Microscopic phase-transition theory of charge density waves: revealing hidden transitions of phason and amplitudon

Abstract: We develop a self-consistent phase-transition theory of charge density waves (CDWs), starting from a purely microscopic model. Specifically, we derive a microscopic CDW gap equation $|\Delta_0(T)|$, taking into account of thermal phase fluctuations (i.e., thermal excitation of phason) and their influence on CDW pinning (i.e., the phason mass) and CDW gap. We demonstrate that as temperature increases from zero, the phason gradually softens, leading to a depinning transition (where the phason becomes gapless) at $T_d$ and a subsequent first-order CDW phase transition at $T_c>T_d$. The predicted values of $T_d$, $T_c$ as well as the large ratio of $|\Delta_0(T=0)|/(k_BT_c)$ for the quasi-one-dimensional CDW material (TaSe$_4$)$_2$I show remarkable quantitative agreements with experimental measurements and explain many of the previously observed key thermodynamic features and unresolved issues in literature. To further validate the theory, we calculate the energy gap of CDW amplitudon and its lifetime, and reveal a transition of amplitudon from a lightly damped to a heavily damped excitation during pinning-depinning transition while its energy gap is nearly unchanged throughout the entire CDW phase. This finding quantitatively captures and explains the recently observed coherent signal in ultrafast THz emission spectroscopy on (TaSe$_4$)$_2$I.