Journal
ADVANCED OPTICAL MATERIALS
Volume -, Issue -, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adom.202202147
Keywords
double alkaline-earth metal chalcogenides; infrared nonlinear optical; open framework; second harmonic generation; structure-property relationship
Categories
Funding
- National Natural Science Foundation of China
- Natural Science Foundation of Tianjin
- [52172006]
- [22071179]
- [51972230]
- [51890864]
- [51890865]
- [20JCJQJC00060]
- [21JCJQJC00090]
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In this study, new infrared nonlinear optical crystals with outstanding performance were successfully designed and synthesized. These crystals achieve the optimal balance between large second harmonic generation response and wide band gap, and have significant potential for practical applications.
Infrared nonlinear optical (IR NLO) crystals are of quite significance in the development of laser technology, yet rationally designing new IR NLO crystal that can satisfy all the property requirements is still a great challenge owing to the incompatibility between large second harmonic generation (SHG) response and wide band gap. Herein, taking AgGaS2 (AGS) as the template and using highly electropositive alkaline-earth metal cations substituting Ag+ cations, the first examples of double alkaline-earth (Ae) metal chalcogenide IR NLO crystals, AeMg(6)Ga(6)S(16) (Ae = Ca, Sr, Ba), are successfully designed and synthesized. Structurally, they possess stable [Mg/Ga-S](infinity) open frameworks, which can accommodate a wide range of cations from the small size of Ca2+ to large Ba2+ cations and all of the resulting compounds melt congruently. More importantly, these materials achieve the optimal balance among the critical performance parameters, including the strong SHG response (approximate to 0.7-0.8 x AGS) and wide band gap (E-g = 3.50-3.54 eV). Theoretical calculations and structure analysis reveal that their superior NLO properties can be attributed to the synergistic contribution of the polarizable MgS6 and GaS4 groups.
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