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Register a new userAnharmonic suppression of Charge density wave in 2H-NbS$_2$
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The temperature dependence of the phonon spectrum in the superconducting transition metal dichalcogenide 2H-NbS$_2$ is measured by diffuse and inelastic x-ray scattering. A deep, wide and strongly temperature dependent softening, of the two lowest energy longitudinal phonons bands, appears along the $mathrm{Gamma M}$ symmetry line in reciprocal space. In sharp contrast to the iso-electronic compounds 2H-NbSe$_2$, the soft phonons energies are finite, even at very low temperature, and no charge density wave instability occurs, in disagreement with harmonic ab-initio calculations. We show that 2H-NbS$_2$ is at the verge of the charge density wave transition and its occurrence is only suppressed by the large anharmonic effects. Moreover, the anharmonicity and the electron phonon coupling both show a strong in-plane anisotropy.
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The charge density wave (CDW) state in van der Waals systems shows interesting scaling phenomena as the number of layers can significantly affect the CDW transition temperature, $T_{CDW}$. However, it is often difficult to use conventional methods to study the phase transition in these systems due to their small size and sensitivity to degradation. Degradation is an important parameter which has been shown to greatly influence the superconductivity in layered systems. Since the CDW state competes with the onset of superconductivity, it is expected that $T_{CDW}$ will also be affected by the degradation. Here, we probe the CDW phase transition by the mechanical resonances of suspended 2H-TaS2 and 2H-TaSe2 membranes and study the effect of disorder on the CDW state. Pristine flakes show the transition near the reported values of 75 K and 122 K respectively. We then study the effect of degradation on 2H-TaS2 which displays an enhancement of $T_{CDW}$ up to 129 K after degradation in ambient air. Finally, we study a sample with local degradation and observe that multiple phase transitions occur at 87 K, 103 K and 118 K with a hysteresis in temperature in the same membrane. The observed spatial variations in the Raman spectra suggest that variations in crystal structure cause domains with different transition temperatures which could result in the hysteresis. This work shows the potential of using nanomechanical resonance to characterize the CDW in suspended 2D materials and demonstrate that degradation can have a large effect on transition temperatures.
Despite being usually considered two competing phenomena, charge-density-wave and superconductivity coexist in few systems, the most emblematic one being the transition metal dichalcogenide 2H-NbSe$_2$. This unusual condition is responsible for specific Raman signatures across the two phase transitions in this compound. While the appearance of a soft phonon mode is a well-established fingerprint of the charge-density-wave order, the nature of the sharp sub-gap mode emerging below the superconducting temperature is still under debate. In this work we use the external pressure as a knob to unveil the delicate interplay between the two orders, and consequently the nature of the superconducting mode. Thanks to an advanced extreme-conditions Raman technique we are able to follow the pressure evolution and the simultaneous collapse of the two intertwined charge density wave and superconducting modes. The comparison with microscopic calculations in a model system supports the Higgs-type nature of the superconducting mode and suggests that charge-density-wave and superconductivity in 2H-NbSe$_2$ involve mutual electronic degrees of freedom. These findings fill knowledge gap on the electronic mechanisms at play in transition metal dichalcogenides, a crucial step to fully exploit their properties in few-layers systems optimized for devices applications.
The interplay between charge density wave (CDW) order and superconductivity has attracted much attention. This is the central issue of along standing debate in simple transition metal dichalcogenides without strong electronic correlations, such as 2H-NbSe$_2$, in which twosuch phases coexist. The importance of anisotropic electron-phonon interaction has been recently highlighted from both theoretical and experimental point of view, and explains some of the key features of the formation of the CDW in this system. On the other hand, other aspects, such as the effects of anharmonicity, remain poorly understood despite their manifest importance in such soft-phonon driven phase transition. At the theoretical level in particular, their prohibitive computational price usually prevents their investigation within conventional perturbative approaches.Here, we address this issue using a combination of high resolution inelastic X-ray scattering measurements of the phonon dispersion, as afunction of temperature and pressure, with state of the art ab initio calculations. By explicitly taking into account anharmonic effects, we obtain an accurate, quantitative, description of the (P,T) dependence of the phonon spectrum, accounting for the rapid destruction of the CDW under pressure by zero mode vibrations - or quantum fluctuations - of the lattice. The low-energy longitudinal acoustic mode that drives the CDW transition barely contributes to superconductivity, explaining the insensitivity of the superconducting critical temperature to the CDW transition.
The pressure evolution of the Raman active electronic excitations of the transition metal dichalcogenides 2H-TaS$_2$ is followed through the pressure phase diagram embedding incommensurate charge-density-wave and superconducting states. At high pressure, the charge-density-wave is found to collapse at 8.5~GPa. In the coexisting charge-density-wave and superconducting orders, we unravel a strong in-gap superconducting mode, attributed to a Higgs mode, coexisting with the expected incoherent Cooper-pair breaking signature. The latter remains in the pure superconducting state reached above 8.5~GPa. Our report constitutes the first observation of such Raman active Higgs mode since the longstanding unique case 2H-NbSe$_2$.
As superconductors are thinned down to the 2D limit, their critical temperature $T_c$ typically decreases. Here we report the opposite behavior, a substantial enhancement of $T_c$ with decreasing thickness, in 2D crystalline superconductor 2H-TaS$_2$. Remarkably, in the monolayer limit, $T_c$ increases to 3.4 K compared to 0.8 K in the bulk. Accompanying this trend in superconductivity, we observe suppression of the charge-density wave (CDW) transition with decreasing thickness. To explain these trends, we perform electronic structure calculations showing that a reduction of the CDW amplitude results in a substantial increase of the density of states at the Fermi energy, which contributes to the enhancement of $T_c$. Our results establish ultra-thin 2H-TaS$_2$ as an ideal platform to study the competition between CDW order and superconductivity.
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