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Journal of Physics Condensed Matter

Anti-Stokes emissions and determination of Stark sub-level diagram of Er3+ions in KY3F10

E. Boulma, Madjid Diaf, J.P. Jouart, M. Bouffard, J.L. Doualan, R. Moncorgé

Published Jun 30, 2006• 11 citations
Publisher

Abstract

We are interested, in this work, in determining the Stark sub-level of Er3+ ions doping a KY3F10 single crystal with a molar concentration of 1%. We have used a new method of measurement of energies of the ground level and emitting levels from excitation and anti-Stokes emission spectra recorded at liquid nitrogen temperature. This technique is based on a spectral analysis of the anti-Stokes emissions recorded after selective excitation with a red dye tunable laser. Thus, we could determine the Stark sub-levels of the ground and the principal emitting levels in the infrared, visible and near-UV ranges with a very good precision.

DOI
10.1088/0953-8984/18/29/012

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[Anti-stokes blue fluorescence and stark splitting of 3H4 in Pr3+:Y2SiO5 (YSO)].

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Excited-state absorption measurements of Tm3+-doped crystals

Jakub W. Szela, Jacob I. Mackenzie

High resolution, absolute excited-state absorption (ESA) spectra, at room temperature, from the long-lived 3F4 energy level of several crystals doped with trivalent thulium (Tm3+) ions have been measured employing high-brightness narrowband (FWHM <30 nm) light emitting diodes (LEDs) as a probe wavelength. The aim of this investigation was to determine the strength of ESA channels at wavelengths addressable by commercially available semiconductor laser diodes operating around 630-680 nm. The favourable lifetime of the 3F4 manifold and negligible ground-state absorption (GSA) for the red-wavelength second-step excitation, ensures a direct and efficient route for a dual-wavelength pumping scheme of the thulium ion, which will enable blue-green laser emission from its 1G4 upper-laser level.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•May 14, 2012•3 citations
We are interested, in this work, in determining the Stark sub-level of Er3+ ions doping a KY3F10 single crystal with a molar concentration of 1%. We have used a new method of measurement of energies of the ground level and emitting levels from excitation and anti-Stokes emission spectra recorded at liquid nitrogen temperature. This technique is based on a spectral analysis of the anti-Stokes emissions recorded after selective excitation with a red dye tunable laser. Thus, we could determine the Stark sub-levels of the ground and the principal emitting levels in the infrared, visible and near-UV ranges with a very good precision.
La conversion de lumiere vers les hautes frequences s'effectue selon trois types de mecanismes d'excitation: absorptions successives de plusieurs photons, transfert d'energie entre les ions dans un etat excite et l'avalanche de photons. Ce dernier processus est un effet collectif base sur un transfert d'energie a partir d'un ion a l'etat excite vers un ion a l'etat fondamental. Sous certaines conditions, ces transferts peuvent conduire a une reaction en chaine entrainant une importante augmentation de l'intensite de la fluorescence anti-Stokes. L'objet de ce travail est l'etude systematique de la fluorescence anti-Stokes des ions de terres rares trivalents dans les cristaux du type fluorite. Les etudes que nous presentons ont ete effectuees en utilisant une excitation monochromatique autour de 650 nm fournie par un laser a colorant. Nous avons etudie plus particulierement les ions erbium et thulium dilues dans les monocristaux de KY3F10. Cette etude nous a permis de determiner les sous niveaux Stark des differents multiplets 2S+1LJ des ions Er3+ et Tm3+ a la temperature de l'azote liquide avec une tres bonne precision. Nous avons aussi expose les resultats relatifs a la dynamique de la fluorescence anti-Stokes en analysant la variation de l'intensite de la fluorescence en fonction de la puissance d'excitation et en effectuant des mesures de durees de vie. Nous rapportons aussi les resultats d'une etude spectroscopique et dynamique des emissions anti-Stokes du meme cristal de KY3F10 dope par des ions Tm3+ demontrant l'effet de sensibilisation des ions Er3+, presents a l'etat de traces, sur les raies d'absorption dans l'etat excite du Tm3+
