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Physical review. B, Condensed matter

Spectral hole burning in Eu3+ -doped highly porous γ -aluminum oxide

S.P. Feofilov, Alexander A. Kaplyanskii, R. I. Zakharchenya, Y. Sun, K. W. Jang, Richard S. Meltzer

Published Aug 1, 1996• 43 citations
Publisher

Abstract

Transient and persistent spectral holes were burned in the $^{7}F_{0}\ensuremath{-}^{5}D_{0}$ transition of ${\mathrm{Eu}}^{3+}$ ions in macromonolithic transparent porous nanocrystalline $\ensuremath{\gamma}$-${\mathrm{Al}}_{2}$${\mathrm{O}}_{3}$ produced by sol-gel technology. An unusual temperature dependence of the transient hole width was observed that differs markedly from that in either crystalline or disordered systems. This temperature dependence is explained in terms of Raman processes involving sizeresonant vibrations of the nanoparticles comprising the structure. Possible mechanisms of hole burning are suggested.

DOI
10.1103/physrevb.54.r3690

Related papers

Persistent and transient spectral hole burning in Pr3+ - and Eu3+ -doped silicate glasses

Thomas Schmidt, R. M. Macfarlane, Silvia Volker

Persistent and time-resolved transient holes were burnt into the $^{1}\mathrm{D}_{2}$${\ensuremath{\leftarrow}}^{3}$${\mathrm{H}}_{4}$ transition of ${\mathrm{Pr}}^{3+}$ and the $^{5}\mathrm{D}_{0}$${\ensuremath{\leftarrow}}^{7}$${\mathrm{F}}_{0}$ transition of ${\mathrm{Eu}}^{3+}$ in silicate glasses. The holewidths were studied as a function of burning-fluence density, wavelength, and temperature between 0.4 and 12 K. Transient holes arising from optical pumping of ground-state nuclear hyperfine levels were found for both ions at T3 K. Their lifetime decreases with increasing temperature. They are accompanied by symmetrically placed antiholes. For ${\mathrm{Eu}}^{3+}$, two pairs of antiholes were found which are attributed to the two europium isotopes, $^{151}\mathrm{Eu}$ and $^{153}\mathrm{Eu}$. For ${\mathrm{Pr}}^{3+}$, an additional mechanism leading to persistent hole burning dominates above 3 K. The holewidth follows a ${\mathit{T}}^{(1.3\ifmmode\pm\else\textpm\fi{}0.1)}$ dependence for ${\mathrm{Pr}}^{3+}$ and a ${\mathit{T}}^{(1.0\ifmmode\pm\else\textpm\fi{}0.1)}$ dependence for ${\mathrm{Eu}}^{3+}$. The temperature dependence is the same as that of the contribution of the two-level systems to the specific heat measured on the same samples and in the same temperature range. The quadrupole splittings of the $^{7}\mathrm{F}_{0}$ ground state and the crystal-field splittings of the $^{7}\mathrm{F}_{1}$ and $^{7}\mathrm{F}_{2}$ levels of ${\mathrm{Eu}}^{3+}$ as a function of excitation wavelength indicate that the strength of the noncubic component of the crystal field varies monotonically for excitation across the $^{5}\mathrm{D}_{0}$${\ensuremath{\leftarrow}}^{7}$${\mathrm{F}}_{0}$ absorption band, falling to zero at the long-wavelength edge. The hole width shows a similar variation with excitation frequency. No influence of the experimental time scale on the hole width was detected for either sample between ${10}^{\mathrm{\ensuremath{-}}2}$ and ${10}^{2}$ s.

