Organic non-linear optical (NLO) materials hold the promise of realizing blue, second harmonic generation (SHG) semiconductor lasers, which have versatile applications due to their large nonlinearities. Among the organic NLO materials known today, conjugated benzene derivative compounds, which have been studied most extensively, have the largest non-linear effects. At the same time, they often have large birefringences and a red-shifted cut-off (>500 nm). These shortcomings have significantly influenced their applications in frequency doubling. 3-Methoxy-4-hydroxy-benzaldehyde (MHBA), grown in our laboratory, is an excellent organic NLO material. Its cut-off is at 375 nm, but it still has large NLO coefficients and relatively small birefringences [1,2]. Even so, MHBA still cannot realize non-critical phase matching (NCPM) in the spectral region of the GaA1As series laser, which is an important factor influencing the blue SHG of lower power laser diodes. Recently, SHG in an organic single-crystalline optical waveguide demonstrated new potentials in laser diode frequency doubling [3, 4]. In this letter, we describe the growth and characterization of MHBA single-crystalline film. MHBA single-cryStalline film was prepared by the Bridgman method. Before film growth, two polished fused quartz substrates (20 x 30mm) were thoroughly cleaned. The paired substrates were dipped into the MHBA melt in a glass tube controlled at a temperature of 95 °C (compared with its melting point of 83 °C). Capillary action ensured that the melt could penetrate into the gap between the two substrates. When the temperature cooled to room temperature the film in the gap was composed of randomly oriented small crystals. After melt penetration, the film inside the substrates was recrystallized to make a large-area single-crystalline film, using the apparatus shown in Fig. 1. The MHBA polycrystalline film inside the paired substrates was suspended and lowered through the growth region in a stove at a motor-controlled rate of 0.3 mmh -1 for recrystallization. In our experiments, the largest area of the grown film was up to 10 x 10 ram. The quality of the prepared film depended on several factors: the cleaning and polishing of the substrates, the temperature distribution in the stove, the stability of the whole growth apparatus, the down speed of the substrates and the purity of raw materials.
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