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The Japan Society of Applied Physics

Atomic-scale structure of optically activated Sm dopants identified with site-selective X-ray absorption spectroscopy

Masashi Ishii

Published Feb 13, 2013• 0 citations
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When introduced as dopants into ${\mathrm{Y}}_{2}{\mathrm{O}}_{3}$, $\mathrm{E}{\mathrm{r}}^{3+}$ ions replace ${\mathrm{Y}}^{3+}$ ions at two crystallographic sites of ${\mathrm{C}}_{2}$ and ${\mathrm{C}}_{3\mathrm{i}}$ point symmetries. The ${\mathrm{C}}_{3\mathrm{i}}$ site is particularly interesting, given that the inversion symmetry prohibits static electric-dipole moments and electric-dipole transitions, resulting in 1.5 \textmu{}m optical transitions characterized by purely magnetic-dipole properties. Employing $\mathrm{E}{\mathrm{r}}^{3+}\phantom{\rule{4pt}{0ex}}^{4}I_{15/2}\ensuremath{\leftrightarrow}^{4}I_{13/2}$ transitions, we examined the inherent ${\mathrm{C}}_{3\mathrm{i}}$ site of $\mathrm{E}{\mathrm{r}}^{3+}$ in ${\mathrm{Y}}_{2}{\mathrm{O}}_{3}$ for its potential in quantum information science and spectral hole burning applications. Our approach involved absorption and site-selective fluorescence spectroscopy to discern $\mathrm{E}{\mathrm{r}}^{3+}$ energy levels and revealed an excited-state lifetime of 14.6 ms. High-resolution laser spectroscopy at 3.7 K indicated an inhomogeneous linewidth of 1.3 GHz in our sample. Orientation-dependent Zeeman laser absorption spectroscopy facilitated the determination of the full $g$ tensors for both the ground and excited states, confirming the ${\mathrm{C}}_{3\mathrm{i}}$ site assignment. Furthermore, it identified a suitable magnetic field direction for mitigating decoherence, a finding corroborated through two-pulse photon echo spectroscopy. Our study presents photon echo coherent transient measurements related to magnetic-dipole-allowed rare-earth ion transitions at the ${\mathrm{C}}_{3\mathrm{i}}$ site. The observed decoherence, attributed to spectral diffusion arising from $\mathrm{E}{\mathrm{r}}^{3+}\text{\ensuremath{-}}\mathrm{E}{\mathrm{r}}^{3+}$ magnetic-dipole interactions, underscores the complex spin dynamics at play in systems with multiple inequivalent dopant sites. Coupled with the practicality of telecom laser wavelengths, our investigation highlights the promise of magnetic-dipole transitions in advancing quantum information science and spectral hole burning applications.

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Optically active defects suspended in an inert solid are an interesting system for sensing and magnetometry at the nanometer scale, in addition to being a potential source of high-density, identical quantum emitters for quantum information. Beyond their response to external fields, the optical absorption and emission spectra also reflect information about the host matrix, which is critical to understand for either application. For the particular system of thulium atoms implanted in solid argon, high resolution laser spectroscopy reveals narrow ensemble linewidths of the 1140 nm f to f ground state spin-orbit transition, which is split due to crystal field effects and hyperfine coupling. Pump-probe spectroscopy is used to identify crystal field levels in at least two stable trapping sites, and the crystal field is determined to be nearly axial in both sites. Strong selection rules indicate that this transition becomes magnetic-electric in the argon host, most likely due to dielectric effects. In the presence of mT magnetic fields, Zeeman shifts are resolvable by laser fluorescence, allowing crystal axis selective polarized spectroscopy. These results show that all-optical detection schemes for DC magnetic fields are already possible with thulium-doped argon, and point towards more informed strategies for monitoring and improving crystal growth and annealing.

arXiv:2507.08140•Physical review. B./Physical review. B•Jun 16, 2025•1 citation
When introduced as dopants into Y2O3{\mathrm{Y}}_{2}{\mathrm{O}}_{3}Y2​O3​, Er3+\mathrm{E}{\mathrm{r}}^{3+}Er3+ ions replace Y3+{\mathrm{Y}}^{3+}Y3+ ions at two crystallographic sites of C2{\mathrm{C}}_{2}C2​ and C3i{\mathrm{C}}_{3\mathrm{i}}C3i​ point symmetries. The C3i{\mathrm{C}}_{3\mathrm{i}}C3i​ site is particularly interesting, given that the inversion symmetry prohibits static electric-dipole moments and electric-dipole transitions, resulting in 1.5 \textmu{}m optical transitions characterized by purely magnetic-dipole properties. Employing $\mathrm{E}{\mathrm{r}}^{3+}\phantom{\rule{4pt}{0ex}}^{4}I_{15/2}\ensuremath{\leftrightarrow}^{4}I_{13/2}$ transitions, we examined the inherent C3i{\mathrm{C}}_{3\mathrm{i}}C3i​ site of Er3+\mathrm{E}{\mathrm{r}}^{3+}Er3+ in Y2O3{\mathrm{Y}}_{2}{\mathrm{O}}_{3}Y2​O3​ for its potential in quantum information science and spectral hole burning applications. Our approach involved absorption and site-selective fluorescence spectroscopy to discern Er3+\mathrm{E}{\mathrm{r}}^{3+}Er3+ energy levels and revealed an excited-state lifetime of 14.6 ms. High-resolution laser spectroscopy at 3.7 K indicated an inhomogeneous linewidth of 1.3 GHz in our sample. Orientation-dependent Zeeman laser absorption spectroscopy facilitated the determination of the full ggg tensors for both the ground and excited states, confirming the C3i{\mathrm{C}}_{3\mathrm{i}}C3i​ site assignment. Furthermore, it identified a suitable magnetic field direction for mitigating decoherence, a finding corroborated through two-pulse photon echo spectroscopy. Our study presents photon echo coherent transient measurements related to magnetic-dipole-allowed rare-earth ion transitions at the C3i{\mathrm{C}}_{3\mathrm{i}}C3i​ site. The observed decoherence, attributed to spectral diffusion arising from $\mathrm{E}{\mathrm{r}}^{3+}\text{\ensuremath{-}}\mathrm{E}{\mathrm{r}}^{3+}$ magnetic-dipole interactions, underscores the complex spin dynamics at play in systems with multiple inequivalent dopant sites. Coupled with the practicality of telecom laser wavelengths, our investigation highlights the promise of magnetic-dipole transitions in advancing quantum information science and spectral hole burning applications.
Optically active defects suspended in an inert solid are an interesting system for sensing and magnetometry at the nanometer scale, in addition to being a potential source of high-density, identical quantum emitters for quantum information. Beyond their response to external fields, the optical absorption and emission spectra also reflect information about the host matrix, which is critical to understand for either application. For the particular system of thulium atoms implanted in solid argon, high resolution laser spectroscopy reveals narrow ensemble linewidths of the 1140 nm f to f ground state spin-orbit transition, which is split due to crystal field effects and hyperfine coupling. Pump-probe spectroscopy is used to identify crystal field levels in at least two stable trapping sites, and the crystal field is determined to be nearly axial in both sites. Strong selection rules indicate that this transition becomes magnetic-electric in the argon host, most likely due to dielectric effects. In the presence of mT magnetic fields, Zeeman shifts are resolvable by laser fluorescence, allowing crystal axis selective polarized spectroscopy. These results show that all-optical detection schemes for DC magnetic fields are already possible with thulium-doped argon, and point towards more informed strategies for monitoring and improving crystal growth and annealing.