Experimental ​ Study of ​Avalanche ​Ionization in the ​Femtosecond ​ Breakdown of ​Atomic ​Layered ​Materials

The engine of modern society is fueled by information, and the desire to obtain, process and relay it ever more quickly is motivation for scientists to dig deeper into pathways that enable this endgame. The implementation of ever-quicker computer processors, optical fiber-based communications, and Light Radar (LiDar) for climate studies are a small subset that illustrate how ubiquitous the applications of optics are. In this context, the study of 2D materials (2DMs) is important due to the fascinating properties they exhibit that could lead to a plethora of future opto-electronic applications that extend beyond what silicon alone can provide. The story began with graphene due to its high conductivity and tensile strength, but due to the difficulty of switching its conductivity, applications in transistors is limited, and other materials such as the transition metal dichalcogenides (TMDs) MoS2 and WS2, which exhibit a bandgap transition from indirect to direct when going from bulk to monolayer, are being explored. The wide bandgap semiconductor hexagonal boron nitride (hBN) has also been piquing interest. The presence of room-temperature stable excitons detected via various spectroscopies suggests applicability in mainstream field-effect transistors, and current industry direction towards so-called ‘nanosheet’ and ‘nano-wire’ channel transistors serve as prime examples of the relevant applicability of such 2D materials. Quantum computing and valley-tronic applications have also been reported [5], making this class of material exciting to study.
When material dimensions are reduced to the single atomic layer (‘monolayer’) limit, fast carrier dynamics become important that can only be investigated by even faster phenomena i.e., femtosecond ‘ultrafast’ laser pulses. When exposed to intense electric fields, several processes can occur; multiphoton absorption (MPA) which utilizes multiple photons to promote a single charge carrier to the conduction band (CB), tunneling ionization (TI) in which the laser field modifies the inter-atomic potential and allows CB access via tunneling, and avalanche ionization (AI) where inter-carrier impact causes ionization. Together, these strong-field ionization (SFI) processes are subject to significant research effort. If SFI-induced excited carrier populations exceed a threshold, damage occurs via a non-thermal ‘ablation’ process typically used for cutting and patterning.
The objective of this work was to explore the ultrafast optical dielectric breakdown (ODB) behavior of 2DMs such as MoS2, WS2, and hBN. The work involves an investigation of the etalon interference effect that causes differences in the ablation threshold fluence for the same material when placed on different substrates, differences in threshold fluence between different 2DMs, as well as an exploration of laser-induced defects added when multiple ultrafast pulses are incident on the material. ODB for the wide bandgap insulator hBN is also demonstrated and characterized using various imaging modalities and spectroscopies for the first time. Through the findings presented in this work, we begin to unravel some aspects of the nature of ablation, particularly the dominance of avalanche ionization as the key carrier generation mechanism in the ODB process in 2D materials. We also establish femtosecond laser direct writing as a useful tool for the nanopatterning of such 2DMs.