“…Acoustic and optical phonons affect fundamental physical properties such as the conduction of sound and heat. For two-dimensional (2D) materials (1,2), van der Waals heterostructure devices (3), topological insulators (4,5), and thermoelectric materials (6)(7)(8), as well as many other materials systems relevant to fields spanning catalysis, biomedical, condensed matter physics, and chemistry, vibrational properties can depend on nano-and atomic-scale structure. However, until now, techniques available to probe the momentum transfer (ℏq) dependence or dispersion of these vibrational modes have been limited to essentially bulk approaches, such as inelastic neutron and x-ray scattering spectroscopies (9,10), reflection electron energy loss spectroscopy (REELS) measuring the average surface response (11,12), or optical techniques limited to q ~0 (where q is the wave vector) (13)(14)(15)(16)(17).…”