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Physical review. B, Condensed matter

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

George E. Venikouas, Greg Quarles, John P. King, Richard C. Powell

Published Sep 1, 1984• 31 citations
Publisher

Abstract

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.

DOI
10.1103/physrevb.30.2401

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Excited-state absorption in Pr3+ : Y3 Al5 O12

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The optical-absorption transitions originating from the lowest 4f5d excited state of ${\mathrm{Pr}}^{3+}$ in ${\mathrm{Y}}_{3}$${\mathrm{Al}}_{5}$${\mathrm{O}}_{12}$ have been studied. The experimental arrangement uses a 7-ns 266-nm light pulse to populate the lowest 4f5d state, and a spatially overlapped, time-sequenced pulse from a frequency-tunable dye laser to induce transitions from that excited state. The excited-state-absorption (ESA) spectrum covering the 900--300-nm probe wavelength range is characterized by two broad peaks centered at 700 and 350 nm on a slowly rising background. The peak ESA cross section at 355 nm is (1\ifmmode\pm\else\textpm\fi{}0.1)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}17}$ ${\mathrm{cm}}^{2}$. The position, shape, and strength of the spectrum suggest that the terminal states of the ESA transitions are the second 4f5d state of ${\mathrm{Pr}}^{3+}$ and the conduction band of the host lattice. The ESA measurements have been extended to transitions from the $^{3}$${\mathit{P}}_{0}$ and $^{1}$${\mathit{D}}_{2}$ excited states of the 4${\mathit{f}}^{2}$ configuration of ${\mathrm{Pr}}^{3+}$ as well. The ESA cross sections at a probe wavelength of 532 nm are (8\ifmmode\pm\else\textpm\fi{}1)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}19}$ ${\mathrm{cm}}^{2}$ and (5.7\ifmmode\pm\else\textpm\fi{}0.6)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}19}$ ${\mathrm{cm}}^{2}$ for transitions from the $^{3}$${\mathit{P}}_{0}$ and $^{1}$${\mathit{D}}_{2}$ excited states, respectively. The terminal state of ESA transitions from these two levels is the lowest 4f5d state. The strong ESA completely inhibits the potential laser action based on emission from these states in this crystal.

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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.

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Optical spectroscopy and decoherence studies of Yb3+ :YAG at 968 nm

Thomas Böttger, Charles W. Thiel, R. L. Cone +2 more

The $^{2}F_{7/2}\ensuremath{\leftrightarrow}^{2}F_{5/2}$ optical transitions of $\mathrm{Y}{\mathrm{b}}^{3+}$ doped into ${\mathrm{Y}}_{3}\mathrm{A}{\mathrm{l}}_{5}{\mathrm{O}}_{12}$ (YAG) were studied for potential quantum information and photonic signal processing applications. Absorption and fluorescence spectroscopy located the energy levels of the ground $^{2}F_{7/2}$ and excited $^{2}F_{5/2}$ manifolds, allowing inconsistencies between previous assignments of crystal field splittings in the literature to be resolved. These measurements reveal an unusually large splitting between the first and second levels in both the ground and excited multiplets, potentially providing for reduced sensitivity to thermally induced decoherence and spin-lattice relaxation. Spectral hole burning through two-level saturation was observed, determining the excited state lifetime to be 860 \ensuremath{\mu}s and resolving ambiguities in previous fluorescence measurements that were caused by the large radiation trapping effects in this material. Optical decoherence measurements using two-pulse photon echoes gave a homogeneous linewidth of 18 kHz for an applied magnetic field of 1 T, narrowing to 5 kHz at 2.5 T. The observed decoherence was described by spectral diffusion attributed to $\mathrm{Y}{\mathrm{b}}^{3+}\mathrm{\ensuremath{-}}\mathrm{Y}{\mathrm{b}}^{3+}$ magnetic dipole interactions. Laser absorption determined an inhomogeneous linewidth of 3.6 GHz for this transition in this 0.05%-doped crystal, which is narrower than for any other rare-earth-ion transition previously studied in the YAG host. The temperature dependence of the transition energy and linewidth of the lowest $^{2}F_{7/2}$ to lowest $^{2}F_{5/2}$ transition centered at 968.571 nm measured from 4 K to 300 K was well described by phonon scattering at higher temperatures, with an additional anomalous linear temperature-dependent broadening at temperatures below 80 K. Two magnetically inequivalent subgroups of $\mathrm{Y}{\mathrm{b}}^{3+}$ ions were identified when a magnetic field was applied along the $\ensuremath{\langle}111\ensuremath{\rangle}$ axis, as expected for the ${D}_{2}$ sites in the cubic symmetry crystal, with ground and excited state effective $g$-values of ${g}_{\mathrm{g}}=3.40$ (3.34) and ${g}_{\mathrm{e}}=1.04$ (2.01), respectively. Together with the convenient diode laser wavelength of this transition, our study suggests that $\mathrm{Y}{\mathrm{b}}^{3+}$:YAG is a promising material system for spectral hole burning and quantum information applications.

