Time Domain Spectroscopy of Graphene

Abstract

This dissertation describes the response of graphene and graphene fragments to ultrafast optical pulses. I will first describe how we created few-cycle optical pulses for interacting with the graphene lattice. These pulses are created through filamentation based pulse compression. I studied how the filamentation process can be optimized through simple means to create the shortest possible pulse. I then examine the extent to which graphene can withstand irradiation from intense ultra-fast pulses. I examine both the high intensity regime at which a single laser pulse will ablate the graphene and a more moderate regime that slowly degrades the graphene from long term exposure to ultrafast pulses. The knowledge lets us both identify a safe working regime for driving the graphene lattice with optical fields as well as use ultrafast lasers to create graphene nano-fragments down to 2nm. Next, I explore the ultrafast dynamics of photo-excited graphene. Graphene undergoes electronic band renormalization after photo exciting carriers. By measuring a differential transmission spectrum, small changes to the band structure can be quantified. I will explain how screened exchange and electron phonon self energies provide corrections to the band structure for different times after carrier excitation. Lastly, I will describe measurements that determine the extent of electron-electron correlations in graphene fragments. By measuring the energy of the two photon state and comparing it the lowest energy one photon state in graphene fragments, we can determine the strength of the correlations in graphene systems.