Enhanced Phonon-Phonon Interactions and Weakened Electron-Phonon Coupling in Charge-Density-Wave Topological Semimetal EuAl4 with a Possible Intermediate Electronic State

TL;DR

This study uses Raman spectroscopy to investigate phonon-phonon interactions and electron-phonon coupling in EuAl4, revealing enhanced PPI, weakened EPC, and a possible intermediate electronic state associated with the charge density wave transition.

Contribution

It provides new insights into the evolution of PPI and EPC across the CDW transition in EuAl4, highlighting the existence of an intermediate electronic state and the contrasting behaviors of PPI and EPC.

Findings

Enhanced phonon-phonon interactions after CDW transition

Weakened electron-phonon coupling below Tc

Evidence for an intermediate electronic state between 50 K and Tc

Abstract

The origin of charge density wave (CDW) is a long-term open issue. Furthermore, the evolution of phonon-phonon interactions (PPI) across CDW transitions has rarely been investigated. Besides, whether electron-phonon coupling (EPC) would be weakened or enhanced after CDW transitions is still under debate. Additionally, CDW provides a fertile ground for uncovering intriguing intermediate electronic states. Here, we report a Raman spectroscopy study of the PPI and EPC in topological semimetal EuAl4 exhibiting a CDW phase below temperature Tc ~ 145 K. The free-charge-carrier-density (nc) and temperature dependences of the Fano asymmetric factors (1/|q|) of the two phonon modes A1g and B1g indicates that below Tc, the EPC becomes weakened probably due to the reduction of the nc. Interestingly, in the temperature range from 50 to 145 K, the steep growth of the 1/|q| leading to the significant deviation from the linear dependence on the nc, together with the shoulder-like features in the temperature evolutions of the 1/|q| and the nc around 50 K, implies the possible existence of an intermediate electronic state with the EPC distinctly larger than the CDW ground state in EuAl4. Furthermore, below Tc, the faster decrease in the full width at half maxima of the B1g phonon mode representing the collective vibrations of the CDW-modulated Al1 atoms suggests that a remarkable growth of the PPI for the B1g phonon mode after the CDW phase transition, which is in contrast to the weakening of the EPC and thus may mainly arise from the strengthening of lattice anharmonicity in EuAl4. Our results not only highlight the significance of the enhanced PPI and the weakened EPC in completely understanding the formation of the CDW phase but also initiate the exploration of novel intermediate electronic states in EuAl4.