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Chalcogenide superlattices (SL) consist of alternately stacked GeTe and Sb 2 Te 3  layers. The structure can act as a 3D topological insulator depending on the constituent layer thicknesses, making the design of the SL period a central issue for advancing chalcogenide SL as potential candidates for spin devices as well as for optimization of the current generation of phase‐change memory devices. Here we explore the periodic structure of chalcogenide SL by observing coherent folded longitudinal acoustic (FLA) phonons excited by femtosecond laser pulse irradiation. The peak frequency of the FLA modes is observed to change upon variation of the thickness of the GeTe layer, which is well reproduced by means of an elastic continuum model. In addition, a new SL structure is unveiled for a sample consisting of thin GeTe and Sb 2 Te 3  layers, which suggests intermixing of Ge atoms. This all‐optical technique based on observation of coherent FLA modes offers a non‐destructive characterization of superlattice structures at atomic resolution.

All‐Optical Detection of Periodic Structure of Chalcogenide Superlattice Using Coherent Folded Acoustic Phonons