Second harmonic generation response of the cubic chalcogenides Ba(_6-x)Sr_x[Ag(_4-y)Sn(_y/4)](SnS₄)₄

Journal Article · Tue Jan 31 23:00:00 EST 2017 · Journal of Solid State Chemistry

DOI:https://doi.org/10.1016/j.jssc.2017.01.025· OSTI ID:1374187

Haynes, Alyssa S.; Liu, Te-Kun; Frazer, Laszlo; Lin, Jyun-Fan; Wang, Shuo-Yu; Ketterson, John B.; Kanatzidis, Mercouri G.; Hsu, Kuei-Fang

We synthesized the barium/strontium solid solution sequence Ba_6-xSr_x[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 Laboratory (ANL)
• 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, Journal Name: Journal of Solid State Chemistry Vol. 248; ISSN 0022-4596
• Publisher: Elsevier
• Country of Publication: United States
• Language: English