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Physical Review B

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

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

Published Apr 24, 2008• 25 citations
Publisher

Abstract

The subgigahertz spectral bandwidth of the lowest energy $1.5\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{m}$ ${\mathrm{Er}}^{3+}$ $^{4}I_{15∕2}\ensuremath{\rightarrow}^{4}I_{13∕2}$ optical transition in ${\mathrm{Er}}^{3+}:{\mathrm{Y}}_{2}\mathrm{Si}{\mathrm{O}}_{5}$ has been increased to $\ensuremath{\sim}22\phantom{\rule{0.3em}{0ex}}\mathrm{GHz}$ by intentionally introducing compositional disorder through codoping with ${\mathrm{Eu}}^{3+}$ 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 ${\mathrm{Er}}^{3+}$ 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 ${\mathrm{Er}}^{3+}$ 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.

DOI
10.1103/physrevb.77.155125

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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.

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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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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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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.

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R. M. Macfarlane, Y. Sun, Flurin Könz +1 more

Summary form only given. Congruent lithium niobate has a disordered, lithium-deficient structure in which Nb/sub Li/ antisites provide charge compensation for lithium vacancies. The disorder is produced by departures from stoichiometry, which play an important role in the photorefractive properties of lithium niobate, particularly two-color photorefractivity at ambient temperatures. Disorder also increases the inhomogeneous linewidth (/spl Gamma//sub inhom/) of optical transitions of impurity centers, which gives a desirable increase in bandwidth for applications involving low temperature spatial-spectral holography where the frequency and time-domain phenomena of spectral hole burning and photon echoes are combined with that of spatial holography. However it also has the potential to increase the homogeneous linewidth (/spl Gamma//sub hom/) by inducing low frequency tunneling modes or "two-level systems" (TLS), reducing the figure of merit for the time-bandwidth product: F=/spl Gamma//sub inhom///spl Gamma//sub hom/. We investigate the role of disorder in lithium niobate by measuring both the inhomogeneous and homogeneous broadening of optical transitions in Pr/sup 3+/ and Er/sup 3+/ doped lithium niobate where the rare-earth ions are generally accepted to substitute for Li/sup +/ ions in sites of nominally C/sub 3/ symmetry.

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The subgigahertz spectral bandwidth of the lowest energy 1.5\ensuremathμm1.5\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{m}1.5\ensuremathμm Er3+{\mathrm{Er}}^{3+}Er3+ 4I15∕2\ensuremath→4I13∕2^{4}I_{15∕2}\ensuremath{\rightarrow}^{4}I_{13∕2}4I15∕2​\ensuremath→4I13∕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∼22GHz\ensuremath{\sim}22\phantom{\rule{0.3em}{0ex}}\mathrm{GHz}\ensuremath∼22GHz 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\ensuremathμm1.5\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{m}1.5\ensuremathμm based on spectral hole burning.
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+.
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.
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.
Rare-earth-ion (REI) ensembles in crystals have remarkable optical and spin properties characterized by narrow homogeneous linewidths relative to the inhomogeneous ensemble broadening. This makes it possible to precisely tailor the ensemble spectral density and therefore the absorption profile by applying narrow-linewidth radiation to transfer population into auxiliary levels, a process broadly known as spectral hole burning (SHB). REI-doped crystals find applications in information processing, both classical (pattern recognition, filtering, spectral analysis) and quantum (photon storage), all protocols requiring suitable ensemble preparation by SHB as a first step. In Er3+^{3+}3+-doped materials, the longest reported hole lifetime is one minute, and longer lifetimes are desirable. Here, we report SHB and accumulated echo measurements in a scheelite crystal of CaWO4_44​ by pumping the electron spin transition of Er3+^{3+}3+ ions at microwave frequencies and millikelvin temperatures, with nuclear spin states of neighboring 183^{183}183W atoms serving as the auxiliary levels. The lifetime of the holes and accumulated echoes rises steeply as the sample temperature is decreased, exceeding a month at 10 mK. Our results demonstrate that millikelvin temperatures can be beneficial for signal processing applications requiring long spectral hole lifetimes.
Summary form only given. Congruent lithium niobate has a disordered, lithium-deficient structure in which Nb/sub Li/ antisites provide charge compensation for lithium vacancies. The disorder is produced by departures from stoichiometry, which play an important role in the photorefractive properties of lithium niobate, particularly two-color photorefractivity at ambient temperatures. Disorder also increases the inhomogeneous linewidth (/spl Gamma//sub inhom/) of optical transitions of impurity centers, which gives a desirable increase in bandwidth for applications involving low temperature spatial-spectral holography where the frequency and time-domain phenomena of spectral hole burning and photon echoes are combined with that of spatial holography. However it also has the potential to increase the homogeneous linewidth (/spl Gamma//sub hom/) by inducing low frequency tunneling modes or "two-level systems" (TLS), reducing the figure of merit for the time-bandwidth product: F=/spl Gamma//sub inhom///spl Gamma//sub hom/. We investigate the role of disorder in lithium niobate by measuring both the inhomogeneous and homogeneous broadening of optical transitions in Pr/sup 3+/ and Er/sup 3+/ doped lithium niobate where the rare-earth ions are generally accepted to substitute for Li/sup +/ ions in sites of nominally C/sub 3/ symmetry.