Second harmonic generation response of the cubic chalcogenides Ba(6-x)Srx[Ag(4-y)Sn(y/4)](SnS4)4
We synthesized the barium/strontium solid solution sequence Ba6-xSrx[Ag(4-y)Sn(y/4)](SnS4)4 for nonlinear optical (NLO) applications in the infrared (IR) via a flux synthesis route. All title compounds are isotypic, crystallizing in the cubic space group I$$\bar{_4}$$ 3d and are composed of a three-dimensional (3D) anionic framework of alternating corner-sharing SnS4 and AgS4 tetrahedra charge balanced by Ba and Sr. The shrinkage of Ba/Sr-S bond lengths causes the tetrahedra in the anionic framework to become more distorted, which results in a tunable band gap from 1.58 to 1.38 eV with increasing x values. The performance of the barium limit (x=0) is also superior to that of Sr (x=6), but surprisingly second harmonic generation (SHG) of the solid solution remains strong and is insensitive to the value of x over the range 0-3.8. Results show that the non-type-I phase-matched SHG produced by these cubic chalcogenides display intensities higher than the benchmark AgGaSe2 from 600 to 1000 nm.
- Research Organization:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Organization:
- National Science Foundation (NSF); Institute for Sustainability and Energy at Northwestern (ISEN); USDOE Office of Science - Office of Basic Energy Sciences - Materials Sciences and Engineering Division
- DOE Contract Number:
- AC02-06CH11357
- OSTI ID:
- 1374187
- Journal Information:
- Journal of Solid State Chemistry, Vol. 248; ISSN 0022-4596
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
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