Evolution of charge-density-wave soft phonon modes in $\mathrm{Pd}_x\mathrm{ErTe}_3$

Abstract

We investigated the lattice dynamics of quasi-two-dimensional Pd-intercalated $\mathrm{ErTe}_3$ in relation to its charge-density-wave (CDW) transitions by means of x-ray diffuse and meV-resolution inelastic x-ray scattering. In pristine $\mathrm{ErTe}_3$, CDW order develops at orthogonal in-plane wave vectors $\boldsymbol{\mathrm{q}}_{1}^{c} = (0, 0, 0.29)$ (the $c\text{-}\mathrm{CDW}$) and $\boldsymbol{\mathrm{q}}_{2}^{a} = (0.31, 0, 0)$ (the $a\text{-}\mathrm{CDW}$), with transition temperatures $T_{1}^{c} = 270$ K and $T_{2}^{a} = 160$ K, respectively. Remarkably, we observe diffuse x-ray scattering already near the higher transition temperature $T_{1}^{c}$ along $a\text{-}\mathrm{CDW}$ but at a slightly different wave vector $\boldsymbol{\mathrm{q}}_{1}^{a} = (0.29, 0, 0)$. Inelastic x-ray scattering for $\mathrm{Pd}_{0.01}\mathrm{ErTe}_3$ shows that a partial phonon softening at $\boldsymbol{\mathrm{q}}_{1}^{a}$, underscoring the strong competition between ordering tendencies along the nearly equivalent in-plane axes of the orthorhombic lattice. For intercalation levels $x \geq 0.02$, the $a\text{-}\mathrm{CDW}$ state is suppressed. Nevertheless, a similar correlation between phonon softening and diffuse scattering persists along the $[100]$ direction, again observed at $\boldsymbol{\mathrm{q}}_{1}^{a} = (0.29, 0, 0)$ and $T_{1}^{c}$. These findings suggest that the $a\text{-}\mathrm{CDW}$ is fully suppressed for $x \geq 0.02$, and that the residual diffuse scattering at $\boldsymbol{\mathrm{q}}_{1}^{a}$ originates from the partial phonon softening associated with the $c\text{-}\mathrm{CDW}$, reflected by the near equality of the absolute size of $\boldsymbol{\mathrm{q}}_{1}^{c}$ and $\boldsymbol{\mathrm{q}}_{1}^{a}$.