Two-Step Relaxation of Non-Equilibrium Electrons in Graphene: The Key to Understanding Pump–Probe Experiments

Abstract

In the majority of experiments targeting nonlinear optical phenomena, the application of high-intensity pulses drives electrons in graphene into a strongly non-equilibrium state. Under these conditions, conventional perturbation theory falls short in explaining graphene’s intricate optical response because of significant deviations in electron distribution over energy states from the equilibrium Fermi-Dirac one. In this work, we present a two-step relaxation model capable of predicting the transient dynamics of graphene’s carriers out of equilibrium, from the generation of spectrally narrow populations of non-thermalized electrons and holes to the establishment of a hot-electron gas and its subsequent cooling toward equilibrium with the crystal lattice. By comparing our model calculations to experimental results, we demonstrate its reliability and relevance to pump–probe experiments, providing insights into the pivotal role of hot electrons in comprehending ultrafast dynamics in graphene.

Keywords

• graphene
• hot electrons
• pump–probe spectroscopy
• nonlinear optics