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In Eu2ZnIrO6, effectively two atoms are active i.e. Ir is magneticallyactive, which results in complex magnetic ordering within the Ir sublattice atlow temperature. On the other hand, although Eu is a van-vleck paramagnet, itis active in the electronic channels involving 4f 6 crystal-field split levels.Phonons, quanta of lattice vibration, involving vibration of atoms in the unitcell, are intimately coupled with both magnetic and electronic degrees offreedom (DoF). Here, we report a comprehensive study focusing on the phonons aswell as intra-configurational excitations in double-perovskite Eu2ZnIrO6. Ourstudies reveal strong coupling of phonons with the underlying magnetic DoFreflected in the renormalization of the phonon self-energy parameters wellabove the spin-solid phase (TN ~ 12 K) till temperature as high as ~ 3TN,evidences broken spin rotational symmetry deep into the paramagnetic phase. Inparticular, all the observed first-order phonon modes show softening of varyingdegree below ~3TN, and low-frequency phonons become sharper, while thehigh-frequency phonons show broadening attributed to the additional availablemagnetic damping channels. We also observed a large number of high-energymodes, 39 in total, attributed to the electronic transitions between 4f-levelsof the rare-earth Eu3+ ion and these modes shows anomalous temperatureevolution as well as mixing of the crystal-field split levels attributed to thestrong coupling of electronic and lattice DoF.

Coupling of lattice, spin and intra-configurational excitations of Eu3+ in Eu2ZnIrO6