A Paired-Ion Framework Composed of Vanadyl Porphyrin Molecular Qubits Extends Spin Coherence Times

Molecular electron spin qubits arranged in precise arrays have great potential for use in quantum information science applications. Molecular qubits are synthetically versatile and can be placed in ordered arrangements upon incorporation into a new class of materials known as paired-ion frameworks (PIFs). A PIF composed of vanadyl porphyrin molecular qubits, <b>VOTCPP-PIF-1</b>, was synthesized as single crystals. Electron paramagnetic resonance spectroscopy was used to study their spin coherence at temperatures up to 293 K. A suspension of <b>VOTCPP-PIF-1</b> at 5 K in dimethylformamide (DMF) had a spin-spin relaxation time (<i>T</i>_m) of 270 ns. In DMF-<i>d</i>_<i>7</i> and at 5 K, the coherence time of this material increased to 370 ns. This increase in <i>T</i>_m is attributed to the lower gyromagnetic ratio of ²H compared to ¹H, which results in weaker electron-nuclear dipolar coupling that reduces the effect of nuclear spin flips on electron spin coherence. In toluene, crystals of <b>VOTCPP-PIF-1</b> had a <i>T</i>_m of 31 ns at 293 K, demonstrating that PIFs are a promising platform for creating materials for quantum information science applications.