We develop a theoretical framework for probing moiré phonon modes using Raman spectroscopy, and illustrate it with the example of twisted bilayer graphene (TBG). These moiré phonons arise from interlayer sliding motion in twisted two-dimensional materials and correspond to fluctuations of the stacking order in reconstructed moiré superlattices. These include both acousticlike phason modes and a set of low-energy optical modes originating from the zone folding of monolayer graphene's acoustic modes, which are accessible via Raman spectroscopy. We show that the Raman response of TBG exhibits a series of low-frequency peaks that clearly distinguish it from that of decoupled layers. We further examine how anharmonicity and angle disorder affect the Raman spectra. Our findings establish Raman spectroscopy as a powerful tool for exploring moiré phonons in a broad class of twisted van der Waals systems.

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• Phonons
• Twistronics
• Dichalcogenides
• Twisted bilayer graphene
• Raman spectroscopy