Abstract
The success of the emerging field of solid-state optical quantum information processing (QIP) critically depends on the access to resonant optical materials. Rare-earth ion (REI)-based molecular systems, whose quantum properties could be tuned taking advantage of molecular engineering strategies, are one of the systems actively pursued for the implementation of QIP schemes. Herein, we demonstrate the efficient polarization of ground-state nuclear spins—a fundamental requirement for all-optical spin initialization and addressing—in a binuclear Eu(III) complex, featuring inhomogeneously broadened 5D0 → 7F0 optical transition. At 1.4 K, long-lived spectral holes have been burnt in the transition: homogeneous linewidth (Γh) = 22 ± 1 MHz, which translates as optical coherence lifetime (T2opt) = 14.5 ± 0.7 ns, and ground-state spin population lifetime (T1spin) = 1.6 ± 0.4 s have been obtained. The results presented in this study could be a progressive step towards the realization of molecule-based coherent light-spin QIP interfaces.
Highlights
The success of the emerging field of solid-state optical quantum information processing (QIP) critically depends on the access to resonant optical materials
Non-Kramers Rare-earth ion (REI) with an even number of f electrons—for example, Eu(III), Pr(III), or Tm(III)—embedded in a matrix with low average magnetic moments have been extensively studied for the implementation of QIP schemes[23]
To implement optical QIP schemes, a molecular Eu(III) complex should feature a long coherence time, photostability, stability to be handled at ambient conditions, and a reasonable luminescence quantum yield
Summary
The success of the emerging field of solid-state optical quantum information processing (QIP) critically depends on the access to resonant optical materials. Color centers in diamond[4], rare-earth ions (REIs) doped in host matrices[2,9,10,11,12,13], and luminescent organic dye molecules (dye impurity), featuring extremely narrow and stable luminescent lines[14,15,16,17], are suitable systems to implement optical qubit operations. REIs feature long optical coherence lifetimes (T2opt), because the 4f–4f optical transitions, covering the whole visible and infrared spectral range, are wellshielded from the surrounding environment by the outer 5s and. The 5D0 → 7F0 transition of Eu(III) is of particular interest because the 5D0 → 7F0 transition is an induced electric dipole transition[24] and is largely unaffected by the magnetic field fluctuations arising from the surrounding environment, thereby long optical coherence lifetimes are associated with the transition
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