Melting Of Charge Density Wave Research Articles

Phonon transport manipulation in TiSe2 via reversible charge density wave melting

Titanium diselenide (TiSe2) is a layered material that under a critical temperature of Tc ≈ 200 K features a periodic modulation of the electron density, known as charge density wave (CDW), which finds applications in quantum information and emerging electronic devices. Here, we present first-principles calculations showing the suppression of the CDW via photoexcitation and consequent stabilization of the undistorted high-temperature phase, in agreement with experimental observations. Interestingly, the unfolded CDW melting is accompanied by a sizable reduction in the thermal conductivity, κ, of up to 25% and a large entropy increase of ~10 J K−1 kg−1. The significant κ variation is almost entirely originated from photoinduced changes in the phonon–phonon scattering processes involving a high-symmetry soft phonon mode. Our results open new possibilities in the design of devices for thermal management and phonon-based logic, and suggest original applications in the of context solid-state cooling.

Nonequilibrium Charge-Density-Wave Melting in 1T-TaS2 Triggered by Electronic Excitation: A Real-Time Time-Dependent Density Functional Theory Study.

Ultrafast charge transfer in van der Waals (vdW) heterostructures enables efficient control of two-dimensional material properties through strong optical absorption and subsequent carrier transfer. Here, using real-time time-dependent density functional theory coupled to molecular dynamics, we investigated the nonequilibrium dynamics of charge-density-wave (CDW) melting in 1T-TaS2 triggered by ultrafast charge transfer in 1T-TaS2/MoSe2 or WSe2 heterostructures. Despite the fast and sufficient charge transfer from the MoSe2 (or WSe2) "electrode" to the 1T-TaS2 layer, the electronic excitation of the vdW heterostructure does not lead to the nonthermal CDW transition of 1T-TaS2. Instead, the TaS2 lattice is heated by carrier-lattice scattering, leading to thermal CDW melting at high ionic temperatures. The lack of nonthermal melting follows from the fact that the time scale of carrier recombination in 1T-TaS2 is similar to or faster than that of charge transfer. These findings provide physical insights into understanding the CDW melting dynamics in vdW heterostructures under nonequilibrium conditions.

Effects of disorder and hydrostatic pressure on charge density wave and superconductivity in 2H−TaS2

We report the comparative effects of disorder and hydrostatic pressure on charge density wave (CDW) and superconductivity (SC) in $2H\text{\ensuremath{-}}{\mathrm{TaS}}_{2}$ by measuring electrical resistivity and ac magnetic susceptibility. For the crystals in the clean limit (low disorder level), CDW ground state is suppressed completely at a critical pressure ${P}_{\mathrm{c}}\ensuremath{\sim}6.24(5)\phantom{\rule{0.16em}{0ex}}\mathrm{GPa}$ where a dome-shaped pressure dependence of superconducting transition temperature ${T}_{\mathrm{c}}$(P) appears with a maximum value of ${{T}_{\mathrm{c}}}^{\mathrm{max}}\ensuremath{\sim}9.15\phantom{\rule{0.16em}{0ex}}\mathrm{K}$, indicating strong competitions between CDW and SC. The temperature exponent $n$ of low-temperature resistivity data decreases from \ensuremath{\sim}3.36 at ambient pressure (AP) to \ensuremath{\sim}1.29(2) at ${P}_{\mathrm{c}}$ and then retains a saturated value \ensuremath{\sim}2.10(4) when the pressure is higher than 7.5 GPa; accordingly, the quadratic temperature coefficient of normal-state resistivity A peaks out just at ${P}_{\mathrm{c}}$ with an enhancement by nearly one order in magnitude. These features strongly manifest that the enhanced critical CDW fluctuations near ${P}_{\mathrm{c}}$ are possible important glues for superconducting pairings. High-pressure magnetic susceptibility indicates that superconducting shielding volume increases with pressure and retains a nearly constant value above ${P}_{\mathrm{c}}$, which evidences that the enhancement of ${T}_{\mathrm{c}}$(P) is accompanied by the expense of CDW. For those crystals in dirty limit (high disorder level), there is no clear CDW phase transition in resistivity; the pressure dependence of ${T}_{\mathrm{c}}$(P) and $n$ broadens up and becomes less apparent in comparison with the clean crystals. Our results suggest that disorder scattering and the melting of CDW are two factors affecting SC, and the melting of CDW dominates the change of ${T}_{\mathrm{c}}$ below ${P}_{\mathrm{c}}$; the enhancement of ${T}_{\mathrm{c}}$(P) is associated with the suppression of CDW by pressure and the increase in the density of states at Fermi level; however, after the CDW collapse, superconducting pairing strength is strongly weakened by impurity scattering above ${P}_{\mathrm{c}}$ according to Anderson's theorem.

