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Physical review. B, Condensed matter

Temperature dependence of the homogeneous width of Eu3+ spectral lines in silicate glass measured by accumulated photon echoes

Ryuzi Yano, Masaharu Mitsunaga, Naoshi Uesugi, Makoto Shimizu

Published Oct 1, 1994• 23 citations
Publisher

Abstract

The temperature-dependent homogeneous width of the $^{5}$${\mathit{D}}_{0\mathrm{\ensuremath{-}}}^{7}$${\mathit{F}}_{0}$ transition of ${\mathrm{Eu}}^{3+}$ in a pure silicate glass fiber has been measured by accumulated photon echoes between 1.6 and 44 K. The temperature dependence of the homogeneous width shows a crossover from T-linear (T7 K) to ${\mathit{T}}^{2}$ (T>7 K). The whole temperature dependence of the homogeneous width between 1.6 and 44 K can be explained by the configurational changes of the glass which is modeled by two-level systems (TLS's) and a Raman process involving low-frequency vibrational modes of the silicate glass (the rotations of ${\mathrm{SiO}}_{4}$ tetrahedra). The T-linear temperature dependence is attributed to the TLS process. The anomalous ${\mathit{T}}^{2}$ dependence down to 10 K cannot be explained by only one process, but can be explained by the contributions of both the TLS process and the Raman process. Above 40 K, the Raman process becomes the dominant dephasing mechanism.