Physical review. B, Condensed matter•Dec 1, 1994•57 citations

Spectral hole burning and excited electrons in Sm2+ -doped Al2O3−SiO2 glasses

Masayuki Nogami, Yoshihiro Abe

Persistent spectral hole burning in the $f\ensuremath{\rightarrow}f$ transition and changes in the $f\ensuremath{\rightarrow}d$ transition spectra upon laser irradiation were investigated in ${\mathrm{Sm}}^{2+}$-doped ${\mathrm{Al}}_{2}{\mathrm{O}}_{3}{\ensuremath{-}\mathrm{S}\mathrm{i}\mathrm{O}}_{2}$ glasses prepared by a sol-gel process. The hole was burned in the ${}^{7}{F}_{0}{\ensuremath{\rightarrow}}^{5}{D}_{0}$ line of ${\mathrm{Sm}}^{2+}$ ions using a DCM dye laser at 77 K and the dependence of the burning efficiency on laser power and burning time was measured. The hole depth increased with increasing laser irradiation time, reaching up to $\ensuremath{\sim}12%$ of the total intensity within a few hundred seconds. Neither an antihole around the burned hole nor a change in the fluorescence line narrowing spectrum were observed after hole burning. The hole depth linearly increased with increasing the incident laser power up to $\ensuremath{\sim}1{\mathrm{W}/\mathrm{m}\mathrm{m}}^{2},$ indicating a single-photon hole-burning process. On the other hand, laser irradiation with a wavelength corresponding to the energy of the ${4f}^{6}\ensuremath{\rightarrow}{4f}^{5}5d$ transition resulted in a decrease of both the absorption and fluorescence intensities but no formation of a hole. It was concluded that the electrons excited in the ${4f}^{5}5d$ level were further excited into the conduction band of the host matrix by a two-photon absorption process and then captured in the trapping center.

Physical review. B, Condensed matter•Jul 1, 1997•41 citations

Spectral hole burning quantum efficiency and electron traps in Sm2+ -ion-doped aluminosilicate glasses

Hongwei Song, Tomokatsu Hayakawa, Masayuki Nogami

Persistent spectral hole burning (PSHB) in the ${}^{7}{F}_{0}{\ensuremath{-}}^{5}{D}_{0}$ transition and the electron excitation in the ${}^{7}{F}_{0}\ensuremath{-}4f5d$ transition of ${\mathrm{Sm}}^{2+}$ doped in ${\mathrm{Al}}_{2}{\mathrm{O}}_{3}{\ensuremath{-}\mathrm{S}\mathrm{i}\mathrm{O}}_{2}$ glasses were studied from the measurements of hole burning efficiency and the refilling of the burnt hole. The PSHB at low temperature is attributed to the optically activated rearrangement of OH bonds surrounding ${\mathrm{Sm}}^{2+}$ ions. On the other hand, the PSHB at high temperature is attributed to one-step electron tunneling in the excitation state. The barrier heights for hole filling corresponding to the two mechanisms were determined to be \ensuremath{\sim}0.27 and \ensuremath{\sim}0.90 eV, respectively. Thermal depth of the trap that captures electrons by two-step ionization via the $4f5d$ state was determined to be \ensuremath{\sim}0.35 eV below the conduction band. A model was proposed for describing the PSHB and electron excitation of ${\mathrm{Sm}}^{2+}$ doped in ${\mathrm{Al}}_{2}{\mathrm{O}}_{3}{\ensuremath{-}\mathrm{S}\mathrm{i}\mathrm{O}}_{2}$ glasses. In addition, the dependence of hole burning efficiency on the ${\mathrm{Al}}_{2}{\mathrm{O}}_{3}$ concentration, temperature, and burning wavelength was also studied.

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Time-resolved ultranarrow optical hole burning of a crystalline solid: Y_2O_3:Eu^3+

Matthew J. Sellars, Richard S. Meltzer, Peter Fisk +1 more

Optical hole burning is used to study optical dephasing of the 7F0 ⇒ 5D0 transition in samples of Y2O3:Eu3+ grown by both flame fusion and laser-heated pedestal growth. The samples exhibited a wide variation in their low-temperature hole widths, and the measured hole linewidths were in reasonable agreement with homogeneous linewidths obtained from values of T2 that were determined with two-pulse photon echoes. The sample that had the longest value of T2 (510 μs) from the echo measurements gave a hole width of 3.5 kHz. This is believed to be the narrowest spectral feature observed directly in the frequency domain for a solid. Other samples produced wider holes that were not correlated with the Eu3+ impurity concentrations. Time-resolved hole burning in one of the samples showed a slow and continuous broadening of the spectral hole from 130 kHz at 3 ms to 900 kHz at 10 s after hole burning. It is suggested that the additional broadening is associated with some form of disorder modes in this ordered crystalline solid.

