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.
Without using any trapping lasers, rare-earth (RE) ions can be doped into some nanofabricated materials in form of nanocrystals in a solid state matrix, thus rendering a natural trap for potential application as a quantum computing device. In particular, passive nuclear spin states of RE ions can be utilized as (i) optical quantum memory (with huge density as yielded from nanocrystals), (ii) qubits by encoding in ground hyperfine states and operated as (iii) two-qubit gate when transferring them to active magnetized electronic states. A feasible implementation of qubits is realised by using those doped RE ions whose open-shell (for inner highly shielded
4f shell electrons) energy levels and statevectors are well described by the crystal field (CF) interaction and hyperfine coupling in which the Hamiltonian is composed of various freeion interactions, the CF potential, electronic and nuclear Zeeman effects as well as the hyperfine interaction. For those qubit encoded in the two ground hyperfine states of RE ions, they can have fairly long lifetimes of days and coherence times (from 1.3s for
Er3+ to 6 hours for
Eu3+) due to the unique spectroscopic properties of RE ions. Because of the recent progress in optical single-ion detection for addressing individual qubits with a specific frequency channel, RE ions could be packed in a solid state 3D matrix at nanometer spacing, hence rendering very high qubit densities for quantum memories. Meanwhile, this configure also leads to strong dipole-dipole interactions (or high connectivity) between qubits which are not nearest neighbors. In this study, Kramers ions like
167Er and
171Yb doped in yttrium orthosilicate
Y2SiO5 (YSO) nanocrystals will be investigated as a promising system for quantum computing because of their weak spin bath and possibility for being directly milled in single nanocrystals as nano-resonators. By using the famous Wien2k package to carry out the first-principles calculations, we can obtain the CF parameters and hyperfine constants as well as various electronic properties like energy gap and band structure for those Kramers RE ions doped in YSO. We shall present some essential findings from first-principles calculations to obtain various properties of the ground and excited CF and hyperfine states for those RE ions with an aim to optimize RE ions doping in YSO nanocrystals for quantum memories and qubits, contributing to scalable quantum computing architectures.