Coupling of phonons with orbital dynamics and magnetism in CuSb$_2$O$_6$

TL;DR

This study uncovers a novel electron-phonon interaction in CuSb$_2$O$_6$ through the coupling of phonons with orbital excitations, revealing complex dynamics and magnetic correlations above the magnetic ordering temperature.

Contribution

It provides the first direct observation of coupled orbital and vibrational excitations and details their interaction and effects in CuSb$_2$O$_6$.

Findings

Orbital wave at ~550 cm$^{-1}$ softens with temperature.

Strong interference between orbital wave and phonon at ~500 cm$^{-1}$.

Phonon anomalies indicate one-dimensional magnetic correlations above $T_N^{3D}$.

Abstract

Strongly interacting phonons and orbital excitations are observed in the same energy range for CuSb$_2$O$_6$, unlocking a so-far unexplored type of electron-phonon interaction. An orbital wave at $\sim 550$ cm$^{-1}$ softens on warming and strongly interferes with a phonon at $\sim 500$ cm$^{-1}$, giving rise to a merged excitation of mixed character. An electronic continuum grows on warming to the orbital ordering temperature $T_{OO}$=400 K, generating an important phonon decay channel. This direct and simultaneous observation of orbital and vibrational excitations reveals details of their combined dynamics. In addition, phonon frequency anomalies due to magnetic correlations are observed below $\sim 150$ K, much above the three-dimensional magnetic ordering temperature $T_N^{3D}=8.5$ K, confirming one-dimensional magnetic correlations along Cu-O-O-Cu linear chains in the paramagnetic state.