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Second-harmonic generation (SHG) is a common technique with many applications. Common inorganic single-crystalline materials used to produce SHG light are effective using short IR/visible wavelengths but generally do not perform well at longer, technologically relevant IR wavelengths such as 1300, 1550, and 2000 nm. Efficient SHG materials possess many of the same key material properties as terahertz (THz) generators, and certain single-crystalline organic THz generation materials have been reported to perform at longer IR wavelengths. Consequently, this work focuses on characterizing three efficient organic THz generators for SHG, namely, DAST (trans-4-[4-(dimethylamino)-N-methylstilbazolium] p-tosylate), DSTMS (4-N,N-dimethylamino-4’-N’-methylstilbazolium 2,4,6-trimethylbenzenesulfonate), and the recently discovered generator PNPA ((E)-4-((4-nitrobenzylidene)amino)-N-phenylaniline). All three of these crystals outperform the beta-barium borate (BBO), an inorganic material commonly used for SHG, using IR pump wavelengths (1200–2000 nm). 

Organic nonlinear optical (NLO) crystals are among the most efficient (>1%) terahertz (THz) radiation generators. However, one of the limitations of using organic NLO crystals is that the unique THz absorptions in each crystal make it difficult to obtain a strong, smooth, and broad emission spectrum. In this work, we combine THz pulses from two complementary crystals, DAST and PNPA, to effectively fill in spectral gaps, creating a smooth spectrum with frequencies out to 5 THz. The combination of pulses also increases the peak-to-peak field strength from 1 MV/cm to 1.9 MV/cm.