Observation of Crystalline Nonlocal Volume Plasmon Waves

Abstract

In plasmonics, nonlocal effects arise when the material response to optical excitations is strongly dependent on the spatial correlations of the excitation. It is well known that a classical free electron gas system supports local Drude volume plasmon waves. Whereas a compressible quantum electron gas system sustains hydrodynamic volume plasmons with nonlocal dispersion isotropic across all high-symmetry directions. Here, distinct from Drude and Hydrodynamic plasmon waves, we present the first observation of crystalline nonlocal volume plasmon waves. We use transmission-based momentum-resolved electron energy loss spectroscopy to measure the volume plasmon dispersion of silicon along all the fundamental symmetry axes, up to high momentum values ($q \sim 0.7$ reciprocal lattice units). We show that crystalline nonlocal plasmon waves have a prominent anisotropic dispersion with higher curvature along the light-mass ($\Gamma K$ \& $\Gamma L$) axes, compared to the heavy-mass ($\Gamma X$) axis. We unveil the origin of this phenomenon by experimentally extracting the anisotropic Fermi velocities of silicon. Our work highlights an exquisite nonlocality-induced anisotropy of volume plasmon waves, providing pathways for probing many-body quantum effects at extreme momenta.