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Acta Physica Sinica

Vacuum ultraviolet spectroscopic properties and 4f5d state of Pr3+doped YAG

Meng Chun-Xia, Huang Shi-Hua, You Fang-Tian, Chang Jian-Jun, Hongshang Peng, Ye Tao, Zhang Guobin, (1)北京交通大学光电子技术研究所, 北京 100044; (2)中国科学技术大学国家同步辐射实验室, 合肥 230026; (3)中国科学院高能物理研究所同步辐射实验室,北京 100039

Published Jan 1, 2005• 2 citations
Publisher

Abstract

Yttrium aluminum garnet (YAG): Pr3+ is synthesized by codeposition me thod. Vacuum ultraviolet (VUV) excitation and emission spectra of YAG: Pr3+ at different temperatures are measured using synchrotron radiation as an excitation source. We analyze the transition process after excitation to 4f5d en ergy band and estimate the Huang-Rhys factor S and phonon energy ηω of YAG: Pr 3+ by multi-phonon relaxation. Emission of self-trapped exciton (STE) and 3P0→3H4,5,6 emission transferr ed from the STE energy appear when YAG: Pr3+is excited by 170nm, whic h is a different transition process from those excited by 240nm and 289nm.

DOI
10.7498/aps.54.5468

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Journal de Physique IV (Proceedings)•Apr 1, 1994•14 citations
Yttrium aluminum garnet (YAG): Pr3+ is synthesized by codeposition me thod. Vacuum ultraviolet (VUV) excitation and emission spectra of YAG: Pr3+ at different temperatures are measured using synchrotron radiation as an excitation source. We analyze the transition process after excitation to 4f5d en ergy band and estimate the Huang-Rhys factor S and phonon energy ηω of YAG: Pr 3+ by multi-phonon relaxation. Emission of self-trapped exciton (STE) and 3P0→3H4,5,6 emission transferr ed from the STE energy appear when YAG: Pr3+is excited by 170nm, whic h is a different transition process from those excited by 240nm and 289nm.
A series of Pr3+/Ce3+ doped yttrium aluminium garnet (Y3Al5O12 or simply YAG) phosphors were synthesized to investigate the energy transfer between Pr3+ and Ce3+ for their potential application in a white light-emitting diode and quantum information storage and processing. The excitation and emission spectra of YAG:Pr3+/Ce3+ were measured and analyzed, and it revealed that the reabsorption between Pr3+ and Ce3+ was so weak that it can be ignored, and the energy transfer from Pr3+ (5d) to Ce3+ (5d) and Ce3+ (5d) to Pr3+ (1D2) did occur. By analyzing the excitation and the emission spectra, the energy transfer from Pr3+ (5d) to Ce3+ (5d) and Ce3+ (5d) to Pr3+ (1D2) was examined in detail with an original strategy deduced from fluorescence dynamics and the Dexter energy transfer theory, and the critical distances of energy transfer were derived to be 7.9 Å and 4.0 Å for Pr3+ (5d) to Ce3+ (5d) and Ce3+ (5d) to Pr3+ (1D2), respectively. The energy transfer rates of the two processes of various concentrations were discussed and evaluated. Furthermore, for the purpose of sensing a single Pr3+ state with a Ce3+ ion, the optimal distance of Ce3+ from Pr3+ was evaluated as 5.60 Å, where the probability of success reaches its maximum value of 78.66%, and meanwhile the probabilities were evaluated for a series of Y3+ sites in a YAG lattice. These results will be of valuable reference for achievement of the optimal energy transfer efficiency in Pr3+/Ce3+ doped YAG and other similar systems.
The spectra of luminescence and magnetic circular polarization of luminescence in the 1 D 2 → 3 F 4 emission band in thulium:yttrium-aluminum garnet Tm3+:YAG (Tm3+:Y3Al5O12) have been investigated at temperatures T = 78 and 293 K, respectively. Based on the analysis of the magnetooptical and optical spectra, the optical transitions between the Stark sublevels of the 3 F 4 and 1 D 2 multiplets in Tm3+:YAG were identified. It is shown that the symmetry and energies of the Stark sublevels of the 3 F 4, 1 D 2, and 3 H 6 multiplets, found experimentally from magnetic and magnetooptical studies, confirm the results of theoretical calculations of the energy spectrum of the rare earth Tm3+ ion in YAG.
Excited-state absorption spectra obtained by a pulsed pump–probe technique specially designed for the near-UV spectral domain were recorded in three Pr3+-doped fluoride crystals (KY3F10,LiYF4, and BaY2F8). These excited-state absorption spectra correspond to optical transitions from the 3P0 or the 1D2 metastable levels of the 4f2 configuration up to the first energy levels of the 4f5d electronic configuration. The position, the anisotropic behavior, and the line shape of the observed excited-state absorption bands are discussed and compared with ground-state absorption (from level 3H4) or direct excitation spectra available in the literature. Subsequently, two-step excitation into the 4f5d high-lying energy levels of Pr3 by means of 3P0 and 1D2 is shown to be an efficient way to produce broadband UV fluorescence by use of pump beams in the blue and the near UV.