Journal of the Optical Society of America B•Aug 1, 1994•35 citations

Power-gated spectral holeburning in MgS:Eu2+, Eu3+: A case for high-density persistent spectral holeburning

Z. Hasan, Levent Biyikli, P. I. Macfarlane

We present the case of photoionization-induced holeburning in rare-earth-doped II–VI compounds for high-density persistent holeburning. In this case, the photoproduct of holeburning is distributed across the entire zero-phonon line. This maximizes the total number of possible spectral holes that can be burned into an inhomogeneous line as well as produces holes that are photoerasable. Experimental data on photon-gated holeburning in MgS:Eu2+, Eu3+ are presented. With the proper choice of the host electronic band structure, the optically active rare-earth ion and its electronic transitions involved in the holeburning process, to the best of our knowledge we have observed the highest number of photon-gated holes ever burned in a single electronic transition. The features of these holes are that they suffer no detectable erasure after several thousands of read cycles, they survive thermal cycling to ∼150 K, and they are completely photoerasable. A special case of photon-gated holeburning, power-gated holeburning, was employed to demonstrate that, in such systems, a single laser can be used for burning, reading, and erasing of the spectral holes.

Applied Physics Letters•Jun 29, 1998•20 citations

Optical dephasing, hyperfine structure, and hyperfine relaxation associated with the 580.8-nm F07 −5 D0 transition of europium in Eu3+ : Y2 O3

William Randall Babbitt, A. Lezama, THOMAS W. MOSSBERG

We have employed spectral-hole-burning, coherent-transient, and optical-rf double-resonance techniques to measure various parameters associated with the 580.8-nm $^{7}\mathrm{F}_{0}$${\mathrm{\ensuremath{-}}}^{5}$${\mathrm{D}}_{0}$ transition of ${\mathrm{Eu}}^{3+}$ doped into ${\mathrm{Y}}_{2}$${\mathrm{O}}_{3}$. In particular, we have measured the hyperfine splittings of the terminal levels (for both $^{151}\mathrm{Eu}$ and $^{153}\mathrm{Eu}$), an effective thermalization rate of the ground-state ${(}^{7}$${\mathrm{F}}_{0}$) hyperfine manifold over the temperature range of \ensuremath{\simeq}4--15 K, and the homogeneous linewidth of the optical transition over the range of \ensuremath{\simeq}14--35 K. Large ratios of inhomogeneous to homogeneous linewidth at elevated temperatures (${10}^{3}$ at 25 K) and long ground-state hyperfine thermalization times (>30 h at 4 K) make this an interesting crystal in the context of spectrally addressable optical memories.

