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Photon echo studies of rare-earth-activated materials for optical memory and signal processing devices

Randy W. Equall

Published Jan 1, 1995• 1 citation
OpenAlex

Abstract

The optical spectroscopy and dynamics of three materials; Eu^3+:Y2SiO5, Pr^3+:Y2SiO5, and Tm^3+:Y2SiO5 that are of interest for application in persistent spectral holeburning optical memory and signal processing devices were investigated using linear and nonlinear spectroscopic techniques.Two-pulse photon echoes have been used to measure the homogeneous linewidths.The effects of instantaneous spectral diffusion were systematically studied to allow accurate determination of the optical resonance widths, and external magnetic fields were applied to characterize the effects of fluctuating nuclear spins of the host lattice on dephasing of the dopant ion.The 7F0 → 5D0 transition of 0.1% Eu^3+ in the two crystallographic sites of Y2SiO5 was studied using photon echoes.Using this material, we succeeded in measuring the narrowest optical resonance in a solid by shielding the crystal from stray electromagnetic fields and using sufficiently low laser power to minimize contributions from instantaneous diffusion.The homogeneous linewidths measured in a magnetic field of 100 G are 122 Hz (site 1) and 167 Hz (site 2).These widths are dominated by population decay, but up to 20 Hz is attributed to 89Y spin fluctuations which have been reduced by the applied magnetic field.Similar studies were performed to determine the contributions to the homogeneous linewidth of the 3H4(1) → 1D2(1) transition for both sites of 0.02% Pr^3+ in Y2SiO5.Linewidths of 2.1 kHz (site 1) and 0.85 kHz (site 2) were obtained with an applied magnetic field of 77 G.A significant contribution of 89Y nuclear spin fluctuations to the zero-field homogeneous linewidth was found.Optically detected nuclear magnetic resonance measurements determined the hyperfine structure of the 3H4 ground state for each site, and photon echo nuclear double resonance was used to determine the hyperfine levels of the lowest component of the 1D2 manifold. 3) 2.1? Ec,2S

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Homogeneous broadening and hyperfine structure of optical transitions in Pr 3 + : Y 2 SiO 5

Randy W. Equall, R. L. Cone, R. M. Macfarlane

Contributions to the homogeneous linewidth of the $^{3}$${\mathit{H}}_{4}$(1)${\ensuremath{\rightarrow}}^{1}$${\mathit{D}}_{2}$(1) transition for the two crystallographic sites of ${\mathrm{Pr}}^{3+}$ in ${\mathrm{Y}}_{2}$${\mathrm{SiO}}_{5}$ have been investigated using photon echoes. The effects of excitation-intensity-dependent dephasing or instantaneous diffusion were systematically studied to allow accurate determination of the optical resonance widths. Homogeneous linewidths of 2.8 kHz (site 1) and 1 kHz (site 2) were measured with no applied magnetic field and with sufficiently low laser intensity to minimize the effects of instantaneous diffusion. Using the same excitation intensity, widths of 2.1 kHz (site 1) and 0.85 kHz (site 2) were obtained with an applied magnetic field of 77 G, demonstrating a significant contribution of $^{89}\mathrm{Y}$ nuclear-spin fluctuations to the zero-field homogeneous linewidth. Extrapolation to zero excitation intensity yielded optical resonance widths that were only slightly narrower than the measured values. Optically detected nuclear magnetic resonance measurements determined the hyperfine structure of the $^{3}$${\mathit{H}}_{4}$ ground state for each site; the hyperfine levels of the lowest component of the $^{1}$${\mathit{D}}_{2}$ manifold for each site were determined using photon echo nuclear double resonance. The relatively large oscillator strength of 3\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}7}$ for a rare-earth ion, in conjunction with long dephasing times makes this material a useful candidate for demonstration of time-domain signal processing and optical data storage.

