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Physical review. B, Condensed matter

Optical-absorption and photoionization measurements from the excited states of Ce 3 + : Y 3 Al 5 O 12

D. S. Hamilton, Swapan Kumar Gayen, Gerald J. Pogatshnik, R.D. Ghen, William J. Miniscalco

Published May 1, 1989• 143 citations
Publisher

Abstract

The optical transitions in ${\mathrm{Ce}}^{3+}$:${\mathrm{Y}}_{3}$${\mathrm{Al}}_{5}$${\mathrm{O}}_{12}$ from the lowest 5d excited state of the ${\mathrm{Ce}}^{3+}$ ion to the host conduction band have been investigated. Two spatially overlapped and time-sequenced laser pulses were used to observe directly the excited-state absorption (ESA) and the two-step photoionization of the cerium ions. The peak cross section of the ESA transition is (1.0\ifmmode\pm\else\textpm\fi{}0.3)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}17}$ ${\mathrm{cm}}^{2}$ at 700 nm. The ESA spectrum was measured from 600 to 880 nm and is used to construct an energy-level diagram for the ${\mathrm{Ce}}^{3+}$ ions relative to the energy-band states of the ${\mathrm{Y}}_{3}$${\mathrm{Al}}_{5}$${\mathrm{O}}_{12}$ host. The energy gap between the lowest relaxed 5d state and the conduction-band edge is estimated to be 10 000 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$. Strong-probe saturation measurements indicate a slow and inefficient back-transfer of excitation to the cerium ions following the ESA. Photoconductivity measurements were used to confirm the two-step photoionization of the cerium ions.

DOI
10.1103/physrevb.39.8807

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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
The optical transitions in Ce3+{\mathrm{Ce}}^{3+}Ce3+:{\mathrm{Y}}_{3}$${\mathrm{Al}}_{5}$${\mathrm{O}}_{12} from the lowest 5d excited state of the Ce3+{\mathrm{Ce}}^{3+}Ce3+ ion to the host conduction band have been investigated. Two spatially overlapped and time-sequenced laser pulses were used to observe directly the excited-state absorption (ESA) and the two-step photoionization of the cerium ions. The peak cross section of the ESA transition is (1.0\ifmmode\pm\else\textpm\fi{}0.3)\ifmmode\times\else\texttimes\fi{}10\ensuremath−17{10}^{\mathrm{\ensuremath{-}}17}10\ensuremath−17 cm2{\mathrm{cm}}^{2}cm2 at 700 nm. The ESA spectrum was measured from 600 to 880 nm and is used to construct an energy-level diagram for the Ce3+{\mathrm{Ce}}^{3+}Ce3+ ions relative to the energy-band states of the {\mathrm{Y}}_{3}$${\mathrm{Al}}_{5}$${\mathrm{O}}_{12} host. The energy gap between the lowest relaxed 5d state and the conduction-band edge is estimated to be 10 000 cm\ensuremath−1{\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}cm\ensuremath−1. Strong-probe saturation measurements indicate a slow and inefficient back-transfer of excitation to the cerium ions following the ESA. Photoconductivity measurements were used to confirm the two-step photoionization of the cerium ions.
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Broad bandwidth 5d→4f transitions in Ce3+ have been considered for tunable laser action. In this letter, optical probe measurements of excited Ce3+ ions in Y3Al5O12 show that stimulated emission in the 550–610-nm region is not possible at 295 K because of excited-state absorption. Transient measurements demonstrate that part of this loss has ≈75-ns lifetime and is associated with absorption from the lowest 5d level; a longer-lifetime loss is also observed. The excited-state-absorption loss is reduced at lower temperatures.
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An experimental study of saturable absorption and excited-state absorption (ESA) in several inorganic saturable absorbers, Cr/sup 4+/:YAG, Cr/sup 4+/:GGG, and Cr/sup 4+/:YSGG, is presented. We provide the theoretical background of absorption characteristics in saturable absorbers that exhibit ESA, with some new results: approximate analytical solutions are proposed for the optical transmission in the case of a slow absorber, and for various light intensity conditions of spatially or temporally Gaussian beams in fast and slow absorbers. Experimentally, partial bleaching of the first excited state itself could be observed in Cr/sup 4+/:YAG at /spl lambda/=1064 nm, yielding the higher excited-state lifetime as /spl tau/*=(0.55/spl plusmn/0.1) ns. The regular transmission bleaching curve was measured in Cr/sup 4+/:GGG, for the first time in this material, yielding /spl sigma//sub ga/=(58/spl plusmn/5)/spl times/10/sup -1/ cm/sup 2/, and /spl sigma/e/sub s/=(13/spl plusmn/2)/spl times/10/sup -19/ cm/sup 2/ at /spl lambda/=1064 nm, ESA spectra were measured for the three materials between /spl sim/700 and 900 nm. All three exhibit crossing between saturable absorption at longer wavelengths and inverse saturable absorption at shorter wavelengths.
The spectral dependence of the photoionization energy of Eu2+:CaF2, Ce3+:YAG, and Sm2+:CaF2 systems have been measured and thresholds experimentally determined and compared with theoretical values calculated from electrostatic models. It is shown that the excited state absorption transitions or the persistent hole burning observed by other authors occur above the threshold energy of photoionization of the impurities and that the states of the crystal which form the bottom of the conduction band may play an important role in the strong probability of these processes. A review of thresholds now known is also given.
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.