Femtosecond Engineering of PolyMethylPentene(PMP) Nonlinearity via NA, Spin/orbital angular momentum (OAM), and In-Situ SC Diagnostics

Abstract

While femtosecond vortex beams are widely studied for photonic fabrication, how OAM affects third-order susceptibility, energy deposition, and structural symmetry in transparent polymers remains unclear. To address this gap, we investigate femtosecond vortex beam interactions with polymethylpentene (PMP) to establish OAM control over beam shaping and energy deposition in laser micromachining. A 775 nm femtosecond laser is frequency-doubled to 387.5 nm and phase-shaped by a reflective liquid crystal-spatial light modulator, with OAM imprinted via computer-generated holograms and independently controlled spin via a quarter-wave plate. Theoretical modeling of the tensorial nonlinear polarization, combined with systematic experiments on low-NA filamentation, supercontinuum spectroscopy using an advanced spectrometer, and high-NA inscription with NA = 0.4 and 0.7, reveals that the same $χ^{(3)}$ tensor components govern all regimes. The transition from perturbative to dissipative behavior is determined solely by whether the local intensity exceeds the plasma formation threshold. Through an analytical framework based on the isotropic material model, the key innovation lies in identifying that $χ_{1122}$ governs the energy deposition and plasma threshold, whereas $χ_{1221}$ mediates the transverse nonlinear current and helicity-dependent asymmetry, thereby converting phase topology into permanent chiral structures. This enables OAM-controlled structuring with sub-micrometer feature sizes (approximately 0.43 $μ$m diameter and approximately 200 nm$^2$ area) and localized intensities reaching $10^{14}$--$10^{15}$ W/cm$^2$, providing an engineering framework for deterministic fabrication of chiral waveguides and photonic devices through precise control of topological charge and focusing conditions.