Enhancing Spin Coherence in Optically Addressable Molecular Qubits through Host-Matrix Control

Optically addressable spins are a promising platform for quantum information science due to their combination of long-lived qubit with spin-optical interface external control and readout. The ability chemically synthesize such systems—to generate optically molecular spins—offers modular architecture which can be transported across different environments atomistically tailored targeted applications through bottom-up design synthesis. Here, we demonstrate how the spin coherence in qubits controlled engineering host environment. By inserting chromium (IV)-based into nonisostructural matrix, noise-insensitive clock transitions, transverse zero-field splitting, that not present when using an isostructural host. This host-matrix leads spin-coherence times more than 10 μs nuclear electron-spin-rich We model dependence on splitting from first principles experimentally verify theoretical predictions four distinct systems. Finally, explore further enhance optical-spin interfaces by investigating key parameters optical linewidth spin-lattice relaxation time. Our results test structure-function relationships tunable highlight opportunities nanoscale sensing noisy environments.Received 18 March 2022Revised 16 June 2022Accepted 1 July 2022DOI:https://doi.org/10.1103/PhysRevX.12.031028Published American Physical Society under terms Creative Commons Attribution 4.0 International license. Further distribution this work must maintain attribution author(s) published article’s title, journal citation, DOI.Published SocietyPhysics Subject Headings (PhySH)Research AreasChemical Physics & ChemistryQuantum engineeringQuantum processingSpintronicsQuantum InformationCondensed Matter, Materials Applied