Abstract Emission and visible photoluminescence excitation spectra of CaF2:Er (0.5 at %) crystals have been studied under different optical pumping conditions. The results demonstrate that anti-Stokes luminescence of the erbium-doped crystals has higher intensity in the case of pumping of the 4I13/2 metastable state of the dopant. Resonance IR photon wavelengths have been determined for two-photon excitation of visible emission in CaF2:Er. A method has been developed for the optical modulation of anti-Stokes luminescence, which allows the nature of the corresponding electron transitions in emission centers to be identified.
The coherent anti-Stokes Raman spectroscopy (CARS) of electronic states of the Ce3+ ion in a CeF3 crystal at 3.8 K is reported. CARS resonances involving the ground state of the 2F5/2 manifold and the Stark components of the 2F7/2 manifold at 2161 and 2239 cm−1 have been detected. Measurements were made with both visible (λ1 ≈ 476 nm, λ2 = 532 nm) and near-ultraviolet (λ1 = 355 nm, λ2 ≈ 385 nm) lasers. The enhancement of the third-order susceptibility owing to the electronic transitions, |χ(3)R/χ(3)NR|max, is as great as 4.8. This represents an order-of-magnitude increase over that in singly resonant electronic CARS experiments in other rare-earth crystals. The CARS data also yielded accurate measurements of the Ce3+ electronic Raman cross sections. In the visible region, σzz(2161 cm−1) = (5.0 ± 1.1) × 10−30 cm2 and σzz(2239 cm−1) = (1.9 ± 0.7) × 10−30 cm2. One could calculate both the absolute magnitude and the dispersion of |χ(3)R|max by modeling the virtual intermediate states as a single degenerate 5d state at 45 000 cm−1.
We have measured coherent anti-Stokes Raman spectra between crystal-field levels of the 2^{2}2F5/2{\mathit{F}}_{5/2}F5/2​ and 2^{2}2F7/2{\mathit{F}}_{7/2}F7/2​ manifolds of the Ce3+{\mathrm{Ce}}^{3+}Ce3+ ion diluted in LuPO4{\mathrm{LuPO}}_{4}LuPO4​ at \ensuremath{\sim}10 K. The anti-Stokes signal is nearly resonant with the lowest crystal-field level of the 5d1{\mathit{d}}^{1}d1 configuration of Ce3+{\mathrm{Ce}}^{3+}Ce3+ at 30 460 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$. For a LuPO4{\mathrm{LuPO}}_{4}LuPO4​ crystal doped with 0.06 mol % Ce3+{\mathrm{Ce}}^{3+}Ce3+, we found enhancements of the third-order susceptibility \ensuremath{\Vert}${\mathrm{\ensuremath{\chi}}}^{(3)\mathrm{R}}$/${\mathrm{\ensuremath{\chi}}}^{(3)\mathrm{NR}}$\ensuremath{\Vert} as high as 11.6. This enhancement is over 20 times larger than that seen previously in singly resonant experiments with pure rare-earth crystals.
In the Pr3+ -doped Y2SiO5, the population in 1D2 of Pr3+ can be transferred to 3P0 state via non-radiative energy transfer by the laser excitation in resonance with 3H4-->1D2 , and we can experimentally study the Stark splitting of 3H4 energy level via 3P0 -->3H4 anti-Stokes emission spectra. Because the anti-Stokes emission spectra can avoid the energy transfer between different crystallographic site 1D2 energy levels, the above splitting lines attribution is more accurate than the assignment via 1D2-->3H4 Stokes spectra by the laser excitation in resonance with 3H4-->1D2. In addition, the character of the anti-Stokes fluorescence decay time was observed.
High resolution, absolute excited-state absorption (ESA) spectra, at room temperature, from the long-lived 3F4 energy level of several crystals doped with trivalent thulium (Tm3+) ions have been measured employing high-brightness narrowband (FWHM <30 nm) light emitting diodes (LEDs) as a probe wavelength. The aim of this investigation was to determine the strength of ESA channels at wavelengths addressable by commercially available semiconductor laser diodes operating around 630-680 nm. The favourable lifetime of the 3F4 manifold and negligible ground-state absorption (GSA) for the red-wavelength second-step excitation, ensures a direct and efficient route for a dual-wavelength pumping scheme of the thulium ion, which will enable blue-green laser emission from its 1G4 upper-laser level.