Large-Size Bulk and Thin-Film Stilbazolium-Salt Single Crystals for Nonlinear Optics and THz Generation

We present new stilbazolium salt DSTMS (4‐N,N‐dimethylamino‐4′‐N′‐methyl‐stilbazolium 2,4,6‐trimethylbenzenesulfonate) with both high second‐order nonlinear optical properties and very favorable crystal growth characteristics. We are able to obtain very large area bulk single crystals of more than 3 × 3 × 0.2 cm3 with a high optical quality without using seed crystals by using low‐temperature solution growth. We also demonstrate the growth of single crystalline thin films of DSTMS with an area of up to 6 × 5 mm2 and a thickness between 5–30 μm. Nonlinear optical measurements reveal that DSTMS possesses large nonlinear optical susceptibilities with χ111(2) = (430 ± 40) pm V–1 at 1.9 μm. Highly efficient generation of broadband THz waves with THz electric field strengths of more than 4 kV cm–1 using 160 fs laser pump pulses at a wavelength λ = 1.45 μm and DSTMS crystals has been demonstrated. A nonlinear optical stilbazolium salt DSTMS that yields very large‐area bulk single crystals and single crystalline thin films with good optical quality and high second order susceptibility of 430 pm/V at 1.9 μm has been developed. Highly efficient generation of THz pulses with DSTMS crystals has been demonstrated (see figure).