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Abstract Yellow organic crystals, like BNA, MNA, and NMBA, can be used to generate terahertz (THz) pulses of light through optical rectification of infrared ultrafast laser pulses. When producing THz with these organic crystals, one needs to consider that 1) their damage thresholds are low due to having low melting points and 2) Fresnel reflection losses due to multiple interfaces reduce the efficiency of the generated THz output. In this work, new heterogeneous multi‐layer “sandwich” structures are developed with these yellow organic crystals by 1) fusing them to sapphire plates to permit the crystal to withstand higher laser fluences and 2) using an index‐matching fluid (liquid crystal MBBA) to decrease Fresnel reflection losses and improve the THz output. It is shown that the sapphire plates increase the damage threshold of these yellow organic crystals by a factor of two or more, thus allowing the crystals to generate higher THz electric fields. Furthermore, it is shown that the THz light output efficiency increases by assembling the yellow crystals into multi‐layered sandwich structures. For some yellow organic crystals, the sandwich structures increase the THz intensity by more than a factor of two. 

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). 

We have improved the THz output and damage threshold of yellow organic THz generation crystals by fusing them to sapphire and using liquid crystals as index matching fluid to reduce reflective losses. 

We present the optical and THz properties of highly efficient organic nonlinear optical crystals PNPA and MNA. These crystals outperform industry standards in broadband THz generation through optical rectification of IR light pulses. 

We have improved the THz output and damage threshold of yellow organic THz generation crystals by fusing them to sapphire and using liquid crystals as index matching fluid to reduce reflective losses. 

We recently developed new organic nonlinear optical crystals for THz generation. We report the optical and THz properties of PNPA and MNA and discuss how they pave the way for the future of THz spectroscopy.