In this work, we studied single-pulse ablation dynamics of a temporally modulated continuous wave laser-material interaction with Al using in situ multimodal time-resolved diagnostics that describe in detail the associated physical and chemical processes. Time-resolved scattering, emission imaging, and optical emission spectroscopy unveiled a sequence of events spread out across three distinct phases: (i) early phase ablation process, associated with particle generation and liquid Al column formation (<20 μs), (ii) secondary detonation when sufficient ejected material is accumulated over the surface (20-50 μs), and (iii) molten liquid Al pool oscillation on the surface, followed by large droplet ejection from the liquid pool (100-500 μs). Atomic Al and AlO were observed with optical emission spectroscopy at different ratios during the entire lifetime of the event, verifying the formation of oxidized Al vapor upon its interaction with air. Morphological and compositional characterization confirmed surface oxidation and material re-solidification in the form of protrusions produced during the irradiation process. This work provides insights into the complex physical and chemical mechanisms of single-pulse ablation in the sub-millisecond laser pulse regime, which are critically important for parameter optimization in a variety of laser processing, microfabrication, and deposition applications.

Graphite is a key material in a variety of cross-cutting applications in energy conversion, energy storage, and nuclear energy. Recently, temporally modulated continuous wave lasers have been shown to produce well-defined ablation features in graphite at relatively high processing speeds. In this work, we analyze in detail the laser ablation dynamics of single-pulse ablation in the sub-millisecond time regime to elucidate the origins of the resulting well-defined ablation craters using a combination of time-resolved emission imaging, diffuse reflection/scattering imaging, and optical emission spectroscopy. These multimodal in situ diagnostics revealed three main contributors to achieve well-defined ablation features: (1) rapid ejection of particles with ∼100 m/s speed, (2) ablation of the graphite in the gaseous form, and (3) absence of bulk liquid motion, which is typically observed in laser processing of metals. Plasma plume formation was sustained throughout the duration of the laser pulse (500 μs). This work provides insights into the complex physical and chemical mechanisms of sub-millisecond laser-matter interactions, which are critical for parameter space optimization and tailoring of laser machining and drilling processes.