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Nonlinear laser spectroscopy of Eu^3+:Y_2SiO_5 and its application to time-domain optical memory

Ryuzi Yano, Masaharu Mitsunaga, Naoshi Uesugi

Linear- and nonlinear-optical properties of Eu3+:Y2SiO5 have been investigated. All the energy levels of the7F0,1,2,… ground-state manifold and the 5D0,1,2 excited-state manifold were identified, and they were found to be doubly structured because of the two inequivalent optical sites. Two absorption lines of the 7F0–5D0 transition were studied in detail by using nonlinear spectroscopic techniques, photon-echo and stimulated-photon-echo methods. It was found by the photon-echo measurement that the optical dephasing time for one site is extremely long and is excitation-intensity dependent. With the smallest possible intensity we observed the longest ever dephasing time in a solid, 822 μs, or a 387-Hz homogeneous linewidth. From the stimulated-photon-echo measurement, the linewidth was found to be constant over a wide range of time scales, implying the absence of spectral diffusion in this crystal. These quite advantageous properties of this crystal were used for the demonstration of two novel types of time-domain optical data readout: time- and frequency-domain hybrid optical memory and spectrally programmed coherent transients.

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Material optimization of Er3+:Y 2 SiO 5 at 1.5 μm for optical processing, memory, and laser frequency stabilization applications

Thomas Boettger, Yongchen Sun, Charles W. Thiel +1 more

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.

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Ultraslow optical dephasing in Eu 3 + : Y 2 SiO 5

Randy W. Equall, Yazhou Sun, R. L. Cone +1 more

We report the measurement of what we believe to be the narrowest known optical resonance in a solid. This was made on the $^{7}$${\mathit{F}}_{0}$${\ensuremath{\rightarrow}}^{5}$${\mathit{D}}_{0}$ transition of ${\mathrm{Eu}}^{3+}$:${\mathrm{Y}}_{2}$${\mathrm{SiO}}_{5}$ at 1.4 K using photon echoes with sufficiently low laser power to almost eliminate contributions from instantaneous diffusion. The optical resonance widths measured for ${\mathrm{Eu}}^{3+}$ ions in the two crystallographic sites of ${\mathrm{Y}}_{2}$${\mathrm{SiO}}_{5}$ and in a magnetic field of 100 G are 122 Hz (site 1) and 167 Hz (site 2). These widths are dominated by population decay, but up to 20 Hz is attributed to $^{89}\mathrm{Y}$ spin fluctuations which have been reduced by the applied magnetic field.

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Photon echo, spectral hole burning, and optically detected magnetic resonance in Yb 3 + 171 : LiNbO 3 bulk crystal and waveguides

F. Chiossi, Eloïse Lafitte-Houssat, Kangwei Xia +11 more

Recent progress in the realization of high-quality optical resonators and waveguides along with the possibility to incorporate rare-earth ions, make lithium niobate a promising material to build integrated platforms for quantum information processing. $^{171}\mathrm{Yb}^{3+}$ is a particularly attractive system because it can show long coherence lifetimes at zero magnetic field thanks to transitions insensitive to magnetic field fluctuations. In this paper, we investigate the optical and spin properties of $^{171}\mathrm{Yb}^{3+}$ ions in ${\mathrm{LiNbO}}_{3}$ bulk crystals as well as implanted waveguides. Using hole-burning spectroscopy and optically detected magnetic resonance, we studied ground and excited state hyperfine structures and probed optical and spin spectral holes. Importantly, the hole linewidths suggest that part of the ions in the waveguides are in a similar environment as in the bulk sample. We furthermore characterized spin population relaxation and coherence lifetimes of $^{171}\mathrm{Yb}^{3+}$ ions in the bulk crystal at temperatures between 50 mK and 9 K. At low temperatures, ${T}_{2}$ up to 9.5 $\ensuremath{\mu}\mathrm{s}$ (34 kHz homogeneous linewidth) and spin relaxation rates as long as $\ensuremath{\approx}100$ ms were measured. Our results show that $^{171}\mathrm{Yb}^{3+}$:$\mathrm{Li}\mathrm{Nb}{\mathrm{O}}_{3}$ is a system that exhibits narrow optical homogeneous linewidths over a 50 GHz bandwidth together with an electron spin degree of freedom. This is of interest for a variety of applications in integrated quantum photonics such as quantum memories or quantum processors.

