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

Scattering between individual charges and collective modes in materials governs fundamental phenomena such as electrical resistance, energy dissipation, switching between different phases, and ordering. The study of such scattering requires a simultaneous access to the ultrafast momentum-resolved dynamics of single-particle and collective excitations, which remains as an experimental challenge. Here, we demonstrate time- and momentum-resolved electron energy-loss spectroscopy, and apply it to graphite showing that large ($\mathrm{\Delta }q\simeq$1.2~Å${}^{-1}$) photoexcited electron-hole (e-h) pockets in the band structure induce a renormalization of the collective in-plane and bulk plasmons that can be described quantitatively by invoking intra- and inter-valley scattering processes mediated by $E_{2g}$ and $A_1^{\mathrm{\prime }}$ phonon modes, which we directly observe by ultrafast electron diffraction and identify via ab initio calculations. Conversely, the photoexcitation of smaller e-h pockets ($\mathrm{\Delta }q\simeq$0.7~Å${}^{-1}$) close to the K point of graphite results in the renormalization of in-plane plasmons, which can only be partially explained by phonon-mediated scattering and thermal expansion. Our results show the importance of combining momentum- and time-resolved information to elucidate microscopic details associated with electronic scattering processes.