Charge-density-wave melting in the one-dimensional Holstein model

We study the Holstein model of spinless fermions, which at half-filling exhibits a quantum phase transition from a metallic Tomonaga-Luttinger liquid phase to an insulating charge-density-wave (CDW) phase at a critical electron-phonon coupling strength. In our work, we focus on the real-time evolution starting from two different types of initial states that are CDW ordered: (i) ideal CDW states with and without additional phonons in the system and (ii) correlated ground states in the CDW phase. We identify the mechanism for CDW melting in the ensuing real-time dynamics and show that it strongly depends on the type of initial state. We focus on the far-from-equilibrium regime and emphasize the role of electron-phonon coupling rather than dominant electronic correlations, thus complementing a previous study of photo-induced CDW melting [H. Hashimoto and S. Ishihara, Phys. Rev. B 96, 035154 (2017)]. The numerical simulations are performed by means of matrix-product-state based methods with a local basis optimization (LBO). Within these techniques, one rotates the local (bosonic) Hilbert spaces adaptively into an optimized basis that can then be truncated while still maintaining a high precision. In this work, we extend the time-evolving block decimation (TEBD) algorithm with LBO, previously applied to single-polaron dynamics, to a half-filled system. We demonstrate that in some parameter regimes, a conventional TEBD method without LBO would fail. Furthermore, we introduce and use a ground-state density-matrix renormalization group method for electron-phonon systems using local basis optimization. In our examples, we account for up to $M_{\rm ph} = 40$ bare phonons per site by working with $O(10)$ optimal phonon modes.

Photoexcitation Induced Quantum Dynamics of Charge Density Wave and Emergence of a Collective Mode in 1T-TaS2.

Photoexcitation is a powerful means in distinguishing different interactions and manipulating the states of matter, especially in charge density wave (CDW) materials. The CDW state of 1T-TaS2 has been widely studied experimentally mainly because of its intriguing laser-induced ultrafast responses of electronic and lattice subsystems. However, the microscopic atomic dynamics and underlying electronic mechanism upon photoexcitation remain unclear. Here, we demonstrate photoexcitation induced ultrafast dynamics of CDW in 1T-TaS2 using time-dependent density functional theory molecular dynamics. We discover a novel collective oscillation mode between the CDW state and a transient state induced by photodoping, which is significantly different from thermally induced phonon mode and attributed to the modification of the potential energy surface from laser excitation. In addition, our finding validates nonthermal melting of CDW induced at low light intensities, supporting that conventional hot electron model is inadequate to explain photoinduced dynamics. Our results provide a deep insight into the coherent electron and lattice quantum dynamics during the formation and excitation of CDW in 1T-TaS2.

Charge Density Wave Melting in One-Dimensional Wires with Femtosecond Subgap Excitation

Charge density waves (CDWs) are symmetry-broken ground states that commonly occur in low-dimensional metals due to strong electron-electron and/or electron-phonon coupling. The nonequilibrium carrier distribution established via photodoping with femtosecond laser pulses readily quenches these ground states and induces an ultrafast insulator-to-metal phase transition. To date, CDW melting has been mainly investigated in the single-photon regime with pump photon energies bigger than the gap size. The recent development of strong-field midinfrared sources now enables the investigation of CDW dynamics following subgap excitation. Here we excite prototypical one-dimensional indium wires with a CDW gap of ∼300 meV with midinfrared pulses at ℏω=190 meV with MV/cm field strength and probe the transient electronic structure with time- and angle-resolved photoemission spectroscopy. We find that the CDW gap is filled on a timescale short compared to our temporal resolution of 300fs and that the band structure changes are completed within ∼1 ps. Supported by a minimal theoretical model we attribute our findings to multiphoton absorption across the CDW gap.

A setup for extreme-ultraviolet ultrafast angle-resolved photoelectron spectroscopy at 50-kHz repetition rate.

Time- and angle-resolved photoelectron spectroscopy (trARPES) is a powerful method to track the ultrafast dynamics of quasiparticles and electronic bands in energy and momentum space. We present a setup for trARPES with 22.3 eV extreme-ultraviolet (XUV) femtosecond pulses at 50-kHz repetition rate, which enables fast data acquisition and access to dynamics across momentum space with high sensitivity. The design and operation of the XUV beamline, pump-probe setup, and ultra-high vacuum endstation are described in detail. By characterizing the effect of space-charge broadening, we determine an ultimate source-limited energy resolution of 60 meV, with typically 80-100 meV obtained at 1-2 × 1010 photons/s probe flux on the sample. The instrument capabilities are demonstrated via both equilibrium and time-resolved ARPES studies of transition-metal dichalcogenides. The 50-kHz repetition rate enables sensitive measurements of quasiparticles at low excitation fluences in semiconducting MoSe2, with an instrumental time resolution of 65 fs. Moreover, photo-induced phase transitions can be driven with the available pump fluence, as shown by charge density wave melting in 1T-TiSe2. The high repetition-rate setup thus provides a versatile platform for sensitive XUV trARPES, from quenching of electronic phases down to the perturbative limit.

Optimizing laser pulses to control photoinduced states of matter

We present a computational approach to optimal laser pulse shaping directed at accessing novel photoinduced states of matter. Results are illustrated for a simple charge-density wave (CDW) model where the targeted effect is CDW melting and negative temperature states. Optimal control is implemented using the Krotov method applied to nonequilibrium tight-binding Hamiltonians where the laser pulse is introduced using the Peierls substitution, and we demonstrate monotonic convergence for this class of problem.

Dynamics of Photoinduced Charge-Density-Wave to Metal Phase Transition inK0.3MoO3

We present the first systematic studies of the photoinduced phase transition from the ground charge density wave (CDW) state to the normal metallic state in the prototype quasi-1D CDW system K0.3MoO3. Ultrafast nonthermal CDW melting is achieved at the absorbed energy density that corresponds to the electronic energy difference between the metallic and CDW states. The results imply that on the subpicosecond time scale when melting and subsequent initial recovery of the electronic order takes place the lattice remains unperturbed.