Physical Review Letters

Resonant Fluorescence Line Narrowing in La1−xP5O14:Ndx3+

Matthijs M. Broer, David L. Huber, William M. Yen, Walter K. Zwicker

Published Aug 9, 1982• 53 citations

Abstract

Donor-donor and donor-acceptor dynamics in ${\mathrm{La}}_{1\ensuremath{-}x}{\mathrm{P}}_{5}{\mathrm{O}}_{14}:{{\mathrm{Nd}}_{x}}^{3+}$ are measured directly with a high-resolution, near-ir laser system. Time-resolved fluorescence line-narrowing measurements show an absence of rapid donor-donor transfer below 20 K and an onset of spectral diffusion at \ensuremath{\approx} 20 K for an $x=0.75$ sample. The linear concentration quenching and exponential decay in the absence of fast diffusion are explained with existing energy-transfer theories and are consistent with room-temperature studies.

DOI: 10.1103/physrevlett.49.394

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Physical Review Letters

Resonant Fluorescence Line Narrowing in La1−xP5O14:Ndx3+

Matthijs M. Broer, David L. Huber, William M. Yen, Walter K. Zwicker

Published Aug 9, 1982• 53 citations

Publisher

Abstract

Donor-donor and donor-acceptor dynamics in

{\mathrm{La}}_{1\ensuremath{-}x}{\mathrm{P}}_{5}{\mathrm{O}}_{14}:{{\mathrm{Nd}}_{x}}^{3+}

are measured directly with a high-resolution, near-ir laser system. Time-resolved fluorescence line-narrowing measurements show an absence of rapid donor-donor transfer below 20 K and an onset of spectral diffusion at \ensuremath{\approx} 20 K for an

x=0.75

sample. The linear concentration quenching and exponential decay in the absence of fast diffusion are explained with existing energy-transfer theories and are consistent with room-temperature studies.

DOI: 10.1103/physrevlett.49.394

Related papers

Trapping of optical excitation by two types of acceptors in La0.72 Pr0.25 Nd0.03 F3

Thomas J. Glynn, I. Laulicht, Liren Lou +2 more

We have investigated the process of quenching of fluorescence from the $^{3}P_{0}$ state of ${\mathrm{Pr}}^{3+}$ in ${\mathrm{La}}_{0.72}$ ${\mathrm{Pr}}_{0.25}$ ${\mathrm{Nd}}_{0.03}$ ${\mathrm{F}}_{3}$ due to cross relaxation to Pr and Nd ions. The fluorescence decay of the ensemble of Pr ions after pulsed excitation is measured as a function of temperature in the (2-70)-K region. Cross relaxation occurs either directly or through a donor-donor transfer within the inhom-geneous line. Knowledge of the dynamics occurring within the inhomogeneous line derived from previous fluorescence line-narrowing experiments is used to analyze the cross-relaxation process from a microscopic viewpoint according to models for fluorescence decay in the presence of traps. In general the decay is consistent with an electric dipole-dipole transfer mechanism. At 2 K the decay can be well described by a direct transfer to Pr and Nd traps without donor-donor transfer. The temperature dependence of the decay at long times can be described for $35<T<70$ K by the hopping model. The agreement with theory is much better if the cross relaxation to Nd ions is assumed to occur mainly via the lowest Stark level of the $^{4}I_{\frac{9}{2}}$ manifold.We have investigated the process of quenching of fluorescence from the $^{3}P_{0}$ state of ${\mathrm{Pr}}^{3+}$ in ${\mathrm{La}}_{0.72}$${\mathrm{Pr}}_{0.25}$${\mathrm{Nd}}_{0.03}$${\mathrm{F}}_{3}$ due to cross relaxation to Pr and Nd ions. The fluorescence decay of the ensemble of Pr ions after pulsed excitation is measured as a function of temperature in the (2-70)-K region. Cross relaxation occurs either directly or through a donor-donor transfer within the inhom-geneous line. Knowledge of the dynamics occurring within the inhomogeneous line derived from previous fluorescence line-narrowing experiments is used to analyze the cross-relaxation process from a microscopic viewpoint according to models for fluorescence decay in the presence of traps. In general the decay is consistent with an electric dipole-dipole transfer mechanism. At 2 K the decay can be well described by a direct transfer to Pr and Nd traps without donor-donor transfer. The temperature dependence of the decay at long times can be described for $35<T<70$ K by the hopping model. The agreement with theory is much better if the cross relaxation to Nd ions is assumed to occur mainly via the lowest Stark level of the $^{4}I_{\frac{9}{2}}$ manifold.

