In this work we present the formation of laser induced periodic surface structures (LIPSS) on spin-coated thin films of several model aromatic polymers including poly(ethylene terephthalate), poly(trimethylene terephthalate) and poly carbonate bis-phenol A upon irradiation with femtosecond pulses of 795 and 265 nm at fluences well below the ablation threshold. LIPSS are formed with period lengths similar to the laser wavelength and parallel to the direction of the laser polarization vector. Formation of LIPSS upon IR irradiation at 795 nm, a wavelength at which the polymers absorb weakly, contrasts with the absence of LIPSS in this spectral range upon irradiation with nanosecond pulses. Real and reciprocal space characterization of LIPSS obtained by Atomic Force Microscopy (AFM) and Grazing Incidence Small Angle X-ray Scattering (GISAXS), respectively, yields well correlated morphological information. Comparison of experimental and simulated GISAXS patterns suggests that LIPSS can be suitably described considering a quasi-one-dimensional paracrystalline lattice and that irradiation parameters have an influence on the order of such a lattice. Fluorescence measurements, after laser irradiation, provide indirect information about dynamics and structure of the polymer at the molecular level. Our results indicate that the LIPSS are formed by interference of the incident and surface scattered waves. As a result of this process, heating of the polymer surface above its glass transition temperature takes place enabling LIPSS formation.

Numerical diagonalization of a one-dimensional (1D) Frenkel exciton Hamiltonian with disorder shows that the low-energy part of the 1D localized exciton spectrum has a hidden structure whose energy scale is determined by the exciton localization length. We propose experimental measurements of two exciton optical transitions in linear molecular aggregates as a method to reveal this structure. We also suggest a formula for the enhancement of spontaneous emission rate of the 1D localized Frenkel exciton adequately allowing for its low-energy density of states.

Numerical calculations of the harmonic yield from diatomic molecular ions initially prepared in a highly excited vibrational state show a remarkable enhancement of the harmonic energies in the plateau in terms of the ponderomotive energy. The two-step scheme that explains the mechanism of harmonic generation by atoms is extended to our double potential-well structure, providing an explanation for the high photon energies produced.

We investigate a simply corrected Keldysh-Faisal-Reiss (KFR) rate formula for laser-induced ionization of atoms in the nonperturbative intensity domain. Predictions of the formula are compared, first, with ab initio Floquet calculations, which show good agreement in the nonperturbative intensity domain for not too short wavelengths. Second, they are found to agree with the results of numerical simulations for the H atom, provided the pulse lengths are not shorter than three field cycles, so that the adiabatic rate becomes a valid parameter. Finally, total single-ionization yields predicted by the present model are compared with 36 different experimental data sets for He, Ne, Ar, Kr, and Xe, covering both linear and circular polarizations, and different wavelengths, pulse durations, and intensities; the results show a remarkable overall agreement with the data.

This work demonstrates the formation of femtosecond laser induced periodic surface structures (LIPSS) by multipulse irradiation with the fundamental and 3rd harmonic of a linearly polarized Ti:sapphire laser (795 and 265 nm) on thin films of the polymers poly (ethylene terephthalate), poly (trimethylene terephthalate), and poly (carbonate bisphenol A) prepared by spin-coating. LIPSS, inspected by atomic force microscopy, are formed upon multiple pulse UV and IR irradiation with wavelength-sized period in a narrow range of fluences below the ablation threshold. Control and tunability of the size and morphology of the periodic structures become thus possible ensuring photochemical integrity of polymer films.