Tunable Quantum Coherence of Luminescent Molecular Spins Organized via Block Copolymer Self‐Assembly

Abstract Electronic or nuclear spins represent promising candidates of qubits for applications in quantum information technologies and spintronic devices. However, it remains a challenge to achieve scalable and spatially defined organization of a large number of spins as qubits, which is essential in the feasible fabrication of quantum circuits. We report a strategy of block copolymer self‐assembly to organize molecular spins as qubits across molecular to micro‐/nano‐scales in polymeric films of organic luminescent radicals centered in star‐like block copolymers. We have achieved not only scalable and spatially defined organization of the molecular spins in polymeric films with long‐range periodic ordering but also controllable spin‐lattice relaxation dynamics and spin coherence lifetimes that can be finely tuned by the domain sizes and rigidities of the polymeric matrices.