Journal of the Optical Society of America B

Interconfigurational two-photon transitions in Nd^3+:Y_3Al_5O_12

Swapan Kumar Gayen, Bin Qing Xie

Published Jun 1, 1993• 8 citations

Abstract

Resonantly enhanced, near-ultraviolet 4f3 → 4f25d two-photon transitions have been observed in trivalent neodymium-doped yttrium aluminum garnet (Nd3+:Y3Al5O12). The two-photon excitation spectra over the 40 400–46 730 cm−1 transition energy range are characterized by sharp resonance peaks on a slowly varying background caused by nonresonant transitions. The peak two-photon cross section involving the 2P1/2 resonant intermediate state is 9 × 10−51 cm4 s, and the integrated cross section is 2.2 × 10−38 cm4.

DOI: 10.1364/josab.10.000993

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Journal of the Optical Society of America B

Interconfigurational two-photon transitions in Nd^3+:Y_3Al_5O_12

Swapan Kumar Gayen, Bin Qing Xie

Published Jun 1, 1993• 8 citations

Publisher

Abstract

DOI: 10.1364/josab.10.000993

Related papers

Resonant enhancement of two-photon transitions to the second excited 4f5dstate in Pr3+ : Y3 Al5 O12

Bin Qing Xie, Y. M. Cheung, Swapan Kumar Gayen

The two-photon absorption cross section for transitions from the $^{3}$ ${\mathit{H}}_{4}$ ground-state manifold to the second excited state of the 4f5d configuration of ${\mathrm{Pr}}^{3+}$ in ${\mathrm{Y}}_{3}$ ${\mathrm{Al}}_{5}$ ${\mathrm{O}}_{12}$ is observed to be enhanced by about two orders of magnitude when the excitation frequency happens to be resonant with the $^{3}$ ${\mathit{P}}_{\mathit{J}}$ (J=0,1,2) and $^{1}$ ${\mathit{I}}_{6}$ intermediate states of the 4 ${\mathit{f}}^{2}$ configuration. The structure and line shape of the two-photon excitation spectrum spanning the 39 600--46 950 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ transition-energy range are entirely dominated by these resonantly enhanced transitions, while the contributions from nonresonant transitions appear as a slowly varying background beneath the strong resonance peaks. A two-photon absorption cross section as high as 4\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}50}$ ${\mathrm{cm}}^{4}$ s is measured at the peak of the resonantly enhanced transition at 44 246 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$, which involves a level of the $^{3}$ ${\mathit{P}}_{2}$ manifold as the intermediate state. The spectrally integrated cross section over that manifold is 3.3\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}38}$ ${\mathrm{cm}}^{4}$ .The two-photon absorption cross section for transitions from the $^{3}$${\mathit{H}}_{4}$ ground-state manifold to the second excited state of the 4f5d configuration of ${\mathrm{Pr}}^{3+}$ in ${\mathrm{Y}}_{3}$${\mathrm{Al}}_{5}$${\mathrm{O}}_{12}$ is observed to be enhanced by about two orders of magnitude when the excitation frequency happens to be resonant with the $^{3}$${\mathit{P}}_{\mathit{J}}$ (J=0,1,2) and $^{1}$${\mathit{I}}_{6}$ intermediate states of the 4${\mathit{f}}^{2}$ configuration. The structure and line shape of the two-photon excitation spectrum spanning the 39 600--46 950 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ transition-energy range are entirely dominated by these resonantly enhanced transitions, while the contributions from nonresonant transitions appear as a slowly varying background beneath the strong resonance peaks. A two-photon absorption cross section as high as 4\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}50}$ ${\mathrm{cm}}^{4}$ s is measured at the peak of the resonantly enhanced transition at 44 246 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$, which involves a level of the $^{3}$${\mathit{P}}_{2}$ manifold as the intermediate state. The spectrally integrated cross section over that manifold is 3.3\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}38}$ ${\mathrm{cm}}^{4}$.

