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Applied Physics Letters

Internal photopumping of Nd3+ (2H9/2, 4F5/2) states in yttrium aluminum garnet by excitation transfer from oxygen deficiency centers and Fe3+ continuum emission

J. Darby Hewitt, Thomas M. Spinka, Andrey A. Senin, James Gary Eden

Published Jul 18, 2011• 7 citations
Publisher

Abstract

Photoexcitation of Nd3+ (2H9/2, 4F5/2) states by the broad (∼70 nm FWHM), near-infrared continuum provided by Fe3+ has been observed at 300 K in bulk yttrium aluminum garnet (YAG) crystals doped with trace concentrations (<50 ppm) of Fe, Cr, and Eu. Irradiation of YAG at 248 nm with a KrF laser, which excites the oxygen deficiency center (ODC) in YAG having peak absorption at ∼240 nm, culminates in ODC→Fe3+ excitation transfer and subsequent Fe3+ emission. This internal optical pumping mechanism for rare earth ions is unencumbered by the requirement for donor-acceptor proximity that constrains conventional Förster-Dexter excitation transfer in co-doped crystals.

DOI
10.1063/1.3614001

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Photoexcitation of Nd3+ (2H9/2, 4F5/2) states by the broad (∼70 nm FWHM), near-infrared continuum provided by Fe3+ has been observed at 300 K in bulk yttrium aluminum garnet (YAG) crystals doped with trace concentrations (<50 ppm) of Fe, Cr, and Eu. Irradiation of YAG at 248 nm with a KrF laser, which excites the oxygen deficiency center (ODC) in YAG having peak absorption at ∼240 nm, culminates in ODC→Fe3+ excitation transfer and subsequent Fe3+ emission. This internal optical pumping mechanism for rare earth ions is unencumbered by the requirement for donor-acceptor proximity that constrains conventional Förster-Dexter excitation transfer in co-doped crystals.
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.
Using a laser diode modulated at 250 and 500 MHz, dependence of enhanced absorption on both sample length and temperature was investigated in an erbium doped yttrium aluminum garnet crystal. The transmitted laser intensity decreased with a decay time of 300 ps for sample lengths greater than 3.0 mm and temperatures higher than 50 K when the incident laser intensity increased. In addition, an emission peak was observed near 835 nm corresponding to the transition from the S3/24 level to the I13/24 in Er3+. It was suggested that the enhanced absorption was caused by stimulated emission in three excited states.
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.
Rare-earth-doped laser materials show strong prospects for quantum information storage and processing, as well as for biological imaging, due to their high-Q 4f↔4f optical transitions. However, the inability to optically detect single rare-earth dopants has prevented these materials from reaching their full potential. Here we detect a single photostable Pr3+ ion in yttrium aluminium garnet nanocrystals with high contrast photon antibunching by using optical upconversion of the excited state population of the 4f↔4f optical transition into ultraviolet fluorescence. We also demonstrate on-demand creation of Pr3+ ions in a bulk yttrium aluminium garnet crystal by patterned ion implantation. Finally, we show generation of local nanophotonic structures and cell death due to photochemical effects caused by upconverted ultraviolet fluorescence of praseodymium-doped yttrium aluminium garnet in the surrounding environment. Our study demonstrates versatile use of rare-earth atomic-size ultraviolet emitters for nanoengineering and biotechnological applications. The optical transitions that occur in rare-earth-doped crystals offer promise for quantum information storage and processing. Kolesovet al.report the optical detection of a single praseodymium ion residing in a crystal host by using an excited-state absorption process to enhance its fluorescence yield.
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.
Negative nonlinear absorption, which causes the transmission to decrease as the laser intensity increases, was observed in a 16 at. % Er:YAG crystal using a laser diode operating at 787 and 784 nm. This effect for 787 nm was strong because 787 nm was the center of an absorption peak that is related to the excited-state absorption from 4I13/2 to 2H11/2. It is suggested that these phenomena take place because the absorption cross section from 4I13/2 to 2H11/2 is larger than that from 4I15/2 to 4I9/2 using a double-absorption model.