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Outstanding Laser Damage Threshold in Li2MnGeS4 and Tunable Optical Nonlinearity in Diamond-Like Semiconductors

MetadataDetails
Publication Date2015-02-24
JournalInorganic Chemistry
AuthorsJacilynn A. Brant, Daniel J. Clark, Yong Soo Kim, Joon I. Jang, Ashley Weiland
InstitutionsDuquesne University, University of Ulsan
Citations110

The new Li2MnGeS4 and Li2CoSnS4 compounds result from employing a rational and simple design strategy that guides the discovery of diamond-like semiconductors (DLSs) with wide regions of optical transparency, high laser damage threshold, and efficient second-order optical nonlinearity. Single-crystal X-ray diffraction was used to solve and refine the crystal structures of Li2MnGeS4 and Li2CoSnS4, which crystallize in the noncentrosymmetric space groups Pna21 and Pn, respectively. Synchrotron X-ray powder diffraction (SXRPD) was used to assess the phase purity, and diffuse reflectance UV-vis-NIR spectroscopy was used to estimate the bandgaps of Li2MnGeS4 (Eg = 3.069(3) eV) and Li2CoSnS4 (Eg = 2.421(3) eV). In comparison with Li2FeGeS4, Li2FeSnS4, and Li2CoSnS4 DLSs, Li2MnGeS4 exhibits the widest region of optical transparency (0.60-25 μm) and phase matchability (≄1.6 μm). All four of the DLSs exhibit second-harmonic generation and are compared with the benchmark NLO material, AgGaSe2. Most remarkably, Li2MnGeS4 does not undergo two- or three-photon absorption upon exposure to a fundamental Nd:YAG beam (Ī» = 1.064 μm) and exhibits a laser damage threshold > 16 GW/cm(2).