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Although silicon oxynitrides are important semiconductors for many practicalapplications, their potential second-order nonlinear optical (NLO)applications, regardless of balanced or controllable performance, have neverbeen systemically explored. Using the first-principles calculations, in thisarticle, we discover that the sinoite (i.e., typical silicon oxynitride Si2N2O)can simultaneously exhibit wide optical bandgap, strong second-harmonicgeneration (SHG) effect, and large birefringence, which are further confirmedby our preliminary experimental data. Importantly, we propose that alloyingengineering can be further applied to control the balanced NLO properties inthe Si2N2O system. Combining first-principles calculations and clusterexpansion theory, we demonstrate that alloying Ge into Si2N2O can easily formlow formation energy Si2(1-x)Ge2xN2O alloys, which can in turn achievecontrollable phase-matching harmonic output with high SHG efficiency atdifferent energy ranges. Therefore, alloy engineering could provide a uniqueapproach to effectively control the balanced NLO performance ofSi2(1-x)Ge2xN2O, making this polar alloy system holding potential applicationsin tunable laser frequency conversion and controllable all-optical devices.

Alloy Engineering of Polar (Si,Ge)2N2O System for Controllable Second Harmonic Performance