-TaSe2, 1T-TaS2 and 1T-TiSe2 exhibit unusually high transition temperatures to different CDW symmetry-reducing phases. These transitions can be affected by the environmental conditions, film thickness and applied electric bias. However, device applications of these intriguing systems at room temperature or their integration with other 2D materials have not been explored. Here, we demonstrate room-temperature current switching driven by a voltage-controlled phase transition between CDW states in films of 1T-TaS2 less than 10 nm thick. We exploit the transition between the nearly commensurate and the incommensurate CDW phases, which has a transition temperature of 350 K and gives an abrupt change in current accompanied by hysteresis. An integrated graphene transistor provides a voltage-tunable, matched, low-resistance load enabling precise voltage control of the circuit. The 1T-TaS2 film is capped with hexagonal boron nitride to provide protection from oxidation. The integration of these three disparate 2D materials in a way that exploits the unique properties of each yields a simple, miniaturized, voltage-controlled oscillator suitable for a variety of practical applications.

Contrast and Raman spectroscopy study of single- and few-layered charge density wave material: 2H-TaSe₂.

In this article, we report the first successful preparation of single- and few-layers of tantalum diselenide (2H-TaSe2) by mechanical exfoliation technique. Number of layers is confirmed by white light contrast spectroscopy and atomic force microscopy (AFM). Vibrational properties of the atomically thin layers of 2H-TaSe2 are characterized by micro-Raman spectroscopy. Room temperature Raman measurements demonstrate MoS2-like spectral features, which are reliable for thickness determination. E1g mode, usually forbidden in backscattering Raman configuration is observed in the supported TaSe2 layers while disappears in the suspended layers, suggesting that this mode may be enabled because of the symmetry breaking induced by the interaction with the substrate. A systematic in-situ low temperature Raman study, for the first time, reveals the existence of incommensurate charge density wave phase transition in single and double-layered 2H-TaSe2 as reflected by a sudden softening of the second-order broad Raman mode resulted from the strong electron-phonon coupling (Kohn anomaly).

Quenching of phase coherence in quasi-one-dimensional ring crystals

A comparison of the single-particle (SP) dynamics of whisker and ring $\mathrm{Nb}{\mathrm{Se}}_{3}$ crystals provides new insight into the phase transition properties of quasi-one-dimensional charge density wave (CDW) systems. In the incommensurate CDW phase, SP relaxation triggered by an ultrafast laser pulse reflects the formation of collective states, and reveals the divergence of the relaxation time when approaching a transition temperature. The degree of divergence is less pronounced in rings than in whiskers, suggesting a loss of phase coherence in ring crystals characterized by a closed-loop topology.

Scanning tunneling microscopy investigations of the local electronic and structural effects of iron substitution in tantalum disulfide

The microscopic structural and electronic properties of the charge density wave (CDW) phases in a series of iron-substituted tantalum disulfide materials, Fe{sub x}Ta{sub 1{minus}x}S{sub 2}, have been characterized with the use of scanning tunneling microscopy (STM). On average, the incommensurate CDW phase exhibits a regular hexagonal superlattice for x(Fe) {<=} 0.02. At the atomic level, however, analysis of real-space STM images shows that there are well-defined defects in this CDW structure. The frequency and size of the defects depend directly on the concentration of iron. These results resolve the source of differences between STM and previous diffraction studies of metal-substituted tantalum disulfide and also indicate that above a critical concentration of iron the properties of the CDW phase in these materials change significantly. The origin of this critical concentration is discussed.

Generalized electronic susceptibility and charge density waves in transition metal dichalcogenides

Lattice vibrations in 2H-TaSe 2 and 2H-NbSe 2 are investigated by one- and two-phonon Raman scattering in the normal and charge density wave (CDW) phases. The generalized electronic susceptibility is obtained from the two-phonon scattering intensity as a function of temperature, and with its use the temperature dependent energies of the Kohn anomaly mode and the soft CDW modes are calculated. The agreement with the directly obtained data from this experiment is excellent. In 2H-TaSe 2 four A g-modes and two B 1g-modes are observed in the commensurate CDW state as expected from the orthorhombic superlattice structure. The discommensuration in the incommensurate CDW phase gives the continuous change of the Raman spectra over the three CDW phases.

Ultrasound measurements in the layered transition-metal dichalcogenides NbSe2and TaS2

Ultrasound measurements in 2H-NbSe2 and 1T-TaS2 are reported. A 3% decrease in the velocity of transverse ultrasonic waves propagating parallel to the c-axis is found in NbSe2 when the temperature is lowered from 220K to 35K. In this material, a 0.2% dip in nu transverse is observed at the incommensurate charge density wave phase transition. The ratio of nu longitudinal to nu transverse is determined to be 1.4 to NbSe2 and 1.7 TaS2.