Kieran M. Smith | Searcharxiv

arXiv2022

Zeeman-Hyperfine Measurements of a Pseudo-Degenerate Quadruplet in CaF$_2$:Ho$^{3+}$

We report Zeeman infra-red spectroscopy of electronic-nuclear levels of $^5$I$_8 \rightarrow ^5$I$_7$ transitions of Ho$^{3+}$ in the C$_{\rm 4v}$(F$^-$) centre in CaF$_2$ with the magnetic field along the $\langle 111\rangle$ direction of the crystal. Transitions to the lowest $^5$I$_7$ state, an isolated electronic doublet, and the next group of states, a pseudo-quadruplet consisting of a doublet and two nearby singlets, exhibit strongly non-linear Zeeman splittings and intensity variations. Simulated spectra based upon a crystal-field analysis give an excellent approximation to the data, illustrating the strong predictive ability of the parametrised crystal-field approach. Anti-crossings in the hyperfine splittings, the basis of quantum information storage in rare-earth doped insulating dielectrics, are also predicted.

cond-mat.mtrl-sci↗

arXiv2021

Complete crystal field calculation of Zeeman-hyperfine splittings in europium

Computational crystal-field models have provided consistent models of both electronic and Zeeman-hyperfine structure for several rare earth ions. These techniques have not yet been applied to the Zeeman-hyperfine structure of Eu$^{3+}$ because modeling the structure of the $J=0$ singlet levels in Eu$^{3+}$ requires inclusion of the commonly omitted lattice electric quadrupole and nuclear Zeeman interactions. Here, we include these terms in a computational model to fit the crystal field levels and the Zeeman-hyperfine structure of the $^7F_0$ and $^5D_0$ states in three Eu$^{3+}$ sites: the C$_{4v}$ and C$_{3v}$ sites in CaF$_2$ and the C$_2$ site in EuCl$_3$.6H$_2$O. Close fits are obtained for all three sites which are used to resolve ambiguities in previously published parameters, including quantifying the anomalously large crystal-field-induced state mixing in the C$_{3v}$ site and determining the signs of Zeeman-hyperfine parameters in all three sites. We show that this model allows accurate prediction of properties for Eu$^{3+}$ important for quantum information applications of these ions, such as relative transition strengths. The model could be used to improve crystal field calculations for other non-Kramers singlet states. We also present a spin Hamiltonian formalism without the normal assumption of no $J$ mixing, suitable for other rare earth ion energy levels where this effect is important.

cond-mat.mtrl-sci↗