Competition Pathways of Energy Relaxation of Hot Electrons through Coupling with Optical, Surface, and Acoustic Phonons

The hot electrons in carbon-based materials exhibit interesting ballistic transport behaviors for designing high-performance single-electron transistors. However, the cooling of such hot electrons back to the equilibrium state may be slowed down by the excessively populated optical phonons, thus limiting their ballistic transport. Therefore, a thorough understanding of the coupling between hot electrons and optical phonons is of critical importance. Here, by varying the thickness of a multilayer graphene film on a supporting substrate, we investigated the competition pathways of the energy relaxation of the photoinduced hot electrons through coupling with the optical, surface, and acoustic phonons. The difference in the τ2 values indicates that thickness plays an important role in the optical phonon population. For the multilayer graphene film thickness less than 3 nm, the super-collision model describes the hot electron cooling dynamics that is strongly affected by the surface phonons from the supporting substrate. As the multilayer graphene film thickness increases from 3 to 20 nm, the accumulation of the optical phonons induces a hot optical phonon effect, resulting in a bottleneck of cooling of the hot electrons. As the multilayer graphene film thickness further increases from 20 to 40 nm, a direct coupling between the hot electrons and acoustic phonons starts to dominate. The surface states of the interfaces at the inner layers of the multilayer graphene film contribute to this direct coupling as an additional cooling channel. The quantitative understanding of the energy relaxation pathways of the hot electrons offers insights into designing high-performance single-electron transistors.

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