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Physical Review B

Optical decoherence studies of yttrium oxyorthosilicate Y 2 SiO 5 codoped with Er 3 + and Eu 3 + for optical signal processing and quantum information applications at 1.5 microns

Charles W. Thiel, William Randall Babbitt, R. L. Cone

Published May 11, 2012• 38 citations
Publisher

Abstract

We report detailed studies of the optical decoherence and spectroscopic properties of the 1536-nm optical transition of the bandwidth-engineered material 0.02$%$Er:1$%$Eu:Y${}_{2}$SiO${}_{5}$. This work is motivated by the need for comprehensive understanding of new resonant optical materials for spatial-spectral holography and quantum information applications. The dependence of optical decoherence on excitation frequency, applied magnetic field strength and orientation, crystal temperature, measurement time scale, and optical excitation density was studied using stimulated photon echo spectroscopy and time-resolved spectral hole-burning techniques. The effects of weak disorder generated by the introduction of Eu${}^{3+}$ ions into the lattice was probed by comparing measurements across the static disorder-induced distribution of transition frequencies as well as by comparing with measurements on 0.02$%$Er:Y${}_{2}$SiO${}_{5}$. The results reveal that the coherence properties of Er:Y${}_{2}$SiO${}_{5}$ are preserved in the disordered system; moreover, the increased inhomogeneity produced by the disorder acts to suppress optical decoherence by inhibiting the electronic spin diffusion process, improving material properties for low magnetic field strengths and at increased temperatures desirable for practical applications.

DOI
10.1103/physrevb.85.174302

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The mechanisms and effects of spectral diffusion for optical transitions of paramagnetic ions have been explored using the inhomogeneously broadened 1536 nm $^{4}\mathrm{I}_{15∕2}\ensuremath{\rightarrow}^{4}\mathrm{I}_{13∕2}$ transition in ${\mathrm{Er}}^{3+}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$. Using photon echo spectroscopy, spectral diffusion was measured by observing the evolution of the effective coherence lifetimes over time scales from $1\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{s}$ to 20 ms for magnetic-field strengths from 0.3 to 6.0 T, temperatures from 1.6 to 6.5 K, and nominal ${\mathrm{Er}}^{3+}$ concentrations of 0.0015%, 0.005%, and 0.02%. To understand the effect of spectral diffusion on material decoherence for different environmental conditions and material compositions, data and models were compared to identify spectral diffusion mechanisms and microscopic spin dynamics. Observations were successfully modeled by ${\mathrm{Er}}^{3+}\ensuremath{-}{\mathrm{Er}}^{3+}$ magnetic dipole interactions and ${\mathrm{Er}}^{3+}$ electron spin flips driven by the one-phonon direct process. At temperatures of 4.2 K and higher, spectral diffusion due to $^{89}\mathrm{Y}$ nuclear spin flips was also observed. The success in describing our extensive experimental results using simple models provides an important capability for exploring larger parameter spaces, accelerating the design and optimization of materials for spatial-spectral holography, and spectral hole-burning devices. The broad insight into spectral diffusion mechanisms and dynamics is applicable to other paramagnetic materials, such as those containing ${\mathrm{Yb}}^{3+}$ or ${\mathrm{Nd}}^{3+}$.

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Controlled compositional disorder in Er 3 + : Y 2 Si O 5 provides a wide-bandwidth spectral hole burning material at 1.5 μ m