Physical review. B./Physical review. B•Jul 26, 2016•28 citations
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}:Nd3+{\mathrm{Nd}}^{3+}Nd3+. 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−4f5d\ensuremath{-}4f5d\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 Nd+3{\mathrm{Nd}}^{+3}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{}${10}^{\ensuremath{-}19}$ cm2{\mathrm{cm}}^{2}cm2. 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{}${10}^{\ensuremath{-}19}$ cm2{\mathrm{cm}}^{2}cm2. 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%.
The two-photon absorption cross section for transitions from the 3^{3}3H4{\mathit{H}}_{4}H4​ ground-state manifold to the second excited state of the 4f5d configuration of Pr3+{\mathrm{Pr}}^{3+}Pr3+ in Y3{\mathrm{Y}}_{3}Y3​Al5{\mathrm{Al}}_{5}Al5​O12{\mathrm{O}}_{12}O12​ is observed to be enhanced by about two orders of magnitude when the excitation frequency happens to be resonant with the 3^{3}3PJ{\mathit{P}}_{\mathit{J}}PJ​ (J=0,1,2) and 1^{1}1I6{\mathit{I}}_{6}I6​ intermediate states of the 4f2{\mathit{f}}^{2}f2 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{}${10}^{\mathrm{\ensuremath{-}}50}$ cm4{\mathrm{cm}}^{4}cm4 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^{3}3P2{\mathit{P}}_{2}P2​ manifold as the intermediate state. The spectrally integrated cross section over that manifold is 3.3\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}38}$ cm4{\mathrm{cm}}^{4}cm4.
The optical-absorption transitions originating from the lowest 4f5d excited state of Pr3+{\mathrm{Pr}}^{3+}Pr3+ in Y3{\mathrm{Y}}_{3}Y3​Al5{\mathrm{Al}}_{5}Al5​O12{\mathrm{O}}_{12}O12​ have been studied. The experimental arrangement uses a 7-ns 266-nm light pulse to populate the lowest 4f5d state, and a spatially overlapped, time-sequenced pulse from a frequency-tunable dye laser to induce transitions from that excited state. The excited-state-absorption (ESA) spectrum covering the 900--300-nm probe wavelength range is characterized by two broad peaks centered at 700 and 350 nm on a slowly rising background. The peak ESA cross section at 355 nm is (1\ifmmode\pm\else\textpm\fi{}0.1)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}17}$ cm2{\mathrm{cm}}^{2}cm2. The position, shape, and strength of the spectrum suggest that the terminal states of the ESA transitions are the second 4f5d state of Pr3+{\mathrm{Pr}}^{3+}Pr3+ and the conduction band of the host lattice. The ESA measurements have been extended to transitions from the 3^{3}3P0{\mathit{P}}_{0}P0​ and 1^{1}1D2{\mathit{D}}_{2}D2​ excited states of the 4f2{\mathit{f}}^{2}f2 configuration of Pr3+{\mathrm{Pr}}^{3+}Pr3+ as well. The ESA cross sections at a probe wavelength of 532 nm are (8\ifmmode\pm\else\textpm\fi{}1)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}19}$ cm2{\mathrm{cm}}^{2}cm2 and (5.7\ifmmode\pm\else\textpm\fi{}0.6)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}19}$ cm2{\mathrm{cm}}^{2}cm2 for transitions from the 3^{3}3P0{\mathit{P}}_{0}P0​ and 1^{1}1D2{\mathit{D}}_{2}D2​ excited states, respectively. The terminal state of ESA transitions from these two levels is the lowest 4f5d state. The strong ESA completely inhibits the potential laser action based on emission from these states in this crystal.
Yttrium Aluminum Garnet (YAG, Y_3 〖Al〗_5 O_12) crystals doped with Erbium have posed an interesting position in the field of rare earth solid state lasers as they possess the property of self-saturation, in which the upper energy level in a laser has a much shorter lifetime than that of the lower level. This is the case of the 2.94μm transition in Er:YAG. That property at first seems to make this material unfit for use as a laser gain medium, however further research into these classes of rare earth materials revealed interesting non-liner energy transfer mechanisms that allow it to be a useful mid wave infra-red (MWIR) coherent source in the continuous wave (CW) and pulsed regimes. This came to fruition due to decades of modeling and