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Physical review. B, Condensed matter

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

Hongwei Song, Tomokatsu Hayakawa, Masayuki Nogami

Published May 1, 1999• 15 citations
Publisher

Abstract

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.

DOI
10.1103/physrevb.59.11760

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Room Temperature Hole-Burning in Sm2+-doped Borate Glasses

Kimihiko Hirao

Recently, the interests in optical memory based on persistent spectral hole burning (PSHB) are increased because of its possibility of the application to high density optical memory. PSHB was observed for an organic dye doped in polymer and rear earth or transition metal doped in inorganic crystal or glasses up to now. Since PSHB was observed by two Russian groups (Gorokhovskii et al. and Kharlamov et al.) for free base phthalocyanine in a n-octane Shpol'skii matrix1 and for perylene and 9-aminoacridine molecules in glassy ethanol matrix2, PSHB materials are studied primarily for the polymer doped with an organic dye. But such materials can make hole only at very low temperature. Room temperature PSHB phenomena were observed on Sm2+ doped fluoride crystals3-5 and glasses6 recently, however these materials' Гih(inhomogeneous line width)/Гh(homogeneous line width)'s which are the parameters of data multiplicity in PSHB optical memory are an order of unity. For the application of PSHB materials to optical memory, high operating temperature, high Гih/Гh, and rapid reaction rate are wanted. Glass has a superiority on the view point of optical memory application because of its broad inhomogeneous line width and productivity. Our group has discovered room temperature PSHB for Sm2+ in borate glass systems whose Гih/Гh is 24.7 PSHB for rear earth metal in glass matrix has not been studied seriously, yet. It is thought that the study of the relationship between the optical hole and glass structure is necessary.

Spectral Hole-Burning and Related Spectroscopies: Science and Applications•Jan 1, 1994•0 citations
Persistent spectral hole burning (PSHB) in the 7F0\ensuremath−5D0{}^{7}{F}_{0}{\ensuremath{-}}^{5}{D}_{0}7F0​\ensuremath−5D0​ transition and the electron excitation in the 7F0\ensuremath−4f5d{}^{7}{F}_{0}\ensuremath{-}4f5d7F0​\ensuremath−4f5d transition of Sm2+{\mathrm{Sm}}^{2+}Sm2+ doped in Al2O3\ensuremath−SiO2{\mathrm{Al}}_{2}{\mathrm{O}}_{3}{\ensuremath{-}\mathrm{S}\mathrm{i}\mathrm{O}}_{2}Al2​O3​\ensuremath−SiO2​ 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 Al2O3\ensuremath−SiO2{\mathrm{Al}}_{2}{\mathrm{O}}_{3}{\ensuremath{-}\mathrm{S}\mathrm{i}\mathrm{O}}_{2}Al2​O3​\ensuremath−SiO2​ 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.
Persistent spectral hole burning (PSHB) and light-induced absorption spectra with the pump of burning light were measured and studied in the Sm2+-doped xAl2O3⋅(100−x)SiO2 glasses to reveal the electron transfer and the formation of PSHB at room temperature. It was observed that the density of Sm2+ at the burnt sites decreased, while that of Sm3+ increased after the burning. The hole depth increased with the increase of Al2O3 concentration. The formation of PSHB is attributed to a one-step electron transfer by tunneling through the excited state, D05. The traps that capture the electrons produced by the ionization of Sm2+ may be related to the oxygen vacancies. In addition, the thermal activated barrier height between the burnt and unburnt configuration was estimated as ∼1.0 eV by thermal hole filling.
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.
The persistent spectral hole-burning phenomenon was investigated for Sm2+ ions-doped Al2O3-SiO2 glasses prepared by the sol-gel method. The efficiency of hole-burning, burned at low temperature ~77K, was proportionally increased with the content of OH groups surrounding the rare-earth ions. The proposed mechanism for hole-burning was the optically activated rearrangement of the OH bonds surrounding the rare-earth ions. The burned-hole was thermally refilled and erased above ~200 K. On the other hand, the glasses obtained by heating in H2 gas or irradiating with x-rays showed PSHB up to room temperature. When heated in H2 gas, the H2 molecules react with oxygen ions to form H2O. Removal of the generated H2O causes the number of oxygen ions surrounding rare-earth ions to decrease, resulting into the reduction of the ions. The hole burning in the H2-treated glasses was performed by the electron transfer between the rare-earth ions and the trapping centers. In contrast, in the x-ray irradiated glass, it was concluded that the rear-earth ions are deuced into the divalent state by electron transfer from the oxygen defect center. The hole defect centers are trapped in oxygen ions bound with Al3+ ions. The spectral hole burning of the x-ray irradiated glasses could be burned by the reverse reaction of the reduction of the rare-earth ions. A short distance between the Sm2+ and oxygen defect centers brought a high-speed hole burning, that is, 30 times faster than in a similar H2 gas treated glass.
Persistent spectral hole burning (PSHB) is expected to be a mechanism for future ultrahigh density multi-wavelength optical memory whose density can be higher than the conventional optical memory by 10 to 104 times. PSHB optical memories are mainly studied for dye-doped polymers, but the hole burning temperatures for such poleymers are limited to tempertures lower than 140 K [1], Recently room-temperature PSHB has been observed in Sm2+ doped halide crystals [2-4] and glasses [5], and borate glasses [6]. The halide crystals are not bulk single crystals but polycrystals.
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.
Recently, the interests in optical memory based on persistent spectral hole burning (PSHB) are increased because of its possibility of the application to high density optical memory. PSHB was observed for an organic dye doped in polymer and rear earth or transition metal doped in inorganic crystal or glasses up to now. Since PSHB was observed by two Russian groups (Gorokhovskii et al. and Kharlamov et al.) for free base phthalocyanine in a n-octane Shpol'skii matrix1 and for perylene and 9-aminoacridine molecules in glassy ethanol matrix2, PSHB materials are studied primarily for the polymer doped with an organic dye. But such materials can make hole only at very low temperature. Room temperature PSHB phenomena were observed on Sm2+ doped fluoride crystals3-5 and glasses6 recently, however these materials' Гih(inhomogeneous line width)/Гh(homogeneous line width)'s which are the parameters of data multiplicity in PSHB optical memory are an order of unity. For the application of PSHB materials to optical memory, high operating temperature, high Гih/Гh, and rapid reaction rate are wanted. Glass has a superiority on the view point of optical memory application because of its broad inhomogeneous line width and productivity. Our group has discovered room temperature PSHB for Sm2+ in borate glass systems whose Гih/Гh is 24.7 PSHB for rear earth metal in glass matrix has not been studied seriously, yet. It is thought that the study of the relationship between the optical hole and glass structure is necessary.