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

Barantani, Francesco; Claude, Rémi; Iyikanat, Fadil; Madan, Ivan; Sapozhnik, Alexey A; Puppin, Michele; Weaver, Bruce; LaGrange, Thomas et al. · Sci Adv · 2025

basic_science · Level V

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Abstract

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 (Δ<i>q</i> ≃1.2 Å<sup>-1</sup>) 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 E<sub>2g</sub> and [Formula: see text] phonon modes, which we directly observe via ultrafast electron diffraction and identify via ab initio calculations. Conversely, smaller electron-hole pockets (Δ<i>q</i> ≃0.7 Å<sup>-1</sup>) 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.