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Register a new userAnharmonic melting of the charge density wave in single-layer TiSe2
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Low dimensional systems with a vanishing band-gap and a large electron-hole interaction have been proposed to be unstable towards exciton formation. As the exciton binding energy increases in low dimension, conventional wisdom suggests that excitonic insulators should be more stable in 2D than in 3D. Here we study the effects of the electron-hole interaction and anharmonicity in single-layer TiSe2. We find that, contrary to the bulk case and to the generally accepted picture, the electron-hole exchange interaction is much smaller in 2D than in 3D and it has negligible effects on phonon spectra. By calculating anharmonic phonon spectra within the stochastic self-consistent harmonic approximation, we obtain TCDW = 440K for an isolated and undoped single-layer and TCDW = 364K for an electron-doping n = 4.6 x 10^13 cm^{-2} , close to the experimental result of 200-280K on supported samples. Our work demonstrates that anharmonicity and doping melt the charge density wave in single-layer TiSe2.
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The impact of variable Ti self-doping on the 1T-TiSe2 charge density wave (CDW) is studied by scanning tunneling microscopy. Supported by density functional theory we show that agglomeration of intercalated-Ti atoms acts as preferential nucleation centers for the CDW that breaks up in phaseshifted CDW domains whose size directly depends on the intercalated-Ti concentration and which are separated by atomically-sharp phase boundaries. The close relationship between the diminution of the CDW domain size and the disappearance of the anomalous peak in the temperature dependent resistivity allows to draw a coherent picture of the 1T-TiSe2 CDW phase transition and its relation to excitons.
We study the structural, electronic and vibrational properties of single-layer 1TNbSe$_2$ from first principles. Within the generalized gradient approximation, the 1T polytype is highly unstable with respect to the 2H. The DFT+U method improves the stability of the 1T phase, explaining its detection in experiments. A charge density wave occurs with a $sqrt{13}timessqrt{13}~R30^{circ}$ periodicity, in agreement with STM data. At $U=0$, the David-star reconstruction displays a flat band below the Fermi level with a marked d$_{z^2-r^2}$ orbital character of the central Nb. The Hubbard interaction induces a magnetic Mott insulating state. Magnetism distorts the lattice around the central Nb atom in the star, reduces the hybridization between the central Nb d$_{z^2-r^2}$ orbital and the neighbouring Se p-states and lifts in energy the flat band becoming non-bonding. This cooperative lattice and magnetic effect amplifies the Mott gap. Single-layer 1TNbSe$_2$ is then a phonon-assisted spin-$1/2$ Magnetic Mott insulator.
The transition metal dichalcogenide $1T$-TiSe$_2$ is a quasi-two-dimensional layered material with a phase transition towards a commensurate charge density wave (CDW) at a critical temperature T$_{c}approx 200$K. The relationship between the origin of the CDW instability and the semimetallic or semiconducting character of the normal state, i.e., with the non-reconstructed Fermi surface topology, remains elusive. By combining angle-resolved photoemission spectroscopy (ARPES), scanning tunneling microscopy (STM), and density functional theory (DFT) calculations, we investigate $1T$-TiSe$_{2-x}$S$_x$ single crystals. Using STM, we first show that the long-range phase coherent CDW state is stable against S substitutions with concentrations at least up to $x=0.34$. The ARPES measurements then reveal a slow but continuous decrease of the overlap between the electron and hole ($e$-$h$) bands of the semimetallic normal-state well reproduced by DFT and related to slight reductions of both the CDW order parameter and $T_c$. Our DFT calculations further predict a semimetal-to-semiconductor transition of the normal state at a higher critical S concentration of $x_c$=0.9 $pm$0.1, that coincides with a melted CDW state in TiSeS as measured with STM. Finally, we rationalize the $x$-dependence of the $e$-$h$ band overlap in terms of isovalent substitution-induced competing chemical pressure and charge localization effects. Our study highlights the key role of the $e$-$h$ band overlap for the CDW instability.
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 non-equilibrium 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 and tunneling regimes, while the intermediate multi-photon regime has received little attention. Here we excite one-dimensional indium wires with a CDW gap of ~300meV with mid-infrared pulses at 190meV with MV/cm field strength and probe the transient electronic structure with time- and angle-resolved photoemission spectroscopy (tr-ARPES). We find that the CDW gap is filled on a timescale short compared to our temporal resolution of 300fs and that the phase transition is completed within ~1ps. Supported by a minimal theoretical model we attribute our findings to multi-photon absorption across the CDW gap.
Among transition metal dichalcogenides (TMDs), VSe$_2$ is considered to develop a purely 3-dimensional (3D) charge-density wave (CDW) at T$_{CDW}$=110 K. Here, by means of high resolution inelastic x-ray scattering (IXS), we show that the CDW transition is driven by the collapse of an acoustic mode at the critical wavevector textit{q}$_{CDW}$= (2.25 0 0.7) r.l.u. and critical temperature T$_{CDW}$=110 K. The softening of this mode starts to be pronounced for temperatures below 2$times$ T$_{CDW}$ and expands over a rather wide region of the Brillouin zone, suggesting a large contribution of the electron-phonon interaction to the CDW formation. This interpretation is supported by our first principles calculations that determine a large momentum-dependence of the electron-phonon interaction, peaking at the CDW wavevector, in the presence of nesting. Fully anharmonic {it ab initio} calculations confirm the softening of one acoustic branch at textit{q}$_{CDW}$ as responsible for the CDW formation and show that van der Waals interactions are crucial to melt the CDW. Our work also highlights the important role of out-of-plane interactions to describe 3D CDWs in TMDs.
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