This paper presents a previously unreported mechanism for the formation of High Spatial Frequency Laser Induced Periodic Surface Structures (HSFL) in GaAs upon irradiation by femtosecond laser pulses (repetition rate = 1 kHz, τ = 150 fs, λ = 390 nm) that is driven by point defect diffusion, desorption of surface atoms, and roughening of the surface. The HSFL have trenches that are 100 nm deep, an average spatial period of 65 nm, and are completely below the original surface. Sub-100 nm periodicity with high depth to period aspect ratio has not been previously observed in GaAs. In the proposed mechanism, laser irradiation generates point defects that diffuse to the surface. Interstitials that reach the surface can be easily desorbed and the remaining vacancies coalesce into vacancy islands. This results in a rough surface, which can excite surface plasmon polaritons. Despite our observations of periodicity corresponding to SPPs, calculations done using the excited dielectric function indicate that SPPs should not be supported. This points to the need to incorporate the cumulative effects of laser irradiation in existing models. This paper also presents evidence that desorption can also occur during HSFL formation in GaAs when irradiated with 780 nm in vacuum. The HSFL have the similar spatial period as GaAs irradiated in air with 780 nm, but completely below the original surface.
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