Solid-state impurity spins with optical control are currently investigated for quantum networks and repeaters. Among these, rare-earth-ion doped crystals are promising as quantum memories for light, with potentially long storage time, high multimode capacity, and high bandwidth. However, with spins there is often a tradeoff between bandwidth, which favors electronic spin, and memory time, which favors nuclear spins. Here, we present optical storage experiments using highly hybridized electron-nuclear hyperfine states in 171 Yb 3+ :Y2SiO5, where the hybridization can potentially offer both long storage time and high bandwidth. We reach a storage time of 1.2 ms and an optical storage bandwidth of 10 MHz that is currently only limited by the optical Rabi drive frequency. This constitutes the first optical storage experiment using spin states in any rare-earth ion with electronic spin. These results pave the way for rare-earth based quantum memories with high bandwidth, long storage time and high multimode capacity, a key resource for quantum repeaters.

Optically addressable spins are actively investigated in quantum communication, processing, and sensing. Optical and spin coherence lifetimes, which determine quantum operation fidelity and storage time, are often limited by spin-spin interactions, which can be decreased by polarizing spins. Spin polarization can be achieved using optical pumping, large magnetic fields, or mK-range temperatures. Here, we show that optical pumping of a small fraction of ions with a fixed-frequency laser, coupled with spin-spin interactions and spin diffusion, leads to substantial spin polarization in a paramagnetic rare-earth doped crystal, 171 Yb 3þ ∶Y 2 SiO 5. Indeed, more than 90% spin polarization has been achieved at 2 K and zero magnetic field. Using this spin polarization mechanism, we further demonstrate an increase in optical coherence lifetime from 0.3 ms to 0.8 ms, due to a strong decrease in spin-spin interactions. This effect opens the way to new schemes for obtaining long optical and spin coherence lifetimes in various solid-state systems such as ensembles of rare-earth ions or color centers in diamond, which are of interest for a broad range of quantum technologies.

Quantum repeaters based on heralded entanglement require quantum nodes that are able to generate multimode quantum correlations between memories and telecommunication photons. The communication rate scales linearly with the number of modes, yet highly multimode quantum storage remains challenging. In this work, we demonstrate an atomic frequency comb quantum memory with a time-domain mode capacity of 1250 modes and a bandwidth of 100 MHz. The memory is based on a Y2SiO5 crystal doped with 171Yb3+ ions, with a memory wavelength of 979 nm. The memory is interfaced with a source of non-degenerate photon pairs at 979 and 1550 nm, bandwidth-matched to the quantum memory. We obtain strong non-classical second-order cross correlations over all modes, for storage times of up to 25 μs. The telecommunication photons propagated through 5 km of fiber before the release of the memory photons, a key capability for quantum repeaters based on heralded entanglement and feed-forward operations. Building on this experiment should allow distribution of entanglement between remote quantum nodes, with enhanced rates owing to the high multimode capacity.

Quantum repeaters based on heralded entanglement require quantum nodes that are able to generate multimode quantum correlations between memories and telecommunication photons. The communication rate scales linearly with the number of modes, yet highly multimode quantum storage remains challenging. In this work, we demonstrate an atomic frequency comb quantum memory with a time-domain mode capacity of 1250 modes and a bandwidth of 100 MHz, to our knowledge the largest number of modes stored in the quantum regime. The memory is based on a Y2SiO5 crystal doped with 171 Yb 3+ ions, with a memory wavelength of 979 nm. The memory is interfaced with a source of non-degenerate photon pairs at 979 and 1550 nm, bandwidth-matched to the quantum memory. We obtain strong non-classical second-order cross correlations over all modes, for storage times of up to 25 µs. The telecommunication photons propagated through 5 km of fiber before the release of the memory photons, a key capability for quantum repeaters based on heralded entanglement and feed-forward operations. Building on this experiment should allow distribution of entanglement between remote quantum nodes, with enhanced rates owing to the high multimode capacity.

We demonstrate a new spin polarization mechanism that combines optical pumping with spin diffusion to achieve large spin polarization in 171Yb3+:Y2SiO5. This is used to increase optical coherence lifetime from 0.3 to 0.8 ms.