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Breaking inversion symmetry in solids plays a central role in nonlinearoptics because it can change material properties, such as producing even-ordernonlinear optical (NLO) effects. Although a centrosymmetric diamond has beendeveloped as a photonic platform, including waveguides and light sources, theNLO effects in bulk diamonds are limited to the third-order. Thus, exploitingmore powerful second-order NLO effects, such as second harmonic generation(SHG), are still challenging. Here we explore symmetry-breaking-inducedsecond-order NLO effects in bulk diamonds using the color center,nitrogen-vacancy center. Exciting with ultrashort laser pulses, SHG andthird-harmonic generation (THG) are simultaneously observed at the same time,exhibiting characteristic intensity patterns, depending on both the excitationfluence and the angle of light polarization. We uncovered that SHG serves asthe source for THG by the cascading process. Our findings will offer NLOeffect-based quantum sensing by diamond color centers, such as imaging of theelectromagnetic field by electro-optic effects on the nanofemto scale.

Second-Harmonic Generation in Bulk Diamond Based on Inversion Symmetry Breaking by Color Centers