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We report the direct observation of energy migration and spectral diffusion in the $^{3}P_{0}$ state of La ${\mathrm{F}}_{3}$ : ${\mathrm{Pr}}^{3+}$ using the technique of time-resolved fluorescence line narrowing on the resonant $^{3}P_{0}\ensuremath{\rightarrow}^{3}H_{4}$ transition. The temperature dependence of the migration process has been measured and various possible transfer mechanisms are discussed. In addition a variation in the excited-state lifetime as a function of absorption frequency and a concentration broadening at zero delay in the nonresonant transition $^{3}P_{0}\ensuremath{\rightarrow}{(^{3}H_{6})}_{1}$ (the lowest Stark level) are reported.We report the direct observation of energy migration and spectral diffusion in the $^{3}P_{0}$ state of La${\mathrm{F}}_{3}$: ${\mathrm{Pr}}^{3+}$ using the technique of time-resolved fluorescence line narrowing on the resonant $^{3}P_{0}\ensuremath{\rightarrow}^{3}H_{4}$ transition. The temperature dependence of the migration process has been measured and various possible transfer mechanisms are discussed. In addition a variation in the excited-state lifetime as a function of absorption frequency and a concentration broadening at zero delay in the nonresonant transition $^{3}P_{0}\ensuremath{\rightarrow}{(^{3}H_{6})}_{1}$ (the lowest Stark level) are reported.

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Fluorescence quenching by cross relaxation in La F3 : Pr3+

John Hegarty, David L. Huber, William M. Yen

We have investigated the process of quenching of fluorescence from the $^{3}P_{0}$ excited state of ${\mathrm{Pr}}^{3+}$ in La ${\mathrm{F}}_{3}$ due to cross relaxation among the Pr ions. The fluorescence decay of the ensemble of Pr ions after pulsed excitation is measured as a function of temperature for Pr concentration of 20 mol%. About 12% of the ions are in nonquenching sites and contribute an exponential component to the decay. The remainder of the decay originates from the bulk of the ions in quenching sites. Cross relaxation occurs directly in steps after transfer within the inhomogeneous line. Knowledge of the dynamics occurring within the inhomogeneous line derived from fluorescence line-narrowing experiments is used to analyze the cross-relaxation process from a microscopic viewpoint based on a recent model for fluorescence in the presence of traps. At 2 K the decay is consistent with an electric dipole-dipole transfer mechanism with a nearest-neighbor quenching rate of 8.9 \ifmmode\times\else\texttimes\fi{} ${10}^{4}$ ${\mathrm{s}}^{\ensuremath{-}1}$ which is independent of temperature for $T<32$ K and which successfully predicts the observed decay rate in Pr ${\mathrm{F}}_{3}$ . The temperature dependence of the decay for $8\ensuremath{\le}T\ensuremath{\le}32$ K is well described by a hopping model for excitation trapping. For $T>35$ K an activation process becomes dominant consistent with the onset of cross relaxation involving the $^{1}D_{2}(5)$ and $^{3}H_{6}(1)$ states in which a 190-${\mathrm{cm}}^{\ensuremath{-}1}$ phonon is created.We have investigated the process of quenching of fluorescence from the $^{3}P_{0}$ excited state of ${\mathrm{Pr}}^{3+}$ in La${\mathrm{F}}_{3}$ due to cross relaxation among the Pr ions. The fluorescence decay of the ensemble of Pr ions after pulsed excitation is measured as a function of temperature for Pr concentration of 20 mol%. About 12% of the ions are in nonquenching sites and contribute an exponential component to the decay. The remainder of the decay originates from the bulk of the ions in quenching sites. Cross relaxation occurs directly in steps after transfer within the inhomogeneous line. Knowledge of the dynamics occurring within the inhomogeneous line derived from fluorescence line-narrowing experiments is used to analyze the cross-relaxation process from a microscopic viewpoint based on a recent model for fluorescence in the presence of traps. At 2 K the decay is consistent with an electric dipole-dipole transfer mechanism with a nearest-neighbor quenching rate of 8.9 \ifmmode\times\else\texttimes\fi{} ${10}^{4}$ ${\mathrm{s}}^{\ensuremath{-}1}$ which is independent of temperature for $T<32$ K and which successfully predicts the observed decay rate in Pr${\mathrm{F}}_{3}$. The temperature dependence of the decay for $8\ensuremath{\le}T\ensuremath{\le}32$ K is well described by a hopping model for excitation trapping. For $T>35$ K an activation process becomes dominant consistent with the onset of cross relaxation involving the $^{1}D_{2}(5)$ and $^{3}H_{6}(1)$ states in which a 190-${\mathrm{cm}}^{\ensuremath{-}1}$ phonon is created.