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Physical review. B./Physical review. B•Jul 17, 2024•8 citations
We report detailed studies of the optical decoherence and spectroscopic properties of the 1536-nm optical transition of the bandwidth-engineered material 0.02%Er:1%Eu:Y2{}_{2}2​SiO5{}_{5}5​. This work is motivated by the need for comprehensive understanding of new resonant optical materials for spatial-spectral holography and quantum information applications. The dependence of optical decoherence on excitation frequency, applied magnetic field strength and orientation, crystal temperature, measurement time scale, and optical excitation density was studied using stimulated photon echo spectroscopy and time-resolved spectral hole-burning techniques. The effects of weak disorder generated by the introduction of Eu3+{}^{3+}3+ ions into the lattice was probed by comparing measurements across the static disorder-induced distribution of transition frequencies as well as by comparing with measurements on 0.02%Er:Y2{}_{2}2​SiO5{}_{5}5​. The results reveal that the coherence properties of Er:Y2{}_{2}2​SiO5{}_{5}5​ are preserved in the disordered system; moreover, the increased inhomogeneity produced by the disorder acts to suppress optical decoherence by inhibiting the electronic spin diffusion process, improving material properties for low magnetic field strengths and at increased temperatures desirable for practical applications.
The mechanisms and effects of spectral diffusion for optical transitions of paramagnetic ions have been explored using the inhomogeneously broadened 1536 nm $^{4}\mathrm{I}_{15∕2}\ensuremath{\rightarrow}^{4}\mathrm{I}_{13∕2}$ transition in Er3+:Y2SiO5{\mathrm{Er}}^{3+}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}Er3+:Y2​SiO5​. Using photon echo spectroscopy, spectral diffusion was measured by observing the evolution of the effective coherence lifetimes over time scales from $1\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{s}$ to 20 ms for magnetic-field strengths from 0.3 to 6.0 T, temperatures from 1.6 to 6.5 K, and nominal Er3+{\mathrm{Er}}^{3+}Er3+ concentrations of 0.0015%, 0.005%, and 0.02%. To understand the effect of spectral diffusion on material decoherence for different environmental conditions and material compositions, data and models were compared to identify spectral diffusion mechanisms and microscopic spin dynamics. Observations were successfully modeled by ${\mathrm{Er}}^{3+}\ensuremath{-}{\mathrm{Er}}^{3+}$ magnetic dipole interactions and Er3+{\mathrm{Er}}^{3+}Er3+ electron spin flips driven by the one-phonon direct process. At temperatures of 4.2 K and higher, spectral diffusion due to 89Y^{89}\mathrm{Y}89Y nuclear spin flips was also observed. The success in describing our extensive experimental results using simple models provides an important capability for exploring larger parameter spaces, accelerating the design and optimization of materials for spatial-spectral holography, and spectral hole-burning devices. The broad insight into spectral diffusion mechanisms and dynamics is applicable to other paramagnetic materials, such as those containing Yb3+{\mathrm{Yb}}^{3+}Yb3+ or Nd3+{\mathrm{Nd}}^{3+}Nd3+.
The subgigahertz spectral bandwidth of the lowest energy $1.5\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{m}$ Er3+{\mathrm{Er}}^{3+}Er3+ $^{4}I_{15∕2}\ensuremath{\rightarrow}^{4}I_{13∕2}$ optical transition in Er3+:Y2SiO5{\mathrm{Er}}^{3+}:{\mathrm{Y}}_{2}\mathrm{Si}{\mathrm{O}}_{5}Er3+:Y2​SiO5​ has been increased to $\ensuremath{\sim}22\phantom{\rule{0.3em}{0ex}}\mathrm{GHz}$ by intentionally introducing compositional disorder through codoping with Eu3+{\mathrm{Eu}}^{3+}Eu3+ impurity ions. This illustrates a general bandwidth control technique for spectral hole burning device applications including spatial-spectral holography and quantum computing. Coherence measurements by stimulated photon echoes demonstrated that the increased disorder does not perturb the dynamical properties of the Er3+{\mathrm{Er}}^{3+}Er3+ transition and, thus, gives the desired bandwidth enhancement without penalty in other properties. The echo measurements and model analysis also show that phonon-driven spin flips of Er3+{\mathrm{Er}}^{3+}Er3+ ions in the ground state are responsible for the spectral diffusion that was observed for the optical transition. These results collectively give a better understanding of both the nature of disorder and of the ion-ion interactions in doped materials, and they also enable the high bandwidths required for signal processing and memory applications at $1.5\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{m}$ based on spectral hole burning.
