Polymethylpentene (PMP) polymers can be used to make advanced optics, especially for midinfrared (MIR) ultrafast optics. In this study, an optical parametric converter pumped by a Ti sapphire femtosecond laser was used to investigate the polymer. The thermal effect generated by loosely focused femtosecond near mid-infrared (MIR) pulses in bulky materials is observed in real-time, and the polymer exhibits thermal stability and conformability. To avoid strong linear absorption and to increase the nonlinear damage threshold, the spectral region for ultrafast applications is 1310 nm (0.95 eV)–1350 nm (0.92 eV). For the process in region VI, there is a sign of stronger coupling for short-wavelength photons, and the pulse duration is recommended to be lower than 160 fs. In the ultraviolet (UV) region, filamentary writing using a low-focused beam, the laser peak power was selected in the range of 2.2 MW–9.2 MW. High-density bulky gratings were written. The refractive-index modulation was significant, and the polymer exhibited highly nonlinear features. This study provides insights into the applications and production of PMP polymers in laser optics and laser engineering.
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