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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Spectral hole-burning of rare-earth ions doped in AL 2 O 3 -SiO 2 glass

Masayuki Nogami, Kazuhiro Suzuki

Published Oct 1, 2002• 0 citations
Publisher

Abstract

Al2O3-SiO2 glasses doped with Sm3+ ions were prepared using sol-gel method, in which the Sm3+ ions were reduced into Sm2+ by heaing in H2-gas or irradiating with x-ray. 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 Sm3+ to decrease, resulting into the resuction of the Sm3+ ions. in contrast, in the x-ray irradiated glass, it is concluded that the Sm3+ ions are reduced into Sm2+ by electron transfer from the oxygen defect center. The hole defect centers are trapped in oxygen ions boound with Al3+ ions. The spectral hole burning of the x-ray irradiated glasses could be burned by the reverse reaction of the reduction of Sm3+ ions, that is, the electron transfer from the excited Sm2+ into the surrounding oxygen. A short distance between the Sm2+ and oxygen defect centers brings fast hole burning. On the other hand, the hole burning in the H2-treated glasses was performed by the electron transfer between the Sm2+ and the trapping center such as Sm3+.

DOI
10.1117/12.458829

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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.

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Trap Effect in Spctral Hole Burning of Sm2+ Doped Crystals

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Since the first observation of persistent photon gated spectral hole burning in BaFCl:Sm2+ at liquid helium temperature[1], the successful improvement on this material has been performed in our laboratory by adding bromine and alkline earth metals in the melt to form MyM'1-yFClxBr1-x:Sm (M,M'=Mg, Ca, Sr, Ba; x,y=0-1) system, in which the inhomogeneous line is broadened significantly[2-5] and room temperature hole burning is realized [6]. The hole burning mechanism is found to be photoionization of Sm2+ followed by electron trapping[1]. A kind of principal electron trap is considered to be Sm3+[1], which brings about hole refilling in the holes burnt formerly as burning the next hole because the generated Sm3+ corresponding to the former holes can trap electrons again released in the next hole burning[7]. That means, writing will erase the stored information. To avoiding this effect, introducing an other kind of trap different from Sm3+ for hole burning is necessary In the present paper, we report the results of hole burning in Sm singly doped and Sm, Yb doubly doped SrFCl crystals at 77K and room temperature. Two different trap effects in hole burning are observed and discussed.

Spectral Hole-Burning and Related Spectroscopies: Science and Applications•Jan 1, 1992•0 citations
Al2O3-SiO2 glasses doped with Sm3+ ions were prepared using sol-gel method, in which the Sm3+ ions were reduced into Sm2+ by heaing in H2-gas or irradiating with x-ray. 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 Sm3+ to decrease, resulting into the resuction of the Sm3+ ions. in contrast, in the x-ray irradiated glass, it is concluded that the Sm3+ ions are reduced into Sm2+ by electron transfer from the oxygen defect center. The hole defect centers are trapped in oxygen ions boound with Al3+ ions. The spectral hole burning of the x-ray irradiated glasses could be burned by the reverse reaction of the reduction of Sm3+ ions, that is, the electron transfer from the excited Sm2+ into the surrounding oxygen. A short distance between the Sm2+ and oxygen defect centers brings fast hole burning. On the other hand, the hole burning in the H2-treated glasses was performed by the electron transfer between the Sm2+ and the trapping center such as Sm3+.
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) 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.
Two kinds of Sm-doped Strontium Borates, SrB 4 O 7 (STB) and SrB 6 O 10 (SHB), were prepared for the spectral hole-burning experiment. Sm 3+ -ions doped into the STB were well reduced to Sm 2+ -ions in air environment. Though partial reduction was observed in SHB, the Sm 3+ -ions successfully reduced in the subsequent X-ray irradiation (SHBX). Permanent spectral hole-burning experiments were conducted for 7 F 0 – 5 D 1 transition band of Sm 2+ -ions. The two samples STB and SHBX showed deep spectral holes at room temperature and 50 K, i.e., 40 and 72% of hole depths in STB and SHBX at 50 K, respectively. The STB showed type I hole-burning properties and SHBX type II. The spectral holes were sustained for over 24 h at room temperature. Multiple holes were burnt in an inhomogeneously broadened band to demonstrate the optical data storage in the frequency domain.
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.
Since the first observation of persistent photon gated spectral hole burning in BaFCl:Sm2+ at liquid helium temperature[1], the successful improvement on this material has been performed in our laboratory by adding bromine and alkline earth metals in the melt to form MyM'1-yFClxBr1-x:Sm (M,M'=Mg, Ca, Sr, Ba; x,y=0-1) system, in which the inhomogeneous line is broadened significantly[2-5] and room temperature hole burning is realized [6]. The hole burning mechanism is found to be photoionization of Sm2+ followed by electron trapping[1]. A kind of principal electron trap is considered to be Sm3+[1], which brings about hole refilling in the holes burnt formerly as burning the next hole because the generated Sm3+ corresponding to the former holes can trap electrons again released in the next hole burning[7]. That means, writing will erase the stored information. To avoiding this effect, introducing an other kind of trap different from Sm3+ for hole burning is necessary In the present paper, we report the results of hole burning in Sm singly doped and Sm, Yb doubly doped SrFCl crystals at 77K and room temperature. Two different trap effects in hole burning are observed and discussed.