Rare earth ion doped crystals are state-of-the-art platforms for processing quantum information, particularly thanks to their excellent optical and spin coherence properties at cryogenic temperatures. Experimental observations have shown that the application of a static magnetic bias field significantly improves the coherence times in the rare earth ions ensemble, but only a few studies have focused on its dependency as a function of both magnetic field direction and amplitude. This is especially true for magnetic field amplitudes under the mT, and for low magnetic dipole moment ions. In this paper, we investigate the relationship between the magnetic field parameters and the decoherence caused by magnetic dipole-dipole coupling with the nearest-neighbor nuclear spins in the crystal. The primary non-Kramers rare earth ions investigated here are europium and praseodymium, but we also extend our study to the ytterbium Kramers ion due to its low magnetic dipole in the mT range. We perform theoretical investigations and simulations of the energy structure and coherence time evolution and identify good correspondences between experimental and simulated spin echo data. This work allows us to pinpoint the most relevant decoherence mechanisms in the considered magnetic field regime, and to predict favorable magnetic configurations.
Rare earth ion doped crystals are state-of-the-art platforms for processing quantum information, particularly thanks to their excellent optical and spin coherence properties at cryogenic temperatures. Experimental observations have shown that the application of a static magnetic bias field significantly improves the coherence times in the rare earth ions ensemble, but only a few studies have focused on its dependency as a function of both magnetic field direction and amplitude. This is especially true for magnetic field amplitudes under the mT, and for low magnetic dipole moment ions. In this paper, we investigate the relationship between the magnetic field parameters and the decoherence caused by magnetic dipole-dipole coupling with the nearest-neighbor nuclear spins in the crystal. The primary non-Kramers rare earth ions investigated here are europium and praseodymium, but we also extend our study to the ytterbium Kramers ion due to its low magnetic dipole in the mT range. We perform theoretical investigations and simulations of the energy structure and coherence time evolution and identify good correspondences between experimental and simulated spin echo data. This work allows us to pinpoint the most relevant decoherence mechanisms in the considered magnetic field regime, and to predict favorable magnetic configurations.
Rare-earth doped crystals have long coherence times and the potential to provide quantum interfaces between microwave and optical photons. Such applications benefit from a high cooperativity between the spin ensemble and a microwave cavity---this motivates an increase in the rare-earth ion concentration which in turn impacts the spin coherence lifetime. We measure spin dynamics of two rare-earth spin species, 145Nd and Yb, doped into Y2SiO5, coupled to a planar microwave resonator in the high-cooperativity regime, in the temperature range 1.2K to 14mK. We identify relevant decoherence mechanisms, including instantaneous diffusion arising from resonant spins and temperature-dependent spectral diffusion from impurity electron and nuclear spins in the environment. We explore two methods to mitigate the effects of spectral diffusion in the Yb system in the low-temperature limit, first, using magnetic fields of up to 1 T to suppress impurity spin dynamics and, second, using transitions with low effective g factors to reduce sensitivity to such dynamics. Finally, we demonstrate how the ``clock transition'' present in the 171Yb system at zero field can be used to increase coherence times up to T2=6(1)ms.
Rare-earth ion doped crystals have proven to be solid platforms for implementing quantum memories. Their potential use for integrated photonics with large multiplexing capability and unprecedented coherence times is at the core of their attractiveness. The best performances of these ions are, however, usually obtained when subjected to a DC magnetic field, but consequences of such fields on the quantum memory protocols have only received little attention. In this paper, we focus on the effect of a DC bias magnetic field on the population manipulation of non-Kramers ions with nuclear quadrupole states, both in the spin and optical domains, by developing a simple theoretical model. We apply this model to explain experimental observations in a 151Eu:Y2SiO5 crystal, and highlight specific consequences on the atomic frequency comb spin-wave protocol. The developed analysis should allows predicting optimal magnetic field configurations for various protocols.
Flip-flop processes due to magnetic dipole-dipole interaction between neighboring ions in crystals doped by rare-earth ions are one of the mechanisms of relaxation between hyperfine levels. Modeling of this mechanism has so far been macroscopic, characterized by an average rate describing the relaxation of all ions. Here, however, we present a microscopic model of flip-flop interactions between individual nuclear spins of dopant ions. Every ion is situated in a unique local environment in the crystal, where each ion has different distances and a unique orientation relative to its nearest neighbors, as determined by the lattice structure. Thus each ion has a unique flip-flop rate and the collective relaxation dynamics of all ions in a bulk crystal is a sum of many exponential decays, giving rise to a distribution of rates rather than a single average decay rate. We employ this model to calculate flip-flop rates in Pr3+:Y2SiO5 and show experimental measurements of population decay of the ground state hyperfine levels at $\ensuremath{\sim}2$ K. We also present a method to measure rates of individual transitions from hole burning spectra that requires significantly fewer fitting parameters in theoretical rate equations compared to earlier work. Furthermore, we measure the effect of external magnetic field on the flip-flop rates and observe that the rates slow down by two orders of magnitude in a field of 5--10 mT.
