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Data for: Mechanistic insights into laser-generated surface nanomorphology from physics-guided, explainable machine learning and molecular dynamics simulations 

Silicon surface amorphization by short pulse laser irradiation is a phenomenon of high importance for device manufacturing and surface functionalization. To provide insights into the processes responsible for laser-induced amorphization, a multiscale computational study combining atomistic molecular dynamics simulations of nonequilibrium phase transformations with continuum-level modeling of laser-induced melting and resolidification is performed. Atomistic modeling provides the temperature dependence of the melting/solidification front velocity, predicts the conditions for the transformation of the undercooled liquid to the amorphous state, and enables the parametrization of the continuum model. Continuum modeling, performed for laser pulse durations from 30 ps to 1.5 ns, beam diameters from 5 to 70 μm, and wavelengths of 532, 355, and 1064 nm, reveals the existence of two threshold fluences for the generation and disappearance of an amorphous surface region, with the kinetically stable amorphous phase generated at fluences between the lower and upper thresholds. The existence of the two threshold fluences defines the spatial distribution of the amorphous phase within the laser spot irradiated by a pulse with a Gaussian spatial profile. Depending on the irradiation conditions, the formation of a central amorphous spot, an amorphous ring pattern, and the complete recovery of the crystalline structure are predicted in the simulations. The decrease in the pulse duration or spot diameter leads to an accelerated cooling at the crystal–liquid interface and contributes to the broadening of the range of fluences that produce the amorphous region at the center of the laser spot. The dependence of the amorphization conditions on laser fluence, pulse duration, wavelength, and spot diameter, revealed in the simulations, provides guidance for the development of new applications based on controlled, spatially resolved amorphization of the silicon surface. 

Abstract Laser ablation is a process that bears both fundamental physics interest and has wide industrial applications. For decades, the lack of probes on the relevant time and length scales has prevented access to the highly nonequilibrium phase decomposition processes triggered by laser excitation. In this study, a close integration of time-resolved probing by intense femtosecond X-ray pulses with large-scale atomistic modeling has yielded unique insights into the ablation dynamics of thin gold films irradiated by femtosecond laser pulses. The emergence and growth of nanoscale density heterogeneities in the expanding ablation plume, predicted in the simulations, are mapped to the rapid evolution of distinct small angle diffraction features. This mapping enables identification of the characteristic signatures of different phase decomposition processes occurring simultaneously in the plume, which are driven by photomechanical and thermodynamic driving forces. Beyond the specific insights into the ablation phenomenon, this study demonstrates the power of joint X-ray probing and atomistic modeling of material dynamics under extreme conditions of thermal and mechanical nonequilibrium.