Physical review. B, Condensed matterMay 1, 1982130 citations

Donor-donor and donor-acceptor dynamics in

{\mathrm{La}}_{1\ensuremath{-}x}{\mathrm{P}}_{5}{\mathrm{O}}_{14}:{{\mathrm{Nd}}_{x}}^{3+}

x=0.75

We have investigated the process of quenching of fluorescence from the

^{3}P_{0}

state of

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

{\mathrm{La}}_{0.72}

{\mathrm{Pr}}_{0.25}

{\mathrm{Nd}}_{0.03}

{\mathrm{F}}_{3}

due to cross relaxation to Pr and Nd ions. The fluorescence decay of the ensemble of Pr ions after pulsed excitation is measured as a function of temperature in the (2-70)-K region. Cross relaxation occurs either directly or through a donor-donor transfer within the inhom-geneous line. Knowledge of the dynamics occurring within the inhomogeneous line derived from previous fluorescence line-narrowing experiments is used to analyze the cross-relaxation process from a microscopic viewpoint according to models for fluorescence decay in the presence of traps. In general the decay is consistent with an electric dipole-dipole transfer mechanism. At 2 K the decay can be well described by a direct transfer to Pr and Nd traps without donor-donor transfer. The temperature dependence of the decay at long times can be described for

35<T<70

K by the hopping model. The agreement with theory is much better if the cross relaxation to Nd ions is assumed to occur mainly via the lowest Stark level of the

^{4}I_{\frac{9}{2}}

manifold.

We report the direct observation of energy migration and spectral diffusion in the

^{3}P_{0}

state of La

{\mathrm{F}}_{3}

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

using the technique of time-resolved fluorescence line narrowing on the resonant $^{3}P_{0}\ensuremath{\rightarrow}^{3}H_{4}$ transition. The temperature dependence of the migration process has been measured and various possible transfer mechanisms are discussed. In addition a variation in the excited-state lifetime as a function of absorption frequency and a concentration broadening at zero delay in the nonresonant transition $^{3}P_{0}\ensuremath{\rightarrow}{(^{3}H_{6})}_{1}$ (the lowest Stark level) are reported.

We have investigated the process of quenching of fluorescence from the

^{3}P_{0}

excited state of

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

in La

{\mathrm{F}}_{3}

due to cross relaxation among the Pr ions. The fluorescence decay of the ensemble of Pr ions after pulsed excitation is measured as a function of temperature for Pr concentration of 20 mol%. About 12% of the ions are in nonquenching sites and contribute an exponential component to the decay. The remainder of the decay originates from the bulk of the ions in quenching sites. Cross relaxation occurs directly in steps after transfer within the inhomogeneous line. Knowledge of the dynamics occurring within the inhomogeneous line derived from fluorescence line-narrowing experiments is used to analyze the cross-relaxation process from a microscopic viewpoint based on a recent model for fluorescence in the presence of traps. At 2 K the decay is consistent with an electric dipole-dipole transfer mechanism with a nearest-neighbor quenching rate of 8.9 \ifmmode\times\else\texttimes\fi{}

{10}^{4}

${\mathrm{s}}^{\ensuremath{-}1}$ which is independent of temperature for

T<32

K and which successfully predicts the observed decay rate in Pr

{\mathrm{F}}_{3}

. The temperature dependence of the decay for $8\ensuremath{\le}T\ensuremath{\le}32$ K is well described by a hopping model for excitation trapping. For

T>35

K an activation process becomes dominant consistent with the onset of cross relaxation involving the

^{1}D_{2}(5)

and

^{3}H_{6}(1)

states in which a 190-${\mathrm{cm}}^{\ensuremath{-}1}$ phonon is created.