PbGa2MSe6 (M = Si, Ge) : Two Exceptional Infrared Nonlinear Optical Crystals

• Two noncentrosymmetric (NCS) quaternary selenides, PbGa2SiSe6 (1) and PbGa2GeSe6 (2), with second-order nonlinear optical (NLO) responses, were synthesized by a conventional high-temperature solid-state reaction method. Compounds 1 and 2 are constructed by three NCS chromophores, [PbSe4], [GaSe4], and [Ga/SiSe4] or [Ga/GeSe4], with the covalent interactions between the X and Se atoms (X = Pb, Ga, Ga/Si, or Ga/Ge). They crystallize in the polar space groups Cc and Fdd2, respectively. Inspiringly, compound 2 is phase-matchable (PM) and shows high laser-induced damage threshold (LIDT) of 3.7 x AgGaS2 and wide transparent region (0.6325 mu m) in the mid-infrared (MIR) region. Most importantly, it presents extraordinary strong second harmonic generation (SHG) at 2.05 mu m radiation of about 12 x AgGaS2 at the particle size of 2545 mu m, which represents the strongest SHG among PM chalcogenides to date. The calculated major SHG tensor elements of compounds 1 and 2 are d31 = 224.7 and d12 = 222.1 pm/V, respectively, while the calculated d36 of AgGaS2 is only 21.2 pm/V.

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NATURVETENSKAP  -- Kemi (hsv//swe)

NATURAL SCIENCES  -- Chemical Sciences (hsv//eng)

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