Long Electron Spin Coherence Times of Atomic Hydrogen Trapped in Silsesquioxane Cages

Abstract

Encapsulated atomic hydrogen in cube-shaped octasilsesquioxane (POSS) cages of the Si₈O₁₂R₈ type (where R is an organic group) is one of the simplest alternative stable systems to paramagnetic endofullerenes that have been regarded as key elements of spin-based quantum technologies. Apart from common sources of decoherence such as nuclear spin and spectral diffusion, all H@POSS species studied so far suffer from additional shortening of T₂ at low temperatures due to methyl group rotations. Here we eliminate this factor for the first time by studying the smallest methyl-free derivative with R = H, namely, H@T₈H₈. By applying dynamical decoupling methods, we measure electron spin coherence times T₂ up to 280 ± 76 μs at T = 90 K and observe a linear dependence of the decoherence rate 1/T₂ on trapped hydrogen concentrations, which we attribute to the spin dephasing mechanism of instantaneous diffusion and a nonuniform spatial distribution of encapsulated H atoms.