Investigation of the Electronic Structure and Optical, EPR, and ODMR Spectroscopic Properties for ¹⁷¹Yb³⁺-Doped Y₂SiO₅ Crystal: A Combined Theoretical Approach

Abstract

Various spectroscopic properties of Yb3+-doped Y2SiO5 crystal have been extensively investigated due to its promising application in quantum information processing. However, the local structure, electronic structure of Yb3+:Y2SiO5 crystal, and its optical and magnetic properties have not been comprehensively studied from a theoretical viewpoint. In this work, the geometric and electronic structures of Yb3+ that replaces two crystallographic Y3+ sites in the Y2SiO5 crystal are first obtained by the method of density functional theory (DFT). Then, the optical, electron paramagnetic resonance (EPR), and optically detected magnetic resonance (ODMR) spectra for 171Yb3+ (nuclear spin I = 1/2) at such two sites are simultaneously calculated in the framework of the complete diagonalization (of energy) matrix (CDM) based on the optimized local structure around 171Yb3+ ion by DFT. The various calculated spectroscopic properties by such combined theoretical approach are consistent with the experimental ones, which demonstrates that CDM is effective and particularly suitable for calculating hyperfine A -tensors under zero, low, and intermediate magnetic field. More importantly, based on the obtained accurate hyperfine structure of 171Yb3+ in Y2SiO5 crystal, the possible “clock transitions”, which can enhance the optical coherence time, can be assigned or predicted by the present approach. This study successfully explains the spectroscopic properties of 171Yb3+-doped Y2SiO5 and provides a feasible method to design and search for practical rare-earth-doped quantum information materials for the community.

Determining the Hyperfine Structure and Clock Transitions for Kramers Rare-Earth Ions in a Crystal under a Magnetic Field: Beyond Spin Hamiltonian

“…Such a Hamiltonian has been widely adopted to calculate various spectroscopic properties of the RE ion in crystals (see Section ). Recently, the ZEFOZ magnetic fields along some direction of the 171 Yb 3+ :Y 2 SiO 5 crystal have been successfully calculated by this method in our work . Similar calculations of other Kramers ion-doped crystals such as Er 3+ :Y 2 SiO 5 are also given in a recent study by Jobbitt et al In Section , the first case study of the 173 Yb 3+ :Y 2 SiO 5 crystal with nuclear spin I = 5/2 shows that if crystal-field parameters (CFPs) of the RE ion in the crystal are reliable enough, the complicated hyperfine sublevels can also be correctly calculated by the complete diagonalization (of energy) matrix (CDM) formalism.…”

Prediction of optical polarization and high-field hyperfine structure via a parametrized crystal-field model for low-symmetry centers in Er3+ -doped Y2SiOJobbitt1, Wells2, Reid3 et al. 2021Phys. Rev. B13150View full textAdd to dashboardCite

“…Recently, crystal-field analyses have been performed for the C 1 symmetry centers in Ce 3+ , Er 3+ and Yb 3+ doped Y 2 SiO 5 [16][17][18][19]; with further analyses under way for Y 2 SiO 5 doped with Nd 3+ , Sm 3+ and Ho 3+ [20][21][22].…”

Zeeman and laser site selective spectroscopy of C1 point group symmetry Sm3+ centres in Y2SiO5: a parametrized crystal-field analysis for the 4f 5 configuration

“…Initial work, which included g tensors for two states for each site, as well as hyperfine data [21] was later extended by using Zeeman spectroscopy to determine magnetic splittings along the D 1 , D 2 , and b axes of the crystal for dozens of states [42]. A similar approach has been independently applied to the two sites in Yb 3+ :Y 2 SiO 5 [23].…”

“…Crystal-field parameters in higher-symmetry sites show a reasonably consistent trend across the rare-earth series (see, for example [35]). For Y 2 SiO 5 the only published fits that make use of directional magnetic data are for for Er 3+ [21,42], Yb 3+ [23], and this work. In comparing parameter sets for different ions, we must take into account that for each site there are two magneticallyinequivalent orientations, which are related by changing the sign of the odd-q crystal-field parameters.…”