Non-technical Description: A central goal of Materials Genome Initiative is to predict superior intrinsic material properties on the atomic scale and translate them to superior technologies we can touch and hold. However, most such material discoveries are lost in translation due to the “mesoscale cliff.” Materials promising on the nanoscale may fail in devices where microstructures up to hundreds of micrometer in size dominate device performance. This team addresses this materials challenge to develop a fundamental knowledge base to deploy the next generation of cryogenic electro-optic materials integrated on silicon for chip-scale quantum integrated circuits. The electro-optic effect describes a material’s optical refractive index change upon the application of an electric field. Electro-modulators power our internet today by converting electrical to optical signals. They are also fundamental building blocks for the emerging scalable optical quantum computing hardware, on-chip trapped ion quantum computing schemes and developments in low temperature science. With these, new materials’ challenges arise, in that, electro-optic modulators must now respond in the gigahertz frequency range, be operated at cryogenic temperatures with low energy budget and must be integrated directly on silicon. This requires materials with cryogenic electro-optic coefficients that are many orders of magnitude higher than the current industry standard. In addition, they require large index and low