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Optics Letters

Photon-gated photoconductivity of Pr^3+:YAG

G. Wittmann, R. M. Macfarlane

Published Mar 15, 1996• 20 citations
Publisher

Abstract

We have observed photon-gated photoconductivity in Pr:YAG, providing clear evidence for photoionization of the trivalent praseodymium ion in the solid state. Photoionization occurs by two-step absorption from (3)H(4)(1) ? (1)D(2)(1) followed by an excited-state absorption from (1)D(2) to the lowest component of the 4f5d configuration. The excitation spectrum of the photocurrent shows sharp (1)D(2) spectral features, providing unambiguous assignment of the photocurrent.

DOI
10.1364/ol.21.000426

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Journal of the Optical Society of America B•Dec 1, 1999•54 citations
We have observed photon-gated photoconductivity in Pr:YAG, providing clear evidence for photoionization of the trivalent praseodymium ion in the solid state. Photoionization occurs by two-step absorption from (3)H(4)(1) ? (1)D(2)(1) followed by an excited-state absorption from (1)D(2) to the lowest component of the 4f5d configuration. The excitation spectrum of the photocurrent shows sharp (1)D(2) spectral features, providing unambiguous assignment of the photocurrent.
We have observed photon-gated spectral hole burning, i.e., hole burning that occurs only in the presence of an additional gating-light source. Gating enhancement factors of 10(4) were observed. In BaClF:Sm(2+) this involves two step photoionization of Sm(2+) and leads to persistent holes in the (4)F(0) --> (5)D(0) (687.9-nm) and (7)F(0) --> (5)D(1) (629.7-nm) absorption lines. The hole widths of 25 MHz at 2 K are much narrower than the inhomogeneous broadening of 16 GHz. The action spectrum of the gating shows a threshold behavior around 2.5 eV. Erasing studies show that Sm(3)+ acts as a trap for the released electrons. A remarkable and novel feature is that the holes can be recovered after temperature cycling to 300 K.
The hyperfine splitting of the ground state and the lowest electronic component of the (1)D(2) excited state have been measured for Pr(3+) in YAG. We show that a particularly simple and powerful technique is the production of sublevel coherence by short-pulse (impact) excitation, which is detected by coherent forward scattering of a weak probe beam and Fourier transformation of the resulting quantum-beat signal. This yielded excited-state splittings of 6.49 and 8.29 MHz. The ground state shows large pseudoquadrupole splittings of 33.4 and 41.6 MHz, which were obtained by optically detected nuclear quadrupole resonance.
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.
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.