New strategy for designing promising mid-infrared nonlinear optical materials: narrowing the band gap for large nonlinear optical efficiencies and reducing the thermal effect for a high laser-induced damage threshold.

Abstract

To circumvent the incompatibility between large nonlinear optical (NLO) efficiencies and high laser-induced damage thresholds (LIDTs) in mid-infrared NLO materials, a new strategy for designing materials with both excellent properties is proposed. This strategy involves narrowing the band gap for large NLO efficiencies and reducing the thermal effect for a high LIDT. To support these proposals, a series of isostructural chalcogenides with various tetrahedral center cations, Na2Ga2MQ6 (M = Ge, Sn; Q = S, Se), were synthesized and studied in detail. Compared with the benchmark AGS, these chalcogenides exhibit significantly narrower band gaps (1.56-1.73 eV, AGS: 2.62 eV) and high NLO efficiencies (1.6-3.9 times that of AGS at 1910 nm), and also outstanding LIDTs of 8.5-13.3 × those of AGS for potential high-power applications, which are contrary to the conventional band gap view but can be attributed to their small thermal expansion anisotropy, surmounting the NLO-LIDT incompatibility. These results shed light on the search for practical IR NLO materials with excellent performance not restricted by NLO-LIDT incompatibility.