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Physical Review B

Spectroscopy and dynamics of Er 3 + : Y 2 Si O 5 at 1.5 μ m

Thomas Böttger, Yazhou Sun, Charles W. Thiel, R. L. Cone

Published Aug 21, 2006• 103 citations
Publisher

Abstract

We present the results of detailed site-selective spectroscopy performed on the $^{4}I_{15∕2}\ensuremath{\leftrightarrow}^{4}I_{13∕2}$ transition of ${\mathrm{Er}}^{3+}:{\mathrm{Y}}_{2}\mathrm{Si}{\mathrm{O}}_{5}$ at $1.5\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{m}$. New determinations of the $^{4}I_{13∕2}$ and $^{4}I_{15∕2}$ crystal-field-level structure for the two crystallographically inequivalent ${\mathrm{Er}}^{3+}$ sites have been made. The fluorescence dynamics of the metastable $^{4}I_{13∕2}:{\mathrm{Y}}_{1}$ excited state was investigated, showing exponential decays for ${\mathrm{Er}}^{3+}$ at both crystallographic sites with fluorescence lifetimes of $11.4\phantom{\rule{0.3em}{0ex}}\mathrm{ms}$ for site 1 and $9.2\phantom{\rule{0.3em}{0ex}}\mathrm{ms}$ for site 2. Exceptionally sharp inhomogeneous absorption lines of 180, 390, and $510\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$ were observed in 0.0015% ${\mathrm{Er}}^{3+}:{\mathrm{Y}}_{2}\mathrm{Si}{\mathrm{O}}_{5}$, 0.005% ${\mathrm{Er}}^{3+}:{\mathrm{Y}}_{2}\mathrm{Si}{\mathrm{O}}_{5}$, and 0.02% ${\mathrm{Er}}^{3+}:{\mathrm{Y}}_{2}\mathrm{Si}{\mathrm{O}}_{5}$ crystals, respectively. The $g$-values for the lowest energy $^{4}I_{15∕2}$ $({\mathrm{Z}}_{1})$ and $^{4}I_{13∕2}$ $({\mathrm{Y}}_{1})$ doublets were measured to be 5.5 and 4.6 for site 1 and 15.0 and 12.9 for site 2 when the magnetic field was oriented along the crystal's ${\mathbit{D}}_{1}$ axis.

