📝 SummarXiv

Abstract

Molecular electron spin qubits offer atomic-level tunability and room-temperature quantum coherence. Their integration into engineered solid-state matrices can enhance performance towards ambient quantum information technologies. Herein, we demonstrate covalent organic frameworks (COFs) as programmable matrices of stable organic radical qubits allowing strategic optimization of spin-phonon and spin-spin interactions. Using two classic boronate-ester frameworks, COF-5 and COF-108, to host semiquinone-like radical qubits, we achieve ultralong spin relaxation time (T1 > 300 {\mu}s) at 298 K, which outperforms most molecular qubits and rivals inorganic spin defects. The suppression of spin relaxation is attributed to rigid and neutral structures as well as carbon-centered spin distributions that effectively weaken spin-phonon coupling. Employing dynamical decoupling methods to both COFs improves their quantum coherence and enables room-temperature detection of nuclear spins including 1H, 11B, and 13C. Our work establishes COFs as designer quantum materials, opening new avenues for quantum sensing of nuclear spins at room temperature.