Photorefractive tuning seeded by third-harmonic light in a diamond photonic crystal cavity

Single-crystal diamond nanocavities have tremendous potential for use in quantum and nonlinear optical technologies. The ability to precisely control their resonant frequencies is essential for many applications, and $\textit{in situ}$ tuning is particularly desirable. In this work, we demonstrate deterministic resonance tuning of a diamond nanocavity. We observed a photorefractive effect in concert with the generation of third-harmonic light within the device. This effect blue-shifted the cavity resonance frequency by $20.2\,(2)\,\text{GHz}$, exceeding the cavity linewidth. The shift corresponded to a fractional change in refractive index of $-1.05\,(1)\times10^{-4}$, and its relaxation occurred over several tens of hours. Although photorefraction is a second-order nonlinear effect and has previously not been observed in diamond owing to its vanishing $\chi^{(2)}$, the observed behaviour is consistent with the generation of non-zero $\chi^{(2)}$ by electric fields from charged crystal defects. In addition to allowing tuning of diamond cavities for resonant nonlinear and quantum photonics applications, this observation could enable the realisation of diamond frequency converters and electro-optical modulators that rely on second-order nonlinearity.