Intensity-dependent optical dephasing is shown to arise from nonresonant excitation of 1% Pr3+{\mathrm{Pr}}^{3+}Pr3+-doped yttrium aluminum garnet (YAG) with UV radiation between 325--355 nm. UV irradiation of the sample with intensities greater than 30 MW/cm2{\mathrm{cm}}^{2}cm2 produces persistent changes in the optical dephasing. Two-pulse photon echo decays on the 3^{3}3H4{\mathit{H}}_{4}H4​${\ensuremath{\rightarrow}}^{1}$D2{\mathit{D}}_{2}D2​ transition of Pr3+{\mathrm{Pr}}^{3+}Pr3+ were measured at 1.5 K before and after exposure to UV radiation. Changes persisting for at least several hours are observed in the echo intensity, echo decay rate, and temporal form of the echo decay. Changes persist if the sample is kept below 10 K, but warming to 77 K results in the echo decays resuming their initial intensity and duration. No change is detected in the optical absorption spectrum of the Pr3+{\mathrm{Pr}}^{3+}Pr3+ ions after UV exposure, indicating that most of the ions remain in that charge state. Although the mechanism giving rise to the increased optical dephasing is not completely understood, the additional dynamics may arise from the UV radiation freeing electrons that become trapped in lattice defects. The presence of the dephasing at low temperatures indicates the availability of low-energy excitations of the electronic system.
Yttrium Aluminum Garnet (YAG, Y_3 〖Al〗_5 O_12) crystals doped with Erbium have posed an interesting position in the field of rare earth solid state lasers as they possess the property of self-saturation, in which the upper energy level in a laser has a much shorter lifetime than that of the lower level. This is the case of the 2.94μm transition in Er:YAG. That property at first seems to make this material unfit for use as a laser gain medium, however further research into these classes of rare earth materials revealed interesting non-liner energy transfer mechanisms that allow it to be a useful mid wave infra-red (MWIR) coherent source in the continuous wave (CW) and pulsed regimes. This came to fruition due to decades of modeling and spectroscopic research investigating the non-linear energy transfer mechanisms of excited state absorption (ESA), energy transfer up-conversion (ETU), and cross relaxation (XR). These effects show up in the rise and fall times of the levels observed through fluorescence. Resulting in the non-exponential rise and fall characteristics and having a squared or even cubed relation to the population. The population evolution for each of the lasing levels is now affected by ions recycling energy and in turn cause the lifetimes of the levels to “effectively” change to a point where simple linear models do not adequately describe the system and its performance. The non-linear energy transfer dynamics of Er:YAG are modeled under high resonant pump conditions. By pumping with selective resonant pumps, the interaction dynamics of the (_ ^4)I_(11/2) and the (_ ^4)I_(13/2) levels in the Erbium ion reveal the contributions from generally ignored non-linear energy transfer mechanisms. Specifically, the multi-photon effect known as excited state absorption (ESA) is modeled by measuring and characterizing the cross section in single crystal Er:YAG samples utilizing a pump and probe technique coupled with transient fluorescence measurements. The measured ESA cross section is then included in the rate equation modeling.
We report on the first observation of low temperature pulsed blue and orange laser emissions in Pr3+:YAG. Furthermore, we compare these results with similar observations in YLiF4 and YAlO3 doped crystals. Pulsed laser oscillations were obtained in crystals with uncoated surfaces by direct excitation of one of the relevant Stark components of the 3P0, 3P1 or 3P2 states. A carefull spectroscopic analysis of all these systems allows to clearly identify the laser transitions as arising from the 3P0 metastable state, the lifetime of which has been measured using a nanosecond pumped dye laser.