Order quantification during laser-induced periodic surface structures (LIPSS) formation in polymer semiconductors

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Abstract
In this work, Grazing Incidence Small-Angle X-ray Scattering (GISAXS) is employed as an in situ, real-time technique to monitor the formation of laser-induced periodic surface structures (LIPSS) on semiconducting polymer (PCDTBT) thin films, complemented by ex-situ Atomic Force Microscopy (AFM) analysis by using the recently proposed code REGUΛARITY. Special emphasis is placed on comparing real-space and reciprocal-space approaches to assess the degree of structural order during LIPSS formation. Both methodologies consistently describe the process through a three-stage mechanism comprising incubation, growth, and stabilization. While real-space analysis provides local information at the micrometer scale, reciprocal-space measurements via GISAXS enable statistical averaging over larger surface areas, revealing complementary aspects of structural evolution. The comparison highlights that spatial heterogeneity dominates during the incubation stage, whereas a progressive increase in long-range order is observed during growth and stabilization. The combination of AFM-based Fourier analysis and GISAXS diffraction enables a quantitative evaluation of ordering, including the detection of higher-order contributions associated with improved structural coherence. These results demonstrate that the joint use of real-space and reciprocal-space techniques provides a comprehensive framework for understanding the kinetics and ordering mechanisms of LIPSS formation in semiconducting polymers.

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