Chemically Tuning Quantized Acoustic Phonons in 2D Layered MoO3 Nanoribbons

Molybdenum trioxide (alpha-MoO3) is a 2D layered metal oxide that can be altered in color from transparent white to dark blue with reversible intercalation of zerovalent metals, and whose mechanical properties can be controlled through intercalation. Here, we use Brillouin laser light spectroscopy to map the entire angular dispersion curves of multiple acoustic phonon branches of 2D layered MoO3, directly probing the effects of phonon quantum confinement when the phonon wavelength is comparable to the material thickness. Since acoustic phonons dictate elasticity, we thereby determine the full elastic stiffness tensor and the thickness of each nanoribbon to a statistical precision (derived from standard error propagation) corresponding to less than a monolayer. We show how intercalation of metallic Sn, Co, and Cu can chemically tune the quantized acoustic phonons and elasticity of MoO3 nanoribbons. This work provides the methodology to extract precise elastic constants from complex Brillouin scattering of 2D materials, taking advantage of phonon confinement to capture the complete elastic response with a single scattering geometry.