Physical review. B, Condensed matter•Feb 1, 1989•70 citations
Transient and persistent spectral holes were burned in the 7F0\ensuremath−5D0^{7}F_{0}\ensuremath{-}^{5}D_{0}7F0​\ensuremath−5D0​ transition of Eu3+{\mathrm{Eu}}^{3+}Eu3+ ions in macromonolithic transparent porous nanocrystalline \ensuremathγ\ensuremath{\gamma}\ensuremathγ-{\mathrm{Al}}_{2}$${\mathrm{O}}_{3} produced by sol-gel technology. An unusual temperature dependence of the transient hole width was observed that differs markedly from that in either crystalline or disordered systems. This temperature dependence is explained in terms of Raman processes involving sizeresonant vibrations of the nanoparticles comprising the structure. Possible mechanisms of hole burning are suggested.
Persistent and time-resolved transient holes were burnt into the 1D2^{1}\mathrm{D}_{2}1D2​${\ensuremath{\leftarrow}}^{3}$H4{\mathrm{H}}_{4}H4​ transition of Pr3+{\mathrm{Pr}}^{3+}Pr3+ and the 5D0^{5}\mathrm{D}_{0}5D0​${\ensuremath{\leftarrow}}^{7}$F0{\mathrm{F}}_{0}F0​ transition of Eu3+{\mathrm{Eu}}^{3+}Eu3+ in silicate glasses. The holewidths were studied as a function of burning-fluence density, wavelength, and temperature between 0.4 and 12 K. Transient holes arising from optical pumping of ground-state nuclear hyperfine levels were found for both ions at T3 K. Their lifetime decreases with increasing temperature. They are accompanied by symmetrically placed antiholes. For Eu3+{\mathrm{Eu}}^{3+}Eu3+, two pairs of antiholes were found which are attributed to the two europium isotopes, 151Eu^{151}\mathrm{Eu}151Eu and 153Eu^{153}\mathrm{Eu}153Eu. For Pr3+{\mathrm{Pr}}^{3+}Pr3+, an additional mechanism leading to persistent hole burning dominates above 3 K. The holewidth follows a ${\mathit{T}}^{(1.3\ifmmode\pm\else\textpm\fi{}0.1)}$ dependence for Pr3+{\mathrm{Pr}}^{3+}Pr3+ and a ${\mathit{T}}^{(1.0\ifmmode\pm\else\textpm\fi{}0.1)}$ dependence for Eu3+{\mathrm{Eu}}^{3+}Eu3+. The temperature dependence is the same as that of the contribution of the two-level systems to the specific heat measured on the same samples and in the same temperature range. The quadrupole splittings of the 7F0^{7}\mathrm{F}_{0}7F0​ ground state and the crystal-field splittings of the 7F1^{7}\mathrm{F}_{1}7F1​ and 7F2^{7}\mathrm{F}_{2}7F2​ levels of Eu3+{\mathrm{Eu}}^{3+}Eu3+ as a function of excitation wavelength indicate that the strength of the noncubic component of the crystal field varies monotonically for excitation across the 5D0^{5}\mathrm{D}_{0}5D0​${\ensuremath{\leftarrow}}^{7}$F0{\mathrm{F}}_{0}F0​ absorption band, falling to zero at the long-wavelength edge. The hole width shows a similar variation with excitation frequency. No influence of the experimental time scale on the hole width was detected for either sample between ${10}^{\mathrm{\ensuremath{-}}2}$ and 102{10}^{2}102 s.
Persistent spectral hole burning in the $f\ensuremath{\rightarrow}f$ transition and changes in the $f\ensuremath{\rightarrow}d$ transition spectra upon laser irradiation were investigated in Sm2+{\mathrm{Sm}}^{2+}Sm2+-doped ${\mathrm{Al}}_{2}{\mathrm{O}}_{3}{\ensuremath{-}\mathrm{S}\mathrm{i}\mathrm{O}}_{2}$ glasses prepared by a sol-gel process. The hole was burned in the ${}^{7}{F}_{0}{\ensuremath{\rightarrow}}^{5}{D}_{0}$ line of Sm2+{\mathrm{Sm}}^{2+}Sm2+ ions using a DCM dye laser at 77 K and the dependence of the burning efficiency on laser power and burning time was measured. The hole depth increased with increasing laser irradiation time, reaching up to $\ensuremath{\sim}12%$ of the total intensity within a few hundred seconds. Neither an antihole around the burned hole nor a change in the fluorescence line narrowing spectrum were observed after hole burning. The hole depth linearly increased with increasing the incident laser power up to $\ensuremath{\sim}1{\mathrm{W}/\mathrm{m}\mathrm{m}}^{2},$ indicating a single-photon hole-burning process. On the other hand, laser irradiation with a wavelength corresponding to the energy of the ${4f}^{6}\ensuremath{\rightarrow}{4f}^{5}5d$ transition resulted in a decrease of both the absorption and fluorescence intensities but no formation of a hole. It was concluded that the electrons excited in the 4f55d{4f}^{5}5d4f55d level were further excited into the conduction band of the host matrix by a two-photon absorption process and then captured in the trapping center.
