Technologies including magnetorheological finishing and CNC polishing are commonly used to finish optical elements, but these methods are often expensive, generate waste through the use of fluids or abrasives, and may not be suited for specific freeform substrates due to the size and shape of finishing tools. Pulsed laser polishing has been demonstrated as a technique capable of achieving nanoscale roughness while offering waste-free fabrication, material-specific processing through direct tuning of laser radiation, and access to freeform shapes using refined beam delivery and focusing techniques. Nanosecond and microsecond pulse duration radiation has been used to perform successful melting-based polishing of a variety of different materials, but this approach leads to extensive heat accumulation resulting in subsurface damage. We have experimentally investigated the ability of femtosecond laser radiation to ablate silicon carbide and silicon. By substituting ultrafast laser radiation, polishing can be performed by direct evaporation of unwanted surface asperities with minimal heating and melting, potentially offering damage-free finishing of materials. Under unoptimized laser processing conditions, thermal effects can occur leading to material oxidation. To investigate these thermal effects, simulation of the heat accumulation mechanism in ultrafast laser ablation was performed. Simulations have been extended to investigate the optimum scanning speed and pulse energy required for processing various substrates. Modeling methodologies and simulation results will be presented.