Observation of dynamical crater-shaped charge distribution in the space–time imaging of monolayer graphene

A better understanding of charge carrier dynamics in graphene is key to improvement of its electronic performance. Here, we present direct space-time visualization of carrier relaxation and diffusion in monolayer graphene using time-resolved scanning electron microscopy techniques. We observed striking fluence-dependent dynamic images, changing from a Gaussian shape to a novel crater-shaped pattern with increasing laser fluence. Such direct observation of dynamic changes in spatial charge distribution is not readily available from the conventional spectroscopic approaches, which reflect essentially overall effective carrier temperature and density. According to our analysis, for this crater-shaped carrier density to occur in aggregated electron-hole pairs in the high fluence regime there exists an unconventional Auger-assisted carrier recombination process to provide effective relaxation channels, most likely involving emission of optical phonons and plasmons, which is dynamically accessible due to a strong temporal overlap among them. The presented model allows us to successfully account for these unexpected phenomena and to quantitatively analyze the observed spatiotemporal behavior.