Persistent spectral hole burning (PSHB) in the ${}^{7}{F}_{0}{\ensuremath{-}}^{5}{D}_{0}$ transition and the electron excitation in the ${}^{7}{F}_{0}\ensuremath{-}4f5d$ transition of Sm2+{\mathrm{Sm}}^{2+}Sm2+ doped in ${\mathrm{Al}}_{2}{\mathrm{O}}_{3}{\ensuremath{-}\mathrm{S}\mathrm{i}\mathrm{O}}_{2}$ glasses were studied from the measurements of hole burning efficiency and the refilling of the burnt hole. The PSHB at low temperature is attributed to the optically activated rearrangement of OH bonds surrounding Sm2+{\mathrm{Sm}}^{2+}Sm2+ ions. On the other hand, the PSHB at high temperature is attributed to one-step electron tunneling in the excitation state. The barrier heights for hole filling corresponding to the two mechanisms were determined to be \ensuremath{\sim}0.27 and \ensuremath{\sim}0.90 eV, respectively. Thermal depth of the trap that captures electrons by two-step ionization via the 4f5d4f5d4f5d state was determined to be \ensuremath{\sim}0.35 eV below the conduction band. A model was proposed for describing the PSHB and electron excitation of Sm2+{\mathrm{Sm}}^{2+}Sm2+ doped in ${\mathrm{Al}}_{2}{\mathrm{O}}_{3}{\ensuremath{-}\mathrm{S}\mathrm{i}\mathrm{O}}_{2}$ glasses. In addition, the dependence of hole burning efficiency on the Al2O3{\mathrm{Al}}_{2}{\mathrm{O}}_{3}Al2​O3​ concentration, temperature, and burning wavelength was also studied.
Optical hole burning is used to study optical dephasing of the 7F0 ⇒ 5D0 transition in samples of Y2O3:Eu3+ grown by both flame fusion and laser-heated pedestal growth. The samples exhibited a wide variation in their low-temperature hole widths, and the measured hole linewidths were in reasonable agreement with homogeneous linewidths obtained from values of T2 that were determined with two-pulse photon echoes. The sample that had the longest value of T2 (510 μs) from the echo measurements gave a hole width of 3.5 kHz. This is believed to be the narrowest spectral feature observed directly in the frequency domain for a solid. Other samples produced wider holes that were not correlated with the Eu3+ impurity concentrations. Time-resolved hole burning in one of the samples showed a slow and continuous broadening of the spectral hole from 130 kHz at 3 ms to 900 kHz at 10 s after hole burning. It is suggested that the additional broadening is associated with some form of disorder modes in this ordered crystalline solid.
We present the case of photoionization-induced holeburning in rare-earth-doped II–VI compounds for high-density persistent holeburning. In this case, the photoproduct of holeburning is distributed across the entire zero-phonon line. This maximizes the total number of possible spectral holes that can be burned into an inhomogeneous line as well as produces holes that are photoerasable. Experimental data on photon-gated holeburning in MgS:Eu2+, Eu3+ are presented. With the proper choice of the host electronic band structure, the optically active rare-earth ion and its electronic transitions involved in the holeburning process, to the best of our knowledge we have observed the highest number of photon-gated holes ever burned in a single electronic transition. The features of these holes are that they suffer no detectable erasure after several thousands of read cycles, they survive thermal cycling to ∼150 K, and they are completely photoerasable. A special case of photon-gated holeburning, power-gated holeburning, was employed to demonstrate that, in such systems, a single laser can be used for burning, reading, and erasing of the spectral holes.
We have employed spectral-hole-burning, coherent-transient, and optical-rf double-resonance techniques to measure various parameters associated with the 580.8-nm 7F0^{7}\mathrm{F}_{0}7F0​${\mathrm{\ensuremath{-}}}^{5}$D0{\mathrm{D}}_{0}D0​ transition of Eu3+{\mathrm{Eu}}^{3+}Eu3+ doped into Y2{\mathrm{Y}}_{2}Y2​O3{\mathrm{O}}_{3}O3​. In particular, we have measured the hyperfine splittings of the terminal levels (for both 151Eu^{151}\mathrm{Eu}151Eu and 153Eu^{153}\mathrm{Eu}153Eu), an effective thermalization rate of the ground-state (7{(}^{7}(7F0{\mathrm{F}}_{0}F0​) hyperfine manifold over the temperature range of \ensuremath{\simeq}4--15 K, and the homogeneous linewidth of the optical transition over the range of \ensuremath{\simeq}14--35 K. Large ratios of inhomogeneous to homogeneous linewidth at elevated temperatures (103{10}^{3}103 at 25 K) and long ground-state hyperfine thermalization times (>30 h at 4 K) make this an interesting crystal in the context of spectrally addressable optical memories.