Physical review. B, Condensed matterMar 1, 19939 citations

Spectroscopy of Y3 Al5 O12 : Nd3+ under high-power, picosecond-pulse excitation

George E. Venikouas, Greg Quarles, John P. King +1 more

High-power, picosecond-pulse excitation was used to study the dynamics of the pumping and decay processes in ${\mathrm{Y}}_{3}$ ${\mathrm{Al}}_{5}$ ${\mathrm{O}}_{12}$ : ${\mathrm{Nd}}^{3+}$ . The observed fluorescence spectral lines are assigned to transitions from three different metastable states excited by both single-photon and two-photon absorption. The branching ratios, lifetimes, and quantum efficiencies of the metastable states are obtained from the data as well as the two-photon absorption cross sections. The results provide useful information concerning ultraviolet pumping efficiencies of the Nd-YAG (Nd-doped yttrium aluminum garnet) laser transition and the $5d\ensuremath{-}4f$ nonradiative decay rate for this material. In addition, the time-resolved spectroscopy method employed here is shown to be an extremely sensitive technique for obtaining two-photon absorption cross sections.High-power, picosecond-pulse excitation was used to study the dynamics of the pumping and decay processes in ${\mathrm{Y}}_{3}$${\mathrm{Al}}_{5}$${\mathrm{O}}_{12}$:${\mathrm{Nd}}^{3+}$. The observed fluorescence spectral lines are assigned to transitions from three different metastable states excited by both single-photon and two-photon absorption. The branching ratios, lifetimes, and quantum efficiencies of the metastable states are obtained from the data as well as the two-photon absorption cross sections. The results provide useful information concerning ultraviolet pumping efficiencies of the Nd-YAG (Nd-doped yttrium aluminum garnet) laser transition and the $5d\ensuremath{-}4f$ nonradiative decay rate for this material. In addition, the time-resolved spectroscopy method employed here is shown to be an extremely sensitive technique for obtaining two-photon absorption cross sections.

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Zhenwen Dai, Jing‐yao Liu, Siyuan Zhang

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Measurement of the Laser Transition Cross Section for Nd+3 in Yttrium Aluminum Garnet

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This paper reports measurements of the room-temperature laser transition cross section of ${\mathrm{Nd}}^{+3}$ in yttrium aluminum garnet at 1.06 \ensuremath{\mu}. One method used is based on the measured upper-state lifetime and a determination of the fluorescence branching ratio for this state. The value thus determined is 3.5\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}19}$ ${\mathrm{cm}}^{2}$ . The second method involves measurement of the ratio of fluorescent intensities from the upper laser level to the ground state and to the lower laser level, and measurement of the cross section in absorption of the transition which involves the ground state. The second method yields a value of 2.7\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}19}$ ${\mathrm{cm}}^{2}$ . The difference represents the contribution of fluorescence to high-lying levels (not included in the determination of branching ratio) and nonradiative transitions. The probable experimental accuracy in both methods is \ifmmode\pm\else\textpm\fi{}15%.This paper reports measurements of the room-temperature laser transition cross section of ${\mathrm{Nd}}^{+3}$ in yttrium aluminum garnet at 1.06 \ensuremath{\mu}. One method used is based on the measured upper-state lifetime and a determination of the fluorescence branching ratio for this state. The value thus determined is 3.5\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}19}$ ${\mathrm{cm}}^{2}$. The second method involves measurement of the ratio of fluorescent intensities from the upper laser level to the ground state and to the lower laser level, and measurement of the cross section in absorption of the transition which involves the ground state. The second method yields a value of 2.7\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}19}$ ${\mathrm{cm}}^{2}$. The difference represents the contribution of fluorescence to high-lying levels (not included in the determination of branching ratio) and nonradiative transitions. The probable experimental accuracy in both methods is \ifmmode\pm\else\textpm\fi{}15%.

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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 +1 more

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.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.

