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Journal of Applied Physics

Evaluation of critical distances for energy transfer between Pr3+ and Ce3+ in yttrium aluminium garnet

Peng Zeng, Xiantao Wei, Shaoshuai Zhou, Min Yin, Yonghu Chen

Published Sep 2, 2016• 10 citations
Publisher

Abstract

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.

DOI
10.1063/1.4962018

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physics.atom-phCross-listedarXiv:2604.21374•Apr 24, 2026
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.
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.
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 exploit the upconversion process, utilizing it as a sensitive tool in site-selective spectroscopy of rare earth ion-doped solids. In the Y3Al5O12:Pr3+ praseodymium-doped yttrium aluminum garnet (YAG:Pr) crystals the Pr ions are situated in sites having slightly different environments. Under pulsed excitation into the D21 level, the upconverted emission from the P03 level of each Pr subsystem exhibits its unique, and easily identifiable, response to pulsed excitation, simplifying the process of selectively exciting ions in different sites. Using this technique, we have been able to identify three different sites in a sample of YAG with Pr concentration of 0.5%. We present the physical reasons for the sensitivity of this technique as an example of a useful approach to distinguish among atomic systems residing in slightly dissimilar environments.
Yttrium Aluminum Garnet (YAG) 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.The non-linear energy transfer dynamics of Er:YAG are modeled under high resonant pump conditions. Specifically the multi-photon effect known as excited state absorption (ESA) is modeled by measuring the cross section in a single crystal Er:YAG sample utilizing a pump and probe technique. The measured ESA cross section is then included in the rate equation modeling that has typically been ignored such an effect when modeling the non-linear ion to ion interactions. By pumping with selective resonant pumps, the interaction dynamics of the upper and the lower laser levels in the Erbium ion reveal the contributions of the non-linear energy transfer mechanisms towards the populations of the levels respectively. This thesis work shows the added accuracy of the rate equation modeling by its inclusion of the measured ESA cross-section and its effect on the population evolution in the Er:YAG system. The model will be tested with measurements made with select Er:YAG crystals being pumped by combinations of resonant infra-red lasers with a chopper spinning at a rate on the order of magnitude of the lower lasing level lifetime.
Yttrium aluminum perovskite (YAP) is a host material that can provide a strong emission from a rare-earth dopant and it has a lower phonon energy than yttrium aluminum garnet (YAG). Therefore, YAP is a promising material for optical refrigeration and radiation balanced laser. We measured the photoluminescence (PL) spectra of ytterbium (Yb)-doped YAP and compared them with those of Yb-doped YAG. The estimated ideal laser cooling efficiencies of Yb-doped YAP and Yb-doped YAG were comparable at 300 K. Based on the temperature-dependent anti-Stokes PL, we found that the laser cooling power of Yb-doped YAP at 470 K is 14.3 times higher than that at 200 K. This enhancement at higher temperatures is 3.2 times larger than that observed for Yb-doped YAG. We attributed the higher laser cooling power of Yb-doped YAP to a lower multi-phonon relaxation rate (and/or a higher energy transfer rate) and an antenna effect caused by the energy transfer from Yb ions that are located at the Y-site to Yb ions that are surrounded by an inhomogeneous alloy structure. The calculated small signal gain of (Yb:Y)AP is 3.5 times larger than that of (Yb:Y)AG. The larger small signal gain of (Yb:Y)AP arises from its strong absorbance and small Stark splitting width.
We show in this article the improvements which can be obtained in the description of the luminescence properties of Pr3+ doped materials by using an extension of the Judd-Ofelt theory in order to relax some strong selection rules and approximations of the standard formalism and to better account for the influence of the 4f5d excited electronic configuration. The demonstration is made by re-examining the case of Pr3+:YAG, a well known luminescent and laser crystal with a very low energy 4f5d absorption band. Our extension thus provides a better agreement between calculated and measured absorption intensities, especially for the hypersensitive 3 H4 →\rightarrow→ 3 P2 transition. A comparison is made with the results obtained in the case of Pr3+:ZBLAN, a laser fluoride glass with much higher 4f5d absorption levels. Our investigation also gives the opportunity, in the case of Pr3+:YAG, to provide more complete and more reliable absorption and emission data than reported in the past literature and to exploit these data to better address the question of laser operation at various emission wavelengths. It is thus demonstrated that laser operation should be possible with improved laser performance at 488 nm, 616 nm and 744 nm, as it was already achieved in the past, but also at 566 nm and 931 nm by using appropriate laser cavities and laser mirrors.