Journal
ADVANCED OPTICAL MATERIALS
Volume -, Issue -, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adom.202300736
Keywords
high laser-induce damage thresholds; mixed anionic; nonlinear optical materials; tetrahedral units; wide bandgap
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Through introducing fluorination into chalcogenides, a wide bandgap IR NLO material Na3SiS3F with unprecedented [SiS3F] tetrahedra is designed and synthesized. Na3SiS3F exhibits a wide bandgap of 4.75 eV, high laser damage induced threshold (approximately 5 times that of AgGaS2), moderate NLO response, large birefringence, and wide IR transparent region. This research provides a promising IR NLO material for high-power laser applications and opens up a new avenue for the design of new wide bandgap IR NLO materials based on NLO-active [SiSiF4-x] (x = 1, 2, 3) mixed anionic tetrahedral group.
The exploration of antilaser damage wide bandgap infrared (IR) nonlinear optical (NLO) materials is urgent but challenging. Herein, by introducing the idea of fluorination into chalcogenides, a wide bandgap IR NLO material Na3SiS3F with unprecedented [SiS3F] tetrahedra is designed and synthesized. Na3SiS3F shows a wide bandgap of 4.75 eV (the largest one in the reported quaternary metal chalcogenides), resulting in a high laser damage induced threshold of approximate to 5 x AgGaS2 (AGS). Meanwhile, the compound has a moderate NLO response (approximate to 0.3 xAGS) with phase-matching behavior, large birefringence (0.15@1064 nm), and wide IR transparent region. The introduction of fluorine breaks the structural symmetry and broadens the highest occupied molecular orbital-lowest unoccupied molecular orbital (HOMO-LUMO) gap, polarizability anisotropy, and hyperpolarizability of the Si-S tetrahedral unit. The results indicate that Na3SiS3F is a promising IR NLO material for the high-power laser application and open an avenue for the design of new wide bandgap IR NLO materials based on NLO-active [SiSiF4-x] (x = 1, 2, 3) mixed anionic tetrahedral group.
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