DOI
10.1103/physrevb.50.9031

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The temperature-dependent homogeneous width of the ^{5}$${\mathit{D}}_{0\mathrm{\ensuremath{-}}}^{7}$${\mathit{F}}_{0} transition of Eu3+{\mathrm{Eu}}^{3+}Eu3+ in a pure silicate glass fiber has been measured by accumulated photon echoes between 1.6 and 44 K. The temperature dependence of the homogeneous width shows a crossover from T-linear (T7 K) to T2{\mathit{T}}^{2}T2 (T>7 K). The whole temperature dependence of the homogeneous width between 1.6 and 44 K can be explained by the configurational changes of the glass which is modeled by two-level systems (TLS's) and a Raman process involving low-frequency vibrational modes of the silicate glass (the rotations of SiO4{\mathrm{SiO}}_{4}SiO4​ tetrahedra). The T-linear temperature dependence is attributed to the TLS process. The anomalous T2{\mathit{T}}^{2}T2 dependence down to 10 K cannot be explained by only one process, but can be explained by the contributions of both the TLS process and the Raman process. Above 40 K, the Raman process becomes the dominant dephasing mechanism.
Measurements of the homogeneous width of the 4^{4}4 G5/2{\mathrm{G}}_{5\mathrm{/}2}G5/2​ , 2^{2}2 G7/2{\mathrm{G}}_{7\mathrm{/}2}G7/2​ ${\mathrm{\ensuremath{-}}}^{4}$ I9/2{\mathrm{I}}_{9\mathrm{/}2}I9/2​ transition of Nd3+{\mathrm{Nd}}^{3+}Nd3+ in a silicate glass fiber at low temperatures by the technique of accumulated photon echoes show that the dephasing processes are one-phonon processes between the Stark levels of Nd3+{\mathrm{Nd}}^{3+}Nd3+ . These dephasing processes differ from the commonly observed processes of rare-earth ion-doped glasses: the local-configurational-change-induced dephasing process and the Raman process with low-frequency modes. The densely distributed Stark levels of the 4^{4}4 G5/2{\mathrm{G}}_{5\mathrm{/}2}G5/2​ and 2^{2}2 G7/2{\mathrm{G}}_{7\mathrm{/}2}G7/2​ states are responsible for one-phonon processes. The transition-wavelength dependences of the homogeneous widths ${\mathrm{\ensuremath{\Gamma}}}_{\mathrm{h}}$ (4.2 K) and ${\mathrm{\ensuremath{\Gamma}}}_{\mathrm{h}}$ (T\ensuremath{\rightarrow}0) are explained by using the one-phonon process model.
Optical dephasing and specific heat measurements were performed on two rare-earth-doped silicate glasses. The effective homogeneous linewidth of the optical transition, ${\mathrm{\ensuremath{\Gamma}}}_{\mathrm{hom}}$ was compared to the two-level-system (TLS) contribution to the specific heat, CvTLS{\mathit{C}}_{\mathit{v}}^{\mathrm{TLS}}CvTLS​, between 0.4 and 12 K. Both ${\mathrm{\ensuremath{\Gamma}}}_{\mathrm{hom}}$ and CvTLS{\mathit{C}}_{\mathit{v}}^{\mathrm{TLS}}CvTLS​ vary as ${\mathit{T}}^{\mathrm{\ensuremath{\alpha}}}$ with the same value of \ensuremath{\alpha} for a given rare-earth/glass sample, but with different \ensuremath{\alpha} for the two samples (\ensuremath{\alpha}=1.3 for the Pr3+{\mathrm{Pr}}^{3+}Pr3+/glass, \ensuremath{\alpha}=1.0 for Eu3+{\mathrm{Eu}}^{3+}Eu3+/glass). From the ratio of ${\mathrm{\ensuremath{\Gamma}}}_{\mathrm{hom}}$ to CvTLS{\mathit{C}}_{\mathit{v}}^{\mathrm{TLS}}CvTLS​ for each glass, it appears that the coupling strengths to the TLS for each rare-earth optical transition are similar, but that the density of TLS differ due to their different compositions.
Two-pulse photon-echo measurements were made on the 7^{7}7F0{\mathit{F}}_{0}F0​${\mathrm{\ensuremath{\leftrightarrows}}}^{5}$D0{\mathit{D}}_{0}D0​ optical transition in a number of crystalline samples of Y2{\mathrm{Y}}_{2}Y2​O3{\mathrm{O}}_{3}O3​:Eu3+{\mathrm{Eu}}^{3+}Eu3+ prepared by three different crystal-growth techniques. For crystals prepared by a laser-heated pedestal growth or arc-imaging furnace process, we report the observation of an additional sample-dependent contribution to the optical dephasing in comparison with a crystal grown by flame fusion. The dephasing rate 1/Tm{\mathit{T}}_{\mathit{m}}Tm​ at 1.4 K is up to two orders of magnitude faster than that previously reported for the flame-fusion-grown crystal, and is uncorrelated with concentration. Measurements up to 14 K show that 1/Tm{\mathit{T}}_{\mathit{m}}Tm​ increases linearly with temperature, in contrast to the expected T7{\mathit{T}}^{7}T7 behavior due to a two-phonon Raman process. The linear temperature dependence is similar to that seen in glasses and disordered crystalline systems, suggesting the presence of disorder in the samples with more rapid dephasing. The crystals were examined by x-ray diffraction, excitation spectroscopy, and near-field optical microscopy to provide information on the nature of the disorder. The effect of annealing on the crystal dynamics is also investigated.
Erbium-doped solids are promising candidates for fiber-based quantum networks due to their emission wavelength, which aligns with the telecom band over which optical fibers exhibit minimal loss. Among these, erbium-doped silica fiber (EDF) stands out for its availability, ease of use, and seamless integration with existing fiber-optic infrastructure. In this work, using the two-pulse photon-echo (2PPE) technique, we measured the homogeneous linewidth of the 4 I 13/2 ↔ 4 I 15/2 optical transition under varying magnetic fields and temperatures. We observed an effective homogeneous linewidth of approximately 8 kHz at ∼7mK at an optimal magnetic field of 0.09 T, representing over two orders of magnitude improvement compared to earlier reports measured at T ≈700mK. We also present a comprehensive model for the combined magnetic field and temperature dependency of the effective homogeneous linewidth. Additionally, we employed three-pulse photon-echo (3PPE) measurements to investigate spectral diffusion and decoherence processes and conclude that Two-Level System (TLS) effects are significantly suppressed at sufficiently low temperatures, below ∼100mK.