Broadband THz Wave Generation and Detection in Organic Crystal PNPA at MHz Repetition Rates

Organic nonlinear optical (NLO) crystals have emerged as efficient room-temperature emitters of broadband THz radiation with high electric field strengths. Although initially confined to high-pulse-energy excitation in the millijoule range with kHz rates, recent efforts have focused on tailoring the physical properties of organic NLO materials for compatibility with popular MHz-rate telecommunication wavelength lasers emitting nanojoule energy pulses. This is motivated by the large potential of such crystals for more portable and user-safe spectroscopic systems, additionally complemented by their room-temperature field-sensitive THz detection capabilities. In this work, the MHz-rate operation of the organic crystal PNPA ((E)-4-((4-nitrobenzylidene)amino)-N-phenylaniline), which was recently discovered through data mining algorithms and reported to surpass the conversion efficiency of rivaling NLO crystals at 1 kHz repetition rate is demonstrated. Using a compact 200 mW Er:fiber laser producing 18 fs pulses at 50 MHz repetition rate, the THz field generation and detection capabilities of PNPA via performing gas phase spectroscopy in the 1.3–8.5 THz range are demonstrated. A dynamic range of 40 dB over 3.6 s and 70 dB over 2 h is obtained. The work extends the family of organic crystals compatible with telecommunication-wavelength excitation using nJ pulses for spectroscopy beyond 5 THz.