Electron cooling in graphene enhanced by plasmon–hydron resonance

Abstract Evidence is accumulating for the crucial role of a solid’s free electrons in the dynamics of solid–liquid interfaces. Liquids induce electronic polarization and drive electric currents as they flow; electronic excitations, in turn, participate in hydrodynamic friction. Yet, the underlying solid–liquid interactions have been lacking a direct experimental probe. Here we study the energy transfer across liquid–graphene interfaces using ultrafast spectroscopy. The graphene electrons are heated up quasi-instantaneously by a visible excitation pulse, and the time evolution of the electronic temperature is then monitored with a terahertz pulse. We observe that water accelerates the cooling of the graphene electrons, whereas other polar liquids leave the cooling dynamics largely unaffected. A quantum theory of solid–liquid heat transfer accounts for the water-specific cooling enhancement through a resonance between the graphene surface plasmon mode and the so-called hydrons—water charge fluctuations—particularly the water libration modes, which allows for efficient energy transfer. Our results provide direct experimental evidence of a solid–liquid interaction mediated by collective modes and support the theoretically proposed mechanism for quantum friction. They further reveal a particularly large thermal boundary conductance for the water–graphene interface and suggest strategies for enhancing the thermal conductivity in graphene-based nanostructures.