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We report GHz longitudinal as well as shear acoustic phonons photoexcitationand photodetection using femtosecond laser pulses in a spin-crossover molecularcrystal. From our experimental observation of time domain Brillouin scatteringtriggered by the photoexcitation of acoustic waves across the low-spin (LS) tohigh-spin (HS) thermal crossover, we reveal a link between molecular spin stateand photoexcitation of coherent GHz acoustic phonons. In particular, weexperimentally evidence an unconventional non-thermal pathway for the laserexcitation of GHz phonons. We also provide experimental insight on the opticaland mechanical parameters evolution across the LS/HS spin crossover temperatureT$_{1/2}$.

applied physics letters

Ultrafast non-thermal laser excitation of gigahertz longitudinal and  shear acoustic waves in spin-crossover molecular crystals  [$Fe(PM-AzA)_{2}$$(NCS)_{2}$]