Pressure dependence of the optical properties of the charge-density-wave compound RTen (n=2 and 3)

Enlarged view: Figure 3.8
Figure 3.8: CDW gap as a function of the lattice constant a for CeTe3 under applied pressures and for the RTe3 series. Dotted lines are guides to the eye.

By performing pressure dependent optical investigations on a novel class of low dimensional materials (rare earth tri-tellurides), we demonstrate that one can tune (in this case gradually suppress) the charge density wave (CDW) gap by reducing the lattice parameter. Such control of the CDW gap is similar to that caused by chemical means (i.e. by alloying through rare-earth substitution). Therefore, we establish the equivalence of chemical and applied pressure in governing the onset of the CDW broken symmetry ground state (Fig. 3.8). This is especially interesting because the present results emphasize that the suppression of the CDW gap is not a result of disorder (which necessarily comes into play as a consequence of chemical substitution), but clearly arises from internal changes of the effective dimensionality of the electronic structure. This strengthens the arguments regarding the link between CDWs and nesting of the Fermi surface in low dimensional materials. We propose that the broadening of the bands upon lattice compression in the layered rare earth tri-tellurides removes the perfect nesting condition of the Fermi surface and therefore diminishes the impact of the CDW transition on their electronic properties.

Enlarged view: Figure 3.9
Figure 3.9: Pressure dependence of R(ω) in the mid-infrared spectral range of LaTe2 at 300 K. The arrow indicates the trend of the reflectivity data upon increasing pressure. The R(ω) points in the energy interval of the diamond absorption (i.e. 1700-2300 cm-1) have been omitted. The thin dotted lines are fits to the data within the Lorentz-Drude (LD) approach.

We have also investigated the pressure dependence of the optical response of LaTe2, which is deep in the charge-density-wave (CDW) ground state even at 300 K. The reflectivity spectrum (Fig. 3.9) is collected in the mid-infrared spectral range at room temperature and at pressures between 0 and 7 GPa. Applying a well established procedure based on the phenomenological Lorentz-Drude (LD) approach, we extract the energy scale due to the single particle excitation across the CDW gap and the Drude weight (Fig. 3.10). We establish that the gap decreases upon compressing the lattice, which shares common features with the behavior seen previously in the RTe3 series and in our recent data on CeTe3 under pressure. This signals a reduction in the quality of nesting upon applying pressure, therefore inducing a lesser impact of the CDW condensate on the electronic properties of LaTe2. The consequent suppression of the CDW gap leads to a release of additional charge carriers, manifested by the shift of weight from the gap feature into the metallic component of the optical response and indicated by the enhancement of the plasma frequency ωp (inset of Fig. 3.10). On the contrary, the power-law behavior, seen in the optical conductivity at energies above the gap excitation and suggesting a weakly interacting limit within the Tomonaga-Luttinger liquid scenario, seems to be only moderately dependent on pressure.

Enlarged view: Figure 3.10
Figure 3.10: Single particle peak energy ωSP (i.e. the CDW gap) as a function of the lattice constant a for LaTe2, CeTe3 and the RTe3 series. Inset: single particle peak energy ωSP versus plasma frequency ωp for LaTe2, as a function of pressure. Pressure is here an implicit variable.

In order to support the suppression of the CDW state upon compressing the lattice, we have also reported an x-ray diffraction study on the charge-density-wave (CDW) LaTe3 and CeTe3 compounds as a function of pressure (Fig. 3.10.1). We extract the lattice constants and the CDW modulation wave-vector. We observe that the intensity of the CDW satellite peaks tend to zero with increasing pressure (Fig. 3.10.2), thus providing direct evidence for a pressure-induced quenching of the CDW phase. Our findings further support the equivalence between chemical and applied pressure in RTe3, put forward by our previous optical investigations.

Fig. 3.10.1
Fig. 3.10.1: Selected XRD patterns on single-crystals of LaTe3 at 300 K and at 0.3 GPa (a) and 5.1 GPa (b), and of CeTe3 at 300 K and at 0.7 GPa (c) and 3.0 GPa (d), and finally on polycrystalline LaTe3 at 270 K and 6.2 GPa (e), and at 30 K and 5.9 GPa (f). Circles highlight the CDW satellite peaks. The modulation vector q is also shown in (a).
Enlarged view: Figure 3.10.2
Figure 3.10.2: Intensity of selected CDW satellite peaks normalized to a nearby Bragg-peak for LaTe3 (a) and CeTe3 (b) at 300 K as a function of pressure and for LaTe3 at 6 GPa as a function of temperature, with the prediction from the BCS theory (c). (d) Ratio b/a as a function of the average lattice constant a. Thin lines in panel (d) are linear interpolations to the data, as guide to the eyes.
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