Enriched silicon is critical for silicon quantum devices since the 29Si isotope is a leading contributor to qubit decoherence. Enriching silicon leads to long quantum coherence times (T2) measured by ESR and in qubit fidelity studies. In this project, we produce crystalline thin films of 28Si enriched to >99.9999% directly from natural abundance silane, a novel approach that allows us to produce the most highly enriched silicon in the world. We are depositing this silicon onto natural silicon substrates and using it to fabricate electronic and quantum devices that provide feedback for refinement of the silicon and other materials used to fabricate the qubits. Additionally, we are exploring novel dopant schemes to enable superconducting-semiconducting materials or direct coupling to photon states that can preserve quantum information.