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Praseodymium (Pr$^{3+}$) ions doped in the site 1 of yttrium orthosilicate (Y$_2$SiO$_5$) has been widely employed as the photonic quantum memory due to their excellent optical coherence and spin coherence. While praseodymium ions occupying the site 2 in Y$_2$SiO$_5$ crystal have better optical coherence as compared with those at site 1, which may enable better performance in quantum memory. Here we experimentally characterize the hyperfine interactions of the ground state $^3$H$_4$ and excited state $^1$D$_2$ of Pr$^{3+}$ at site 2 in Y$_2$SiO$_5$ using Raman heterodyne detected nuclear magnetic resonance. The Hamiltonians for the hyperfine interaction are reconstructed for both ground state $^3$H$_4$ and excited state $^1$D$_2$ based on the Raman heterodyne spectra in 201 magnetic fields. The two-pulse spin-echo coherence lifetime for the ground state is measured to be 2.6$\pm$0.1 ms at site 2 with zero magnetic field, which is more than five times longer than that at site 1. The magnetic fields with zero first order Zeeman shift in the hyperfine transition for Pr$^{3+}$ at site 2 in Y$_2$SiO$_5$ are identified.

$\mathrm {^{151}Eu^{3+}}$-doped yttrium silicate ($\mathrm {^{151}Eu^{3+}:Y_2SiO_5}$ ) crystal is a unique material that possesses hyperfine states with coherence time up to 6 h. Many efforts have been devoted to the development of this material as optical quantum memories based on the bulk crystals, but integrable structures (such as optical waveguides) that can promote $\mathrm {^{151}Eu^{3+}:Y_2SiO_5}$-based quantum memories to practical applications, have not been demonstrated so far. Here we report the fabrication of type 2 waveguides in a $\mathrm {^{151}Eu^{3+}:Y_2SiO_5}$ crystal using femtosecond-laser micromachining. The resulting waveguides are compatible with single-mode fibers and have the smallest insertion loss of $4.95\ dB$. On-demand light storage is demonstrated in a waveguide by employing the spin-wave atomic frequency comb (AFC) scheme and the revival of silenced echo (ROSE) scheme. We implement a series of interference experiments based on these two schemes to characterize the storage fidelity. Interference visibility of the readout pulse is $0.99\pm 0.03$ for the spin-wave AFC scheme and $0.97\pm 0.02$ for the ROSE scheme, demonstrating the reliability of the integrated optical memory.

An experimental platform of ultralow-temperature pulsed ENDOR (electron-nuclear double resonance) spectroscopy is constructed for the bulk materials. Coherent property of the coupled electron and nuclear spins of the rare-earth (RE) dopants in a crystal (143Nd3+:Y2SiO5) is investigated from 100 mK to 6 K. At the lowest working temperatures, two-pulse-echo coherence time exceeding 2 ms and 40 ms are achieved for the electron and nuclear spins, while the electronic Zeeman and hyperfine population lifetimes are more than 15 s and 10 min. With the aid of the near-unity electron spin polarization at 100 mK, the complete hyperfine level structure with 16 energy levels is measured using ENDOR technique without the assistance of the reconstructed spin Hamiltonian. These results demonstrate the suitability of the deeply cooled paramagnetic RE-doped solids for memory components aimed for quantum communication and quantum computation. The developed experimental platform is expected to be a powerful tool for paramagnetic materials from various research fields.

Macroscopic realism is a classical worldview that a macroscopic system is always determinately in one of the two or more macroscopically distinguishable states available to it, and so is never in a superposition of these states. The question of whether there is a fundamental limitation on the possibility to observe quantum phenomena at the macroscopic scale remains unclear. Here we implement a strict and simple protocol to test macroscopic realism in a light-matter interfaced system. We create a micro-macro entanglement with two macroscopically distinguishable solid-state components and rule out those theories which would deny coherent superpositions of up to 76 atomic excitations shared by 10^10 ions in two separated solids. These results provide a general method to enhance the size of superposition states of atoms by utilizing quantum memory techniques and to push the envelope of macroscopicity at higher levels., Comment: 8 pages, 4 figures

The faithful storage and coherent manipulation of quantum states with matter-systems enable the construction of large-scale quantum networks based on quantum repeater. To achieve useful communication rates, highly multimode quantum memories will be required to construct a multiplexed quantum repeater. Here, we present the first demonstration of the on-demand storage of orbital-angular-momentum states with weak coherent pulses at the single-photon-level in a rare-earth-ion doped crystal. Through the combination of this spatial degree-of-freedom with temporal and spectral degrees of freedom, we create a multiple-degree-of-freedom memory with high multimode capacity. This device can serve as a quantum mode converter with high fidelity, which is the fundamental requirements for the construction of a multiplexed quantum repeater. This device further enables essentially arbitrary spectral and temporal manipulations of spatial-qutrit-encoded photonic pulses in real-time. Therefore, the developed quantum memory can serve as a building block for scalable photonic quantum information processing architectures.

Probing collective spin dynamics is a current challenge in the field of magnetic resonance spectroscopy and has important applications in material analysis and quantum information protocols. Recently, the rare-earth ion doped crystals are an attractive candidate for making long-lived quantum memory. Further enhancement of its performance would benefit from the direct knowledge on the dynamics of nuclear-spin bath in the crystal. Here we detect the collective dynamics of nuclear-spin bath located around the rare-earth ions in a crystal using dynamical decoupling spectroscopy method. From the measured spectrum, we analyze the configuration of the spin bath and characterize the flip-flop time between two correlated nuclear spins in a long time scale ($\sim $1s). Furthermore, we experimentally demonstrate that the rare-earth ions can serve as a magnetic quantum sensor for external magnetic field. These results suggest that the rare-earth ion is a useful probe for complex spin dynamics in solids and enable quantum sensing in the low-frequency regime, revealing promising possibilities for applications in diverse fields., Comment: The unit in Fig.4 has been corrected

The spin coherence time of $^{151}$Eu$^{3+}$ which substitutes the yttrium at site 1 in Y$_2$SiO$_5$ crystal has been extended to 6 hours in a recent work [\textit{Nature} \textbf{517}, 177 (2015)]. To make this long-lived spin coherence useful for optical quantum memory applications, we experimentally characterize the hyperfine interaction of the optically-excited state $^5$D$_0$ using Raman-heterodyne-detected nuclear magnetic resonance. The effective spin Hamiltonians for excited and ground state are fitted based on the experimental spectra obtained in 200 magnetic fields with various orientations. To show the correctness of the fitted parameters and potential application in quantum memory protocols, we also characterize the ground-state hyperfine interaction and predict the critical magnetic field which produces the 6-hour-long coherence time. The complete energy level structure for both the $^7$F$_0$ ground state and $^5$D$_0$ excited state at the critical magnetic field are obtained. These results enable the design of quantum memory protocols and the optimization of optical pumping strategy for realization of photonic quantum memory with hour-long lifetime.