Physical review. B./Physical review. B•May 31, 2022•7 citations

LASER FREQUENCY STABILIZATION TO SPECTRAL HOLE BURNING FREQUENCY REFERENCES IN ERBIUM-DOPED CRYSTALS: MATERIAL AND DEVICE OPTIMIZATION

Thomas Böttger

Narrow spectral holes in the absorption lines of Er doped crystals have been explored as references for frequency stabilizing external cavity diode lasers at the important 1.5 μm optical communication wavelength. Allan deviations of the beat signal between two independent stabilized lasers as low as 200 Hz over 10 ms integration time have been achieved using regenerative spectral holes in Er:Y2SiO5 and Er:KTP, while drift was reduced to ~ 7 kHz/min by incorporating the inhomogeneous absorption line as a fixed reference. During active stabilization, the transient spectral hole was continuously regenerated as hole burning balanced relaxation. In contrast, persistent spectral holes in Er:D:CaF2, with lifetimes of several weeks, provided programmable and transportable secondary frequency references that maintained sub-kilohertz stability over several seconds and enabled 6 kHz stability over 3 1.6 10 s × . The error signal was derived from the spectral hole transmission using frequency modulation spectroscopy. A servo amplifier applied fast frequency corrections to the injection current of the laser diode and slower adjustments to the piezo-driven feedback prism plate. These stabilized lasers provide ideal sources for spectral hole burning applications based on optical coherent transients, where laser stability is required over the storage time of the material. Since the lifetime of the frequency reference is exactly the material storage time, this requirement is automatically met by using our technique. This was demonstrated in Er:Y2SiO5 and successfully transferred to high-bandwidth signal processing applications. The material Er:Y2SiO5 was optimized for these applications. The I15/2 and I13/2 crystal field levels were site-selectively determined by absorption and fluorescence spectroscopy. The excited state lifetime was measured to be 11.4 ms for site 1 and 9.2 ms for site 2. Zeeman experiments and two-pulse photon echo spectroscopy as a function of magnetic field orientation were used to determine the anisotropic electronic g-values for both Er sites and established a preferred magnetic field orientation for minimizing homogeneous line broadening by spectral diffusion. The spectral diffusion was characterized by stimulated photon echo spectroscopy and successfully described with established theories. In a 0.02 atomic percent Er:Y2SiO5 crystal at B = 0.8 T and T = 1.6 K, line broadening became significant after 10 μs, increasing the homogeneous linewidth from 7.5 kHz to 75 kHz after 120 μs. Spectral diffusion, primarily caused by direct phonon driven Er spin-flips in the ground state, can be controlled to negligible levels with proper magnetic field strength and orientation, temperature, and erbium concentration. In optimizing Er:Y2SiO5, the narrowest optical resonance in any solid-state material of 73 Hz was measured.