spectroscopic research investigating the non-linear energy transfer mechanisms of excited state absorption (ESA), energy transfer up-conversion (ETU), and cross relaxation (XR). These effects show up in the rise and fall times of the levels observed through fluorescence. Resulting in the non-exponential rise and fall characteristics and having a squared or even cubed relation to the population. The population evolution for each of the lasing levels is now affected by ions recycling energy and in turn cause the lifetimes of the levels to “effectively” change to a point where simple linear models do not adequately describe the system and its performance. The non-linear energy transfer dynamics of Er:YAG are modeled under high resonant pump conditions. By pumping with selective resonant pumps, the interaction dynamics of the (_ ^4)I_(11/2) and the (_ ^4)I_(13/2) levels in the Erbium ion reveal the contributions from generally ignored non-linear energy transfer mechanisms. Specifically, the multi-photon effect known as excited state absorption (ESA) is modeled by measuring and characterizing the cross section in single crystal Er:YAG samples utilizing a pump and probe technique coupled with transient fluorescence measurements. The measured ESA cross section is then included in the rate equation modeling.
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.
The $^{2}F_{7/2}\ensuremath{\leftrightarrow}^{2}F_{5/2}$ optical transitions of Yb3+\mathrm{Y}{\mathrm{b}}^{3+}Yb3+ doped into Y3Al5O12{\mathrm{Y}}_{3}\mathrm{A}{\mathrm{l}}_{5}{\mathrm{O}}_{12}Y3​Al5​O12​ (YAG) were studied for potential quantum information and photonic signal processing applications. Absorption and fluorescence spectroscopy located the energy levels of the ground 2F7/2^{2}F_{7/2}2F7/2​ and excited 2F5/2^{2}F_{5/2}2F5/2​ manifolds, allowing inconsistencies between previous assignments of crystal field splittings in the literature to be resolved. These measurements reveal an unusually large splitting between the first and second levels in both the ground and excited multiplets, potentially providing for reduced sensitivity to thermally induced decoherence and spin-lattice relaxation. Spectral hole burning through two-level saturation was observed, determining the excited state lifetime to be 860 \ensuremath{\mu}s and resolving ambiguities in previous fluorescence measurements that were caused by the large radiation trapping effects in this material. Optical decoherence measurements using two-pulse photon echoes gave a homogeneous linewidth of 18 kHz for an applied magnetic field of 1 T, narrowing to 5 kHz at 2.5 T. The observed decoherence was described by spectral diffusion attributed to $\mathrm{Y}{\mathrm{b}}^{3+}\mathrm{\ensuremath{-}}\mathrm{Y}{\mathrm{b}}^{3+}$ magnetic dipole interactions. Laser absorption determined an inhomogeneous linewidth of 3.6 GHz for this transition in this 0.05%-doped crystal, which is narrower than for any other rare-earth-ion transition previously studied in the YAG host. The temperature dependence of the transition energy and linewidth of the lowest 2F7/2^{2}F_{7/2}2F7/2​ to lowest 2F5/2^{2}F_{5/2}2F5/2​ transition centered at 968.571 nm measured from 4 K to 300 K was well described by phonon scattering at higher temperatures, with an additional anomalous linear temperature-dependent broadening at temperatures below 80 K. Two magnetically inequivalent subgroups of Yb3+\mathrm{Y}{\mathrm{b}}^{3+}Yb3+ ions were identified when a magnetic field was applied along the $\ensuremath{\langle}111\ensuremath{\rangle}$ axis, as expected for the D2{D}_{2}D2​ sites in the cubic symmetry crystal, with ground and excited state effective ggg-values of gg=3.40{g}_{\mathrm{g}}=3.40gg​=3.40 (3.34) and ge=1.04{g}_{\mathrm{e}}=1.04ge​=1.04 (2.01), respectively. Together with the convenient diode laser wavelength of this transition, our study suggests that Yb3+\mathrm{Y}{\mathrm{b}}^{3+}Yb3+:YAG is a promising material system for spectral hole burning and quantum information applications.