Electronic and nuclear spins can function as qubits—the basic unit of quantum computers. Spins are quantum systems containing two or more levels for which a coherent superposition state can be established and manipulated by electromagnetic radiations—recall magnetic resonance techniques ubiquitous in chemistry and biological applications. Spin states that act as qubits can be achieved in inorganic semiconductors as impurities, or in insulators, like diamond, as defect- dopant states. However, key challenges for this class of spin qubit are the limited ability to tailor qubit properties and, especially, to control qubit-qubit distances, and, hence, interactions. In contrast, spins in molecular systems have recently leapt to the forefront as a potential qubit technology with a unique combination of traits. They have the potential to be operated in the solid-state and at room-temperature. They exhibit ultrafast (ns to ps) gate operations, which lowers the requirement for coherence times. Coherence times for molecular qubits can be 10^4 to 10^6 times longer than gate operations. Beyond this, they address the challenges faced by spins associated with inorganic impurities or defect-states. Namely, concepts from supramolecular chemistry can be applied to prepare discrete multiple-qubit constructs, while crystalline coordination polymer chemistry, e.g., in the form of metal-organic frameworks or covalent- organic frameworks, offers a strategy for organizing qubits into extended arrays.

In this workshop, we will delve into the theoretical basis for molecular spin systems as important building blocks for next-generation quantum information systems, spanning fundamental spin- phonon relaxation processes, spin-spin entanglement control, and spin-photon entanglement and transduction, including use of quantum-photon sources and photonic cavities. We will also discuss the advanced characterization tools and methods being used to explore and exploit these systems, including electron paramagnetic resonance spectroscopy and optical, magnetic and scanning probe techniques. Finally, we will focus on the chemical synthesis of molecules, their assemblies and hybrid materials most promising for realizing key quantum phenomena of coherence, entanglement and transduction.