•Jan 1, 2002•15 citations
The optical spectroscopy and dynamics of three materials; Eu^3+:Y2SiO5, Pr^3+:Y2SiO5, and Tm^3+:Y2SiO5 that are of interest for application in persistent spectral holeburning optical memory and signal processing devices were investigated using linear and nonlinear spectroscopic techniques.Two-pulse photon echoes have been used to measure the homogeneous linewidths.The effects of instantaneous spectral diffusion were systematically studied to allow accurate determination of the optical resonance widths, and external magnetic fields were applied to characterize the effects of fluctuating nuclear spins of the host lattice on dephasing of the dopant ion.The 7F0 → 5D0 transition of 0.1% Eu^3+ in the two crystallographic sites of Y2SiO5 was studied using photon echoes.Using this material, we succeeded in measuring the narrowest optical resonance in a solid by shielding the crystal from stray electromagnetic fields and using sufficiently low laser power to minimize contributions from instantaneous diffusion.The homogeneous linewidths measured in a magnetic field of 100 G are 122 Hz (site 1) and 167 Hz (site 2).These widths are dominated by population decay, but up to 20 Hz is attributed to 89Y spin fluctuations which have been reduced by the applied magnetic field.Similar studies were performed to determine the contributions to the homogeneous linewidth of the 3H4(1) → 1D2(1) transition for both sites of 0.02% Pr^3+ in Y2SiO5.Linewidths of 2.1 kHz (site 1) and 0.85 kHz (site 2) were obtained with an applied magnetic field of 77 G.A significant contribution of 89Y nuclear spin fluctuations to the zero-field homogeneous linewidth was found.Optically detected nuclear magnetic resonance measurements determined the hyperfine structure of the 3H4 ground state for each site, and photon echo nuclear double resonance was used to determine the hyperfine levels of the lowest component of the 1D2 manifold. 3) 2.1? Ec,2S
Contributions to the homogeneous linewidth of the 3^{3}3H4{\mathit{H}}_{4}H4​(1)${\ensuremath{\rightarrow}}^{1}$D2{\mathit{D}}_{2}D2​(1) transition for the two crystallographic sites of Pr3+{\mathrm{Pr}}^{3+}Pr3+ in Y2{\mathrm{Y}}_{2}Y2​SiO5{\mathrm{SiO}}_{5}SiO5​ have been investigated using photon echoes. The effects of excitation-intensity-dependent dephasing or instantaneous diffusion were systematically studied to allow accurate determination of the optical resonance widths. Homogeneous linewidths of 2.8 kHz (site 1) and 1 kHz (site 2) were measured with no applied magnetic field and with sufficiently low laser intensity to minimize the effects of instantaneous diffusion. Using the same excitation intensity, widths of 2.1 kHz (site 1) and 0.85 kHz (site 2) were obtained with an applied magnetic field of 77 G, demonstrating a significant contribution of 89Y^{89}\mathrm{Y}89Y nuclear-spin fluctuations to the zero-field homogeneous linewidth. Extrapolation to zero excitation intensity yielded optical resonance widths that were only slightly narrower than the measured values. Optically detected nuclear magnetic resonance measurements determined the hyperfine structure of the 3^{3}3H4{\mathit{H}}_{4}H4​ ground state for each site; the hyperfine levels of the lowest component of the 1^{1}1D2{\mathit{D}}_{2}D2​ manifold for each site were determined using photon echo nuclear double resonance. The relatively large oscillator strength of 3\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}7}$ for a rare-earth ion, in conjunction with long dephasing times makes this material a useful candidate for demonstration of time-domain signal processing and optical data storage.
Linear- and nonlinear-optical properties of Eu3+:Y2SiO5 have been investigated. All the energy levels of the7F0,1,2,… ground-state manifold and the 5D0,1,2 excited-state manifold were identified, and they were found to be doubly structured because of the two inequivalent optical sites. Two absorption lines of the 7F0–5D0 transition were studied in detail by using nonlinear spectroscopic techniques, photon-echo and stimulated-photon-echo methods. It was found by the photon-echo measurement that the optical dephasing time for one site is extremely long and is excitation-intensity dependent. With the smallest possible intensity we observed the longest ever dephasing time in a solid, 822 μs, or a 387-Hz homogeneous linewidth. From the stimulated-photon-echo measurement, the linewidth was found to be constant over a wide range of time scales, implying the absence of spectral diffusion in this crystal. These quite advantageous properties of this crystal were used for the demonstration of two novel types of time-domain optical data readout: time- and frequency-domain hybrid optical memory and spectrally programmed coherent transients.
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.
