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Physical review. B, Condensed matter

Vacuum-ultraviolet spectroscopy and quantum cutting for Gd3+ in LiYF4

R. T. Wegh, Harry Donker, Andries Meijerink, Ralf-Johan Lamminmäki, Jorma P. Holsa

Published Dec 1, 1997• 280 citations

Abstract

A systematic spectroscopic study of the ${4f}^{7}$ energy levels of ${\mathrm{Gd}}^{3+}$ in ${\mathrm{LiYF}}_{4}$ in the vacuum-ultraviolet spectral region $(50000--70000{\mathrm{cm}}^{\mathrm{\ensuremath{-}}1})$ is reported. Using energy-level calculations, all observed spectral lines could be assigned to free-ion term symbols (including term symbols with unusually high $L$ and $J,$ e.g., a ${}^{2}{Q}_{23/2}$ level around $67000{\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$). From the ${}^{6}{G}_{J}$ levels around $50000{\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ quantum cutting (or two-photon luminescence, photon-cascade emission) is observed: the emission of a red photon due to the ${}^{6}{G}_{J}{\ensuremath{\rightarrow}}^{6}{P}_{J}$ transition is followed by the emission of an ultraviolet photon due to the ${}^{6}{P}_{J}{\ensuremath{\rightarrow}}^{8}{S}_{7/2}$ transition.

DOI: 10.1103/physrevb.56.13841

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A systematic spectroscopic study of the

{4f}^{7}

energy levels of

{\mathrm{Gd}}^{3+}

in

{\mathrm{LiYF}}_{4}

in the vacuum-ultraviolet spectral region

(50000--70000{\mathrm{cm}}^{\mathrm{\ensuremath{-}}1})

is reported. Using energy-level calculations, all observed spectral lines could be assigned to free-ion term symbols (including term symbols with unusually high

L

and

J,

e.g., a

{}^{2}{Q}_{23/2}

level around

67000{\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}

). From the

{}^{6}{G}_{J}

levels around

50000{\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}

quantum cutting (or two-photon luminescence, photon-cascade emission) is observed: the emission of a red photon due to the

{}^{6}{G}_{J}{\ensuremath{\rightarrow}}^{6}{P}_{J}

transition is followed by the emission of an ultraviolet photon due to the

{}^{6}{P}_{J}{\ensuremath{\rightarrow}}^{8}{S}_{7/2}

transition.

The energy levels of lanthanide ions have been studied in great detail in the energy range up to $40\phantom{\rule{0.2em}{0ex}}000\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$

(250\phantom{\rule{0.3em}{0ex}}\mathrm{nm})

. Recently an increased interest in the high energy levels between 40 000 and $70\phantom{\rule{0.2em}{0ex}}000\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$ has emerged, partly triggered by the need for new luminescent materials for vacuum ultraviolet (VUV) excitation. Using synchrotron radiation many new energy levels have been discovered for various lanthanide ions. However, the spectral resolution of a synchrotron is limited and to resolve the complete energy level structure higher resolution tunable lasers are required. Unfortunately no high-resolution tunable lasers are available in the VUV. To overcome this problem two-photon spectroscopy may be applied. In this paper resonant two-photon spectroscopy is applied to measure the energy level structure of

{\mathrm{Gd}}^{3+}

in fluorides. Excited state excitation (ESE) from the

^{6}P_{7∕2}

level is shown to provide high-resolution spectra of the high energy levels of

{\mathrm{Gd}}^{3+}

. The extension of the energy level structure is used to improve energy level calculations, which is especially beneficial for

{\mathrm{Gd}}^{3+}

where only a limited number of energy levels is available from conventional laser spectroscopy.

Intraconfiguration ${4f}^{7}\ensuremath{\rightarrow}{4f}^{7}$ transitions of

{\mathrm{Eu}}^{2+}

in

{\mathrm{KMgF}}_{3}

have been investigated by two-photon excitation (TPE) spectroscopy at 10 K. Emission bands due to the ${}^{6}{\stackrel{\ensuremath{\rightarrow}}{{P}_{7/2}}}^{8}{S}_{7/2}$ and ${}^{6}{\stackrel{\ensuremath{\rightarrow}}{{I}_{7/2}}}^{8}{S}_{7/2}$ transitions are obtained by two-photon excitation into the

{}^{6}{I}_{J}

(J=7/2,9/2,17/2,11/2,15/2,13/2)

and

{}^{6}{D}_{J}

(J=1/2,7/2,3/2,5/2)

states. The TPE spectrum of the ${}^{6}{\stackrel{\ensuremath{\rightarrow}}{{I}_{7/2}}}^{8}{S}_{7/2}$ emission is observed to be different from that of the ${}^{6}{\stackrel{\ensuremath{\rightarrow}}{{P}_{7/2}}}^{8}{S}_{7/2}$ emission. This is explained by the relative positions of the lowest crystal-field component of the

{}^{6}{I}_{7/2}

level and the lowest level of the

{4f}^{6}5d

configuration for cubic-site and non-cubic-site

{\mathrm{Eu}}^{2+}

ions. The observed TPE spectra are satisfactorily interpreted by a suggestion that the ${}^{6}{\stackrel{\ensuremath{\rightarrow}}{{I}_{7/2}}}^{8}{S}_{7/2}$ emission is produced by only cubic-site

{\mathrm{Eu}}^{2+},

while the ${}^{6}{\stackrel{\ensuremath{\rightarrow}}{{P}_{7/2}}}^{8}{S}_{7/2}$ emission is produced by both cubic-site

{\mathrm{Eu}}^{2+}

and non-cubic-site

{\mathrm{Eu}}^{2+}.