We study spin-lattice relaxation times of electron spins in Er
3+:CaWO
4 at millikelvin temperature, detected via their coupling to a low-mode volume superconducting resonator. At large magnetic field supporting strong phonon-emission rates, we observe a noticeable increase in relaxation times with increasing spin-excitations, which exhibit a unique
[tanh(ℏω0/kBT)]2 temperature dependence. These observations are typical of a phonon-bottlenecked spin relaxation, and have implications for quantum technologies that exploit rare-earth spin ensembles as coherent resources.
We investigate the lattice dynamics of CaWO
4, a promising host crystal for erbium-based quantum memories, using inelastic neutron scattering together with density-functional perturbation theory. The measured phonon dispersion along the (100), (001), and (101) reciprocal space direction reveals phonon bands extending up to 130 meV, with a gap between 60 and 80 meV, in good agreement with our calculations. From a symmetry analysis of the phonon eigenmodes, we identify eight Raman-active modes that can couple directly to the Er
3+ crystal-field operators, including a low-energy
Bg mode at 9.1 meV that is expected to play a dominant role in phonon-assisted spin-lattice relaxation. These results provide a microscopic description of the phonon bath in CaWO
4 and establish a basis for engineering phononic environments to mitigate the loss of stored quantum states and optimize Er-doped CaWO
4 for quantum-memory applications.
Rare earth ion (REI)-doped oxide thin films are attractive for the application of quantum interconnects due to their stable optical levels and scalability
1−3. Among them, Er
3+ doped CaWO
4 is promising because it possesses narrow optical linewidth transitions and a long spin coherence time
4−6. The electron spin coherence is limited at high temperatures by paramagnetic impurities and by the presence of the 14.3%
183W nuclear spin. To further increase the spin coherence time at millikelvin temperatures, where the paramagnetic impurities are frozen out, our approach is to synthesize chemically and isotopically purified thin films as a host material. We first grow non-isotopically enriched Er
3+ doped CaWO
4 thin films, which exhibit a 214(13) MHz photoluminescence (PL) inhomogeneous linewidth, indicating the thin film has high crystalline quality. We then grow isotopically enriched CaWO
4 thin films using an isotopically purified
186WO
3 source. Time of flight secondary ion mass spectrometry (ToF-SIMS) was used to measure the relative concentration of W isotopes.
183W, the only W isotope that has a net nuclear spin and is the major cause of spin decoherence, was at a relative abundance of 1.2%, a factor of 10 lower than natural abundance. We also observed PL emission from single ions after integrating nano-photonic devices with the thin film. These results establish isotopically engineered CaWO
4 thin films as a promising platform for future studies of nuclear-spin-limited coherence and for scalable rare-earth-ion-based quantum nanophotonic devices.