We report the measurement of what we believe to be the narrowest known optical resonance in a solid. This was made on the 7^{7}7F0{\mathit{F}}_{0}F0​${\ensuremath{\rightarrow}}^{5}$D0{\mathit{D}}_{0}D0​ transition of Eu3+{\mathrm{Eu}}^{3+}Eu3+:Y2{\mathrm{Y}}_{2}Y2​SiO5{\mathrm{SiO}}_{5}SiO5​ at 1.4 K using photon echoes with sufficiently low laser power to almost eliminate contributions from instantaneous diffusion. The optical resonance widths measured for Eu3+{\mathrm{Eu}}^{3+}Eu3+ ions in the two crystallographic sites of Y2{\mathrm{Y}}_{2}Y2​SiO5{\mathrm{SiO}}_{5}SiO5​ and in a magnetic field of 100 G are 122 Hz (site 1) and 167 Hz (site 2). These widths are dominated by population decay, but up to 20 Hz is attributed to 89Y^{89}\mathrm{Y}89Y spin fluctuations which have been reduced by the applied magnetic field.
Recent progress in the realization of high-quality optical resonators and waveguides along with the possibility to incorporate rare-earth ions, make lithium niobate a promising material to build integrated platforms for quantum information processing. 171Yb3+^{171}\mathrm{Yb}^{3+}171Yb3+ is a particularly attractive system because it can show long coherence lifetimes at zero magnetic field thanks to transitions insensitive to magnetic field fluctuations. In this paper, we investigate the optical and spin properties of 171Yb3+^{171}\mathrm{Yb}^{3+}171Yb3+ ions in LiNbO3{\mathrm{LiNbO}}_{3}LiNbO3​ bulk crystals as well as implanted waveguides. Using hole-burning spectroscopy and optically detected magnetic resonance, we studied ground and excited state hyperfine structures and probed optical and spin spectral holes. Importantly, the hole linewidths suggest that part of the ions in the waveguides are in a similar environment as in the bulk sample. We furthermore characterized spin population relaxation and coherence lifetimes of 171Yb3+^{171}\mathrm{Yb}^{3+}171Yb3+ ions in the bulk crystal at temperatures between 50 mK and 9 K. At low temperatures, T2{T}_{2}T2​ up to 9.5 $\ensuremath{\mu}\mathrm{s}$ (34 kHz homogeneous linewidth) and spin relaxation rates as long as $\ensuremath{\approx}100$ ms were measured. Our results show that 171Yb3+^{171}\mathrm{Yb}^{3+}171Yb3+:LiNbO3\mathrm{Li}\mathrm{Nb}{\mathrm{O}}_{3}LiNbO3​ is a system that exhibits narrow optical homogeneous linewidths over a 50 GHz bandwidth together with an electron spin degree of freedom. This is of interest for a variety of applications in integrated quantum photonics such as quantum memories or quantum processors.
Narrow spectral holes in the absorption lines of Er doped crystals have been explored as references for frequency stabilizing external cavity diode lasers at the important 1.5 μm optical communication wavelength. Allan deviations of the beat signal between two independent stabilized lasers as low as 200 Hz over 10 ms integration time have been achieved using regenerative spectral holes in Er:Y2SiO5 and Er:KTP, while drift was reduced to ~ 7 kHz/min by incorporating the inhomogeneous absorption line as a fixed reference. During active stabilization, the transient spectral hole was continuously regenerated as hole burning balanced relaxation. In contrast, persistent spectral holes in Er:D:CaF2, with lifetimes of several weeks, provided programmable and transportable secondary frequency references that maintained sub-kilohertz stability over several seconds and enabled 6 kHz stability over 3 1.6 10 s × . The error signal was derived from the spectral hole transmission using frequency modulation spectroscopy. A servo amplifier applied fast frequency corrections to the injection current of the laser diode and slower adjustments to the piezo-driven feedback prism plate. These stabilized lasers provide ideal sources for spectral hole burning applications based on optical coherent transients, where laser stability is required over the storage time of the material. Since the lifetime of the frequency reference is exactly the material storage time, this requirement is automatically met by using our technique. This was demonstrated in Er:Y2SiO5 and successfully transferred to high-bandwidth signal processing applications. The material Er:Y2SiO5 was optimized for these applications. The I15/2 and I13/2 crystal field levels were site-selectively determined by absorption and fluorescence spectroscopy. The excited state lifetime was measured to be 11.4 ms for site 1 and 9.2 ms for site 2. Zeeman experiments and two-pulse photon echo spectroscopy as a function of magnetic field orientation were used to determine the anisotropic electronic g-values for both Er sites and established a preferred magnetic field orientation for minimizing homogeneous line broadening by spectral diffusion. The spectral diffusion was characterized by stimulated photon echo spectroscopy and successfully described with established theories. In a 0.02 atomic percent Er:Y2SiO5 crystal at B = 0.8 T and T = 1.6 K, line broadening became significant after 10 μs, increasing the homogeneous linewidth from 7.5 kHz to 75 kHz after 120 μs. Spectral diffusion, primarily caused by direct phonon driven Er spin-flips in the ground state, can be controlled to negligible levels with proper magnetic field strength and orientation, temperature, and erbium concentration. In optimizing Er:Y2SiO5, the narrowest optical resonance in any solid-state material of 73 Hz was measured.