Microwave and optical transitions of rare-earth ions enable microwave-to-optical frequency transduction. This transduction is a coherent process; therefore, the narrow linewidths and long coherence times of rare-earth ions are crucial for achieving efficient frequency conversion. Particularly long coherence times can be achieved with small-spin materials, as unpaired electronic and nuclear spins introduce magnetic noise, serving as a decoherent source of the transitions. However, complete spin-free rare-earth materials cannot exist without charge compensation. Consequently, residual spins in existing rare-earth materials act as a bottleneck, limiting both their spin and optical coherence times. Rather than focusing on nearly spin-free materials, this thesis investigates the microwave and optical transitions of rare-earth ions in materials that are fully concentrated with electronic spins. Recent studies on rare-earth magnetic materials have demonstrated narrow optical linewidths resulting from magnetic ordering and a particularly strong coupling between microwave cavity modes and the collective excitations of rare-earth ions. Although these recent studies are noteworthy, the energy-level transitions, especially optical transitions, of rare-earth ions in magnetic materials remain largely unexamined. In this thesis, various spectroscopic studies are employed to characterise their transition properties and to develop a model of energy levels. The model presented is expected to be applicable to other rare-earth magnetic materials, thereby opening avenues for further investigation in this class of systems. Two types of rare-earth magnetic materials are investigated: neodymium gallate with a stoichiometric concentration of neodymium ions, and gadolinium vanadate doped with a low (ppm) concentration of erbium ions. Microwave and optical transmission spectroscopy are employed under externally applied magnetic fields to characterise the energy-state transitions of the rare-earth ions in both materials. The magnetic phases and corresponding spin configurations influence the observed spectra, making conventional approaches to spectral simulation inadequate. To address this challenge, mean field and magnon-coupled crystal-field models are developed in this thesis to predict magnon and optical transition spectra. These simulations exhibit good agreement with experimental results, allowing for the characterisation of transition properties. Following the characterisation of the material, a new transduction approach is introduced, developed, and implemented using doped rare-earth ions in a magnetic material. In this scheme, coherent conversion between microwave and optical modes is achieved by exciting an optical transition of the doped ions.
Eu3+:Y2SiO5 crystals are promising candidates for quantum memories because their nuclear spin coherence lifetime can be extended to 47 seconds at a particular magnetic field. Although an extended coherence lifetime of 6 hours can be achieved with a large number of dynamic decoupling sequences, these pulses will also introduce unwanted noise. To realize quantum storage with a lifetime of hours, it is necessary to quantitatively characterize the spin decoherence process of Eu3+ ions to guide the experimental efforts. In practice, a number of limiting factors could impose a limit on the achievable spin coherence lifetime, which includes the spin inhomogeneous broadening of the Eu3+ ensemble and the homogeneity and stability of the external magnetic field. Here, we provide a Monte Carlo simulation model of the nuclear spin decoherence process of Eu3+ ions in Y2SiO5 crystals, and these limiting factors are considered to provide an accurate prediction of the spin coherence lifetimes. This method is universal and can be applied to other rare-earth-ion-doped crystals.
In many important situations, the dominant dephasing mechanism in cryogenic rare-earth-metal-ion--doped systems is due to magnetic field fluctuations from spins in the host crystal. Operating at a magnetic field where a transition has a zero first-order Zeeman (ZEFOZ) shift can greatly reduce this dephasing. Here we identify the location of transitions with a zero first-order Zeeman shift for optical transitions in Pr3+:YAG and for spin transitions in Er3+:Y2SiO5. The long coherence times that ZEFOZ can enable would make Pr3+:YAG a strong candidate for achieving the strong-coupling regime of cavity QED, and would be an important step forward in creating long-lived telecommunications wavelength quantum memories in Er3+:Y2SiO5. This work relies mostly on published spin-Hamiltonian parameters, but Raman heterodyne spectroscopy was performed on Pr3+:YAG to measure the parameters for the excited state.