Applied Physics LettersJul 18, 20117 citations

Orientation of Nd3+ dipoles in yttrium aluminum garnet: Experiment and model

Sylvain Schwartz, Gilles A. Feugnet, Maxence Rebut +2 more

We report an experimental study of the $1.064\text{ }\ensuremath{\mu}\text{m}$ transition dipoles in neodymium-doped yttrium aluminum garnet (Nd:YAG) by measuring the coupling constant between two orthogonal modes of a laser cavity for different cuts of the YAG gain crystal. We propose a theoretical model in which the transition dipoles, slightly elliptic, are oriented along the crystallographic axes. Our experimental measurements show a very good quantitative agreement with this model and predict a dipole ellipticity between 2% and 3%. This work provides an experimental evidence for the simple description in which transition dipoles and crystallographic axes are collinear in Nd:YAG (with an accuracy better than $1\ifmmode^\circ\else\textdegree\fi{}$), a point that has been discussed for years.We report an experimental study of the $1.064\text{ }\ensuremath{\mu}\text{m}$ transition dipoles in neodymium-doped yttrium aluminum garnet (Nd:YAG) by measuring the coupling constant between two orthogonal modes of a laser cavity for different cuts of the YAG gain crystal. We propose a theoretical model in which the transition dipoles, slightly elliptic, are oriented along the crystallographic axes. Our experimental measurements show a very good quantitative agreement with this model and predict a dipole ellipticity between 2% and 3%. This work provides an experimental evidence for the simple description in which transition dipoles and crystallographic axes are collinear in Nd:YAG (with an accuracy better than $1\ifmmode^\circ\else\textdegree\fi{}$), a point that has been discussed for years.

arXiv:0905.3125Physical Review AJun 9, 200913 citations

The two-photon absorption cross section for transitions from the

^{3}

{\mathit{H}}_{4}

ground-state manifold to the second excited state of the 4f5d configuration of

{\mathrm{Pr}}^{3+}

{\mathrm{Y}}_{3}

{\mathrm{Al}}_{5}

{\mathrm{O}}_{12}

is observed to be enhanced by about two orders of magnitude when the excitation frequency happens to be resonant with the

^{3}

{\mathit{P}}_{\mathit{J}}

(J=0,1,2) and

^{1}

{\mathit{I}}_{6}

intermediate states of the 4

{\mathit{f}}^{2}

configuration. The structure and line shape of the two-photon excitation spectrum spanning the 39 600--46 950 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ transition-energy range are entirely dominated by these resonantly enhanced transitions, while the contributions from nonresonant transitions appear as a slowly varying background beneath the strong resonance peaks. A two-photon absorption cross section as high as 4\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}50}$

{\mathrm{cm}}^{4}

s is measured at the peak of the resonantly enhanced transition at 44 246 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$, which involves a level of the

^{3}

{\mathit{P}}_{2}

manifold as the intermediate state. The spectrally integrated cross section over that manifold is 3.3\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}38}$

{\mathrm{cm}}^{4}

High-power, picosecond-pulse excitation was used to study the dynamics of the pumping and decay processes in

{\mathrm{Y}}_{3}

{\mathrm{Al}}_{5}

{\mathrm{O}}_{12}

{\mathrm{Nd}}^{3+}

. The observed fluorescence spectral lines are assigned to transitions from three different metastable states excited by both single-photon and two-photon absorption. The branching ratios, lifetimes, and quantum efficiencies of the metastable states are obtained from the data as well as the two-photon absorption cross sections. The results provide useful information concerning ultraviolet pumping efficiencies of the Nd-YAG (Nd-doped yttrium aluminum garnet) laser transition and the $5d\ensuremath{-}4f$ nonradiative decay rate for this material. In addition, the time-resolved spectroscopy method employed here is shown to be an extremely sensitive technique for obtaining two-photon absorption cross sections.

This paper reports measurements of the room-temperature laser transition cross section of

{\mathrm{Nd}}^{+3}

in yttrium aluminum garnet at 1.06 \ensuremath{\mu}. One method used is based on the measured upper-state lifetime and a determination of the fluorescence branching ratio for this state. The value thus determined is 3.5\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}19}$

{\mathrm{cm}}^{2}

. The second method involves measurement of the ratio of fluorescent intensities from the upper laser level to the ground state and to the lower laser level, and measurement of the cross section in absorption of the transition which involves the ground state. The second method yields a value of 2.7\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}19}$

{\mathrm{cm}}^{2}

. The difference represents the contribution of fluorescence to high-lying levels (not included in the determination of branching ratio) and nonradiative transitions. The probable experimental accuracy in both methods is \ifmmode\pm\else\textpm\fi{}15%.