DOI
10.1103/physrevb.74.075107

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We present the results of detailed site-selective spectroscopy performed on the 4I15∕2\ensuremath↔4I13∕2^{4}I_{15∕2}\ensuremath{\leftrightarrow}^{4}I_{13∕2}4I15∕2​\ensuremath↔4I13∕2​ transition of Er3+:Y2SiO5{\mathrm{Er}}^{3+}:{\mathrm{Y}}_{2}\mathrm{Si}{\mathrm{O}}_{5}Er3+:Y2​SiO5​ at 1.5\ensuremathμm1.5\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{m}1.5\ensuremathμm. New determinations of the 4I13∕2^{4}I_{13∕2}4I13∕2​ and 4I15∕2^{4}I_{15∕2}4I15∕2​ crystal-field-level structure for the two crystallographically inequivalent Er3+{\mathrm{Er}}^{3+}Er3+ sites have been made. The fluorescence dynamics of the metastable 4I13∕2:Y1^{4}I_{13∕2}:{\mathrm{Y}}_{1}4I13∕2​:Y1​ excited state was investigated, showing exponential decays for Er3+{\mathrm{Er}}^{3+}Er3+ at both crystallographic sites with fluorescence lifetimes of 11.4ms11.4\phantom{\rule{0.3em}{0ex}}\mathrm{ms}11.4ms for site 1 and 9.2ms9.2\phantom{\rule{0.3em}{0ex}}\mathrm{ms}9.2ms for site 2. Exceptionally sharp inhomogeneous absorption lines of 180, 390, and 510MHz510\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}510MHz were observed in 0.0015% Er3+:Y2SiO5{\mathrm{Er}}^{3+}:{\mathrm{Y}}_{2}\mathrm{Si}{\mathrm{O}}_{5}Er3+:Y2​SiO5​, 0.005% Er3+:Y2SiO5{\mathrm{Er}}^{3+}:{\mathrm{Y}}_{2}\mathrm{Si}{\mathrm{O}}_{5}Er3+:Y2​SiO5​, and 0.02% Er3+:Y2SiO5{\mathrm{Er}}^{3+}:{\mathrm{Y}}_{2}\mathrm{Si}{\mathrm{O}}_{5}Er3+:Y2​SiO5​ crystals, respectively. The ggg-values for the lowest energy 4I15∕2^{4}I_{15∕2}4I15∕2​ (Z1)({\mathrm{Z}}_{1})(Z1​) and 4I13∕2^{4}I_{13∕2}4I13∕2​ (Y1)({\mathrm{Y}}_{1})(Y1​) doublets were measured to be 5.5 and 4.6 for site 1 and 15.0 and 12.9 for site 2 when the magnetic field was oriented along the crystal's \mathbitD1{\mathbit{D}}_{1}\mathbitD1​ axis.
Erbium-doped solids are a promising platform for quantum technology due to the Er3+\mathrm{E}{\mathrm{r}}^{3+}Er3+ 1.5-\textmu{}m optical transition in the telecom C band that can offer long coherence times. To characterize the intrinsic C2{\mathrm{C}}_{2}C2​ site of Er3+\mathrm{E}{\mathrm{r}}^{3+}Er3+ in Y2O3{\mathrm{Y}}_{2}{\mathrm{O}}_{3}Y2​O3​ for quantum information and photonic signal-processing applications, absorption and site-selective fluorescence spectroscopy were used to assign the Er3+4I15/2\mathrm{E}{\mathrm{r}}^{3+}\phantom{\rule{4pt}{0ex}}^{4}I_{15/2}Er3+4I15/2​$\ensuremath{\leftrightarrow}$4I13/2^{4}I_{13/2}4I13/2​ transitions. The lowest-to-lowest transition occurs at 1535.608 nm and laser absorption determined an inhomogeneous linewidth of 780 MHz in a 0.005%-doped crystal at 3.4 K. Time-resolved fluorescence established an upper limit for the excited-state lifetime of 8.5 ms. Angular-dependent Zeeman absorption was used to determine ground- and excited-state ggg tensors. The C2{\mathrm{C}}_{2}C2​-site ggg tensor components for the ground state are gx=1.60{g}_{x}=1.60gx​=1.60, gy=4.71{g}_{y}=4.71gy​=4.71, and gz=11.93{g}_{z}=11.93gz​=11.93 with a tipping angle of \ensuremath{\alpha} = $2.{06}^{\ensuremath{\circ}}$, whereas for the excited state the components are gx=1.08{g}_{x}=1.08gx​=1.08, gy=4.36{g}_{y}=4.36gy​=4.36, and gz=10.07{g}_{z}=10.07gz​=10.07 with a tipping angle of \ensuremath{\alpha} = $\ensuremath{-}11.{7}^{\ensuremath{\circ}}$. Optical decoherence can be suppressed by the application of a magnetic field parallel to $\ensuremath{\langle}111\ensuremath{\rangle}$ crystal axes where all C2{\mathrm{C}}_{2}C2​ sites become nearly magnetically equivalent with large ggg values so that spin flips of neighboring Er3+\mathrm{E}{\mathrm{r}}^{3+}Er3+ ions can be simultaneously suppressed. Using this magnetic field direction, two-pulse photon echoes gave a homogeneous linewidth of 5 kHz for an applied magnetic field of 0.5 T, narrowing and saturating at 2.5 kHz at 3.5 T. Decoherence over intermediate magnetic fields was described by spectral diffusion due to $\mathrm{E}{\mathrm{r}}^{3+}\text{\ensuremath{-}}\mathrm{E}{\mathrm{r}}^{3+}$ magnetic dipole interactions driven by the direct phonon process. With Er3+\mathrm{E}{\mathrm{r}}^{3+}Er3+:Y2O3{\mathrm{Y}}_{2}{\mathrm{O}}_{3}Y2​O3​ absorption at a convenient telecom laser wavelength and the ability to fabricate waveguides, our study suggests that this is a promising material system for quantum information and spectral hole-burning signal-processing applications.
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Erbium ions in crystals show considerable promise for the technologies that will form the backbone of future networked quantum information technology. Despite advances in leveraging erbium's fibre-compatible infrared transition for classical and quantum applications, the transitions are, in general, not well understood. We present detailed absorption and laser site-selective spectroscopy of the C3v_{\rm 3v}3v​(O2−^{2-}2−) centre in CaF2_22​:Er3+^{3+}3+ as an interesting erbium site case study. The 4^{4}4I15/2_{15/2}15/2​Z1→4_1 \rightarrow {^{4}}1​→4I13/2_{13/2}13/2​Y1_11​ transition has a low-temperature inhomogeneous linewidth of 1 GHz with hyperfine structure observable from the 167^{167}167Er isotope. A parametrized crystal-field Hamiltonian is fitted to 34 energy levels and the two ground state magnetic splitting factors. The wavefunctions are used to perform a transition intensity analysis and electric-dipole parameters are fitted to absorption oscillator strengths. Simulated spectra for the 4^{4}4I11/2→4_{11/2}\rightarrow {^{4}}11/2​→4I15/2_{15/2}15/2​ and 4^{4}4I13/2→4_{13/2} \rightarrow {^{4}}13/2​→4I15/2_{15/2}15/2​ inter-multiplet transitions are in excellent agreement with the experimentally measured spectra. The 4^{4}4I13/2_{13/2}13/2​ excited state lifetime is 25.0\,ms and the intensity calculation is in excellent agreement with this value.
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