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We utilize near-infrared femtosecond pulses to investigate coherent phononoscillations of Ca2RuO4. The coherent Ag phonon mode of the lowest frequencychanges abruptly not only its amplitude but also the oscillation-phase as thespin order develops. In addition, the phonon mode shows a redshift entering themagnetically ordered state, which indicates a spin-phonon coupling in thesystem. Density functional theory calculations reveal that the Ag oscillationsresult in octahedral tilting distortions, which are exactly in sync with thelattice deformation driven by the magnetic ordering. We suggest that thestructural distortions by the spin-phonon coupling can induce the unusualoscillation-phase shift between impulsive and displacive type oscillations.

Strong spin-phonon coupling unveiled by coherent phonon oscillations in Ca2RuO4