Quantum information technologies necessitate the development of materials systems that can coherently store and manipulate quantum states well enough for error correction. Color centers in solids (“artificial atoms”) have emerged as leading candidate systems, promising to combine the favorable coherence properties of isolated atoms with the scalability and stability of solid-state technologies. In this Perspective, we break down the challenges associated with modeling quantum phenomena in multiqubit solid-state material systems, leveraging advances in high-performance supercomputing and algorithms in computational physics.

Exascale high-performance computing will be able to bring quantitative accuracy to multiqubit calculations in the next few years—greatly speeding up the identification, characterization, and optimization of novel solid-state quantum materials. This dramatic increase in computational power has enabled scientists to study how the coupled nuclear, electronic, and photonic degrees of freedom interact in materials. We provide a forward-looking view on how recent advances at the intersection of materials physics and quantum information can accelerate the discovery and development of new and improved solid-state qubits. In particular, we present new computational approaches for performing large-scale simulations of multiqubit systems using ab initio methods, quantum embedding methods, and open quantum system techniques. We provide a theorists’ point of view on the rational design of multiqubit systems using these new computational approaches. Our Perspective identifies a path for bridging the gap between the model Hamiltonians used to develop quantum algorithms and control sequences and the ab initio calculations used to understand and characterize single solid-state-based qubits.