Spatial-spectral holography using spectral hole burning materials is a powerful technique for performing real-time, wide-bandwidth information storage and signal processing. For operation in the important 1.5 μm communication band, the material Er3+:Y2SiO5 enables applications such as laser frequency stabilization, all-optical correlators, analog signal processing, and data storage. Site-selective absorption and emission spectroscopy identified spectral hole burning transitions and excited state T1 lifetimes in the 1.5 μm spectral region. The effects of crystal temperature, Er3+-dopant concentration, magnetic field strength, and crystal orientation on spectral diffusion were explored using stimulated photon echo spectroscopy, which is the "prototype" interaction mechanism for device applications. The performance of Er3+:Y2SiO5 and related Er3+ materials has been dramatically enhanced by reducing the effect of spectral diffusion on the coherence lifetime T2 through fundamental material design coupled with the application of an external magnetic field oriented along specific directions. A preferred magnetic field orientation that maximized T2 by minimizing the effects of spectral diffusion was determined using the results of angle-dependent Zeeman spectroscopy. The observed linewidth broadening due to spectral diffusion was successfully modeled by considering the effect of one-phonon (direct) processes on Er3+ - Er3+ interactions. The reported studies improved our understanding of Er3+ materials, explored the range of conditions and material parameters required to optimize performance for specific applications, and enabled measurement of the narrowest optical resonance ever observed in a solid-with a homogeneous linewidth of 73 Hz. With the optimized materials and operating conditions, photon echoes were observed up to temperatures of 5 K, enabling 0.5 GHz bandwidth optical signal processing at 4.2 K and providing the possibility for operation with a closed-cycle cryocooler.
Enhancement of optical coherence in 167^{167}167Er:Y2_22​SiO5_55​ crystal at sub-Kelvin temperatures
Er3+^{3+}3+:Y2_22​SiO5_55​ crystal is a promising candidate with a great variety of its potential applications in quantum information processing and quantum communications ranging from optical/microwave quantum memories to circuit QED and microwave-to-optics frequency converters. Some of the above listed applications require ultra-low temperature environment, i.e., temperatures T≲0.1 T\lesssim0.1~T≲0.1 K. Most of the experiments with erbium doped crystals have been so far carried out at temperatures above 1.5~K. Therefore, only little information is known about Er3+^{3+}3+:Y2_22​SiO5_55​ coherence properties at millikelvins. Here, we investigate optical decoherence of 167^{167}167Er:Y2_22​SiO5_55​ crystal by performing 2- and 3-pulse echo experiments at millikelvin temperature range and at weak and moderate magnetic fields. We show that the deep freezing of the crystal results in an increase of optical coherence time by one order of magnitude compared to temperature of 1.5 Kelvin and magnetic field of $\sim$0.2~T, taken as a reference point. We further describe the detailed investigation of the decoherence mechanisms in this regime.
Decoherence of the 795 nm 3H6^{3}\mathrm{H}{}_{6}3H6​ to 3H4^{3}\mathrm{H}{}_{4}3H4​ transition in 11%{\mathrm{Tm}}^{3+}:{\mathrm{Y}}_{3}{\mathrm{Ga}}_{5}{\mathrm{O}}_{12}1 (Tm:YGG) is studied at temperatures as low as 1.2 K. The temperature, magnetic field, frequency, and time scale (spectral diffusion) dependence of the optical coherence lifetime is measured. Our results show that the coherence lifetime is impacted less by spectral diffusion than other known thulium-doped materials. Photon echo excitation and spectral hole burning methods reveal uniform decoherence properties and the possibility to produce full transparency for persistent spectral holes across the entire 56 GHz inhomogeneous bandwidth of the optical transition. Temperature-dependent decoherence is well described by elastic Raman scattering of phonons with an additional weaker component that may arise from a low density of glass-like dynamic disorder modes (two-level systems). Analysis of the observed behavior suggests that an optical coherence lifetime approaching 1 ms may be possible in this system at temperatures below 1 K for crystals grown with optimized properties. Overall, we find that Tm:YGG has superior decoherence properties compared to other Tm-doped crystals and is a promising candidate for applications that rely on long coherence lifetimes, such as optical quantum memories and photonic signal processing.
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.