Ultrafast momentum-resolved visualization of the interplay between phonon-mediated scattering and plasmons in graphite

Scattering between charges and collective modes in materials governs phenomena such as electrical resistance, energy dissipation, and phase switching. Studying such scattering requires simultaneous access to ultrafast and momentum-resolved dynamics of single-particle and collective excitations, which remains an experimental challenge. Here, we present time- and momentum-resolved electron energy loss spectroscopy, and we apply it to graphite, demonstrating that large (Δq ≃1.2 Å−1) photoexcited electron-hole pockets induce a renormalization of in-plane and bulk plasmons. This effect is explained by intra- and intervalley scattering processes mediated by E2g and A′1 phonon modes, which we directly observe via ultrafast electron diffraction and identify via ab initio calculations. Conversely, smaller electron-hole pockets (Δq ≃0.7 Å−1) result in the renormalization of in-plane plasmons, which can only be partially explained by phonon-mediated scattering and thermal expansion. Our results highlight the importance of combining momentum- and time-resolved information to elucidate electronic scattering processes.