Mixed (FAPbI3)₀.₉₂(MAPbBr3)₀.₀₈ perovskite thin films exhibit strong nonlinear optical responses, rendering them promising candidates for applications in photonics and optical communications. In this work, we present a systematic study on the ultrafast third-order nonlinear optical processes in mixed perovskite nanocrystals (NCs) by exploring the generation of third harmonic radiation and giant two-photon absorption-based photoluminescence (PL) when excited by femtosecond laser pulses of a 1030 nm central wavelength. A comparative analysis of the coherent third harmonic generation in the thin-film-containing perovskite nanocrystals has shown a 40× enhancement of the third harmonic signal compared to the signal generated in the pure quartz substrate. The cubic dependence of the third-nonlinear optical response of the (FAPbI₃)₀.₉₂(MAPbBr₃)₀.₀₈ perovskites on the intensity of the driving radiation was identified using broadband 38 femtosecond driving pulses. The positive nonlinear refractive index (γ = +1.4 × 10⁻¹² cm²·W⁻¹) is found to play an important role in improving the phase-matching conditions of the interacting pulses by generating a strong third order harmonic. The giant two-photon absorption (TPA)-assisted PL peak was monitored and a blue shift of the PL was obtained in the higher intensity range of the laser pulses, with the absorption coefficient β estimated to be~+7.0 cm·MW⁻¹ at a 1030 nm laser wavelength.

Ultrafast laser ablation of metal surfaces is a common physical process used to generate periodic surface structures with tuneable multifunctionality for various applications in science and technology. In this work, the formation of femtosecond laser-induced periodic surface structures (LIPSSs) is investigated with 50 kHz repetition rate laser of 40 fs pulse duration and a central wavelength ( λ w = 1030 nm ) along with its second ( λ 2 w = 515 nm ) and third ( λ 3 w = 343 nm ) harmonic components. The variation in the LIPSS periodicity is demonstrated by changing the wavelength of the ablating laser pulses. LIPSS with periodicity ∼0.85 μ m at the fundamental ablating pulses, ∼0.42 μ m periodicity at the second harmonic, and ∼0.35 μ m periodicity at the third harmonic were observed. The third harmonic radiation was generated in an air-filament with minimal temporal delay with respect to the fundamental driving pulses to structure Nickel surfaces at ambient conditions. The approach demonstrates the potential for generating very fine LIPSS on materials’ surfaces using the efficient high-order harmonics of an infrared fundamental laser beam.