B. Z. Malkin

Direct measurements of anticrossings of the electron-nuclear energy levels in LiYF4∶Ho3+ with submillimeter EPR spectroscopy

The electron paramagnetic resonance (EPR) spectra of impurity Ho3+ ions in monocrystals LiYF4∶Ho3+ (0.1 and 1%) with the natural abundance of6Li (7.42%) and7Li (92.58%) isotopes, and in the sample7LiYF4∶Ho3+ (0.1%) isotopically pure in7Li were taken at the temperature 4.2 K in the frequency range of 165–285 GHz. Resonance transitions between crystal field sublevels (the ground non-Kramers doublet and the nearest excited singlet) of the5I8 term were detected. The refined set of crystal field parameters and the effective constant of the magnetic hyperfine interaction were determined from the detailed analysis of the recorded spectra at frequencies varied by 0.05 GHz. The fine structure of EPR lines with intervals of about 300 MHz observed in the sample LiYF4∶Ho3+ (0.1%) can be interpreted as a result of the isotopic disorder in the Li sublattices. Direct information about energy gaps at the anticrossing points of the electron-nuclear sublevels of the ground doublet was obtained. These gaps are induced by the hyperfine interaction that mixes doublet and singlet states and by random crystal fields. Weak EPR signals from distorted single ion and pair centers of impurity Ho3+ ions were resolved. From a comparison of the measured and simulated spectra, estimates of spectral parameters of the dimer centers have been obtained.

Coherent manipulation of dipolar coupled spins in an anisotropic environment

We study coherent dynamics in a system of dipolar coupled spin qubits diluted in solid and subjected to a driving microwave field. In the case of rare earth ions, anisotropic crystal background results in anisotropic g tensor and thus modifies the dipolar coupling. We develop a microscopic theory of spin relaxation in transient regime for the frequently encountered case of axially symmetric crystal field. The calculated decoherence rate is nonlinear in Rabi frequency. We show that the direction of static magnetic field that corresponds to the highest spin g-factor is preferable in order to obtain higher number of coherent qubit operations. The results of calculations are in excellent agreement with our experimental data on Rabi oscillations recorded for a series of CaWO4 crystals with different concentrations of Nd3+ ions.

Coherent spin dynamics in a gadolinium-doped CaWO4 crystal

We report the first observation of Rabi oscillations in the spin-7/2 ensemble of trivalent gadolinium ions hosted in CaWO4 single crystal. A number of transitions within the lowest electronic multiplet 8S7/2 of Gd3+ ion are studied using a combination of continuous-wave and pulsed electron paramagnetic resonance spectroscopy. The corresponding Rabi damping curves and the spin coherence times are detected at varying strengths of the microwave field. These data are well reproduced by a theoretical model which accounts for the inhomogeneity of the microwave field within the crystal sample volume and the magnetic dipole interactions in the diluted spin ensemble.

Multi-range high-frequency EPR spectroscopy of LiYF4 and LiLuF4 crystals doped by rare-earth ions

EPR spectra of isostructural LiYF4 and LiLuF4 crystals doped by Dy3+, Er3+, and Ho3+ ions are measured at 4.2 K in the frequency range 40–800 GHz. The effects caused by isotopic disorder in the lithium sublattice, the random crystal field, and the interaction between paramagnetic impurity ions are detected and studied. The results of the measurements are used to determine the spectral characteristics of the compounds and the crystal field parameters. It is demonstrated that the formation of the isotope structure of the EPR signal is dominated by local deformations of the crystal lattice induced by mass defects.