Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Physical review. B, Condensed matter

Inhomogeneous broadening in the La1−xPrxF3 system

Ann J. Silversmith, Liren Lou, William M. Yen

Published Sep 1, 1982• 11 citations
Publisher

Abstract

The origin of inhomogeneous broadening in Pr-doped La${\mathrm{F}}_{3}$ is examined by making time-resolved fluorescence measurements. Different positions in the inhomogeneous line are selectively excited, and the lifetime of the fluorescence is measured. The lifetime changes in a systematic way as the pump laser is scanned across the line. We have explained this change as a variation in local concentration of ${\mathrm{Pr}}^{3+}$ ions at the different energies within the inhomogeneous line.

DOI
10.1103/physrevb.26.2656

Related papers

Time-Resolved Fluorescence Line-Narrowing Studies in La F3 : Pr3+

R. Flach, D. S. Hamilton, Peter M. Selzer +1 more

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.

Physical Review Letters•Oct 13, 1975•62 citations

Temporal variation of the fluorescence line shape and relaxation processes in La F3 : Pr3+

Shui T. Lai, Shihua Huang, William M. Yen

The temporal dependence of the fluorescence line shape of Pr ion diluted in La${\mathrm{F}}_{3}$ has been studied in detail. The line-shape study is based on the assumption that the cross relaxation between Pr ions dominates the nonradiative process. The ion-ion interaction has been directly probed by the two-ion cooperative absorption process under which a $^{3}P_{0}$ level lifetime dilation has been observed. The dilation effect can be suppressed when the spectral energy transfer is switched on by raising the temperature of the host crystal. The temporal behavior of the fluorescence line shape of the $^{1}D_{2}$ level has been systematically investigated. The "inhomogeneous" linewidth is found to be composed of a main central peak and a series of ion-pair satellites. The shorter decay lifetime of the ion-pair states results in the narrowing of the emission line shape at later times. The energy positions of the ion-pair states have been measured from the $^{1}D_{2}$ ion pairs up-conversion fluorescence process. The lifetime of the ion-pair states is determined by the coupling strength of the cross relaxation from an excited ion to its partner ion and hence varies according to the ion-pair separation. The decay under the inhomogeneous width is nonexponential in general. Based on the number of the distinguished ion pair levels, a concept of the sphere of influence is introduced. Following this model, an approach has been developed which allows us to study the decay characteristics. Systematical trends emerge from such analysis. The cross-relaxation coupling constants for ion pairs have been extracted from the decay curves and profiles of the ion-pairs line shape have been mapped out. Their peak positions agree with those obtained from $^{1}D_{2}$ ion-pair up-conversion fluorescence measurements.

Physical review. B, Condensed matter•Sep 1, 1982•24 citations

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.

Physical review. B, Condensed matter•May 1, 1982•130 citations

Spectral energy transfer in Pr F3 , Pr Cl3

D. S. Hamilton, Peter M. Selzer, William M. Yen

Time-resolved fluorescence line narrowing is used to study spectral energy transfer in Pr${\mathrm{F}}_{3}$ and Pr${\mathrm{Cl}}_{3}$. The excitation spectrum of Pr${\mathrm{F}}_{3}$ in the region of the ${(^{3}H_{4})}_{1}\ensuremath{\rightarrow}^{3}P_{0}$ absorption indicates that several strong satellite lines accompany the main transition, their origin being ascribed to different ${\mathrm{Pr}}^{3+}$ ions lying in strongly perturbed lattice sites. The spectral transfer within the inhomogeneously broadened main transiton is measured, where the energy mismatch is about 2 ${\mathrm{cm}}^{\ensuremath{-}1}$. This process is characterized by a strong ($\ensuremath{\sim}{T}^{4.3}$) dependence of the transfer probability on sample temperature. The growth of the full inhomogeneous emission profile accompanies a uniform decay of the donor line shape. A transfer process between the lowest-energy satellite ions is also measured. Here the energy mismatch is 32 ${\mathrm{cm}}^{\ensuremath{-}1}$ resulting in a weak temperature dependence for the transfer rate. Both the intraline and intersatellite transfer are characterized by simple exponential rate equations. Recent calculations of phonon-assisted transfer probabilities are compared to our measurements, with the intersatellite transfer ascribed to a "one-phonon direct" process whereas the transfer within the main transition occurs by a "one-phonon second-order" mechanism. In Pr${\mathrm{Cl}}_{3}$ the transfer times are faster than the 15-nsec response time of our detection system indicating a much stronger ion-ion coupling.

Physical review. B, Solid state•Sep 1, 1977•62 citations

Optical Pumping Detection of Anomalous NQR Spectra of Pr3+ in Pr3+:LaF3

Lawrence L. Wald, Erwin Louis Hahn, Matjaž Lukač

The nature of inhomogeneous broadening in rare earth systems plays an important role in the dynamical optical properties of ions in crystals. For this reason much of the work on the nature of the inhomogeneous broadening in rare earth doped systems has concentrated on the investigation of ion-ion interactions such as spectral transfer and up conversion processes.1,3 Variations in homogeneous optical dephasing times across the inhomogeneous optical line have also been reported.4 These studies concentrate on the variations of collective effects of ion- ion interactions at different positions in the inhomogeneous optical line in relatively heavily doped rare earth systems. We report variations in optically detected NQR (ODNQR) linewidths and shifts of Pr3+ hyperfme transitions in the optical ground state as a function of position in the inhomogeneous optical line and for satellite transitions of the 1D2-3H4 transition in lightly doped (0.5 at. %) Pr3+:LaF3.

Spectral Hole-Burning and Related Spectroscopies: Science and Applications•Jan 1, 1991•0 citations

Variation of the Pr^3+ nuclear quadrupole resonance spectrum across the inhomogeneous optical line in Pr^3+:LaF_3

Lawrence L. Wald, Matjaž Lukač, Erwin Louis Hahn

We report nuclear quadrupole resonance (NQR) frequency and linewidth variations of the Pr3+ ground-state hyperfine levels for various positions within the 3H4(Γ1)–1D2(Γ1) inhomogeneous optical line and satellite transitions of Pr3+:LaF3. A linear increase in the broadening of the Pr3+ hyperfine transitions, without a shift of central frequency, is measured by the Stark modulated optical pumping hole-burning technique as the laser is tuned toward the wings of the inhomogeneous optical transition. The linear variation is attributed to electric quadrupole broadening caused by changes in the local density of point defects across the Stark-broadened optical transition. The optically detected NQR spectra of the satellite transitions associated with Pr ion pairs are shifted in frequency and for most satellites are narrower than the NQR spectra found in the wings of the main inhomogeneous optical line.

Journal of the Optical Society of America B•May 1, 1992•7 citations
The origin of inhomogeneous broadening in Pr-doped LaF3{\mathrm{F}}_{3}F3​ is examined by making time-resolved fluorescence measurements. Different positions in the inhomogeneous line are selectively excited, and the lifetime of the fluorescence is measured. The lifetime changes in a systematic way as the pump laser is scanned across the line. We have explained this change as a variation in local concentration of Pr3+{\mathrm{Pr}}^{3+}Pr3+ ions at the different energies within the inhomogeneous line.
We report the direct observation of energy migration and spectral diffusion in the 3P0^{3}P_{0}3P0​ state of LaF3{\mathrm{F}}_{3}F3​: Pr3+{\mathrm{Pr}}^{3+}Pr3+ 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.
The temporal dependence of the fluorescence line shape of Pr ion diluted in LaF3{\mathrm{F}}_{3}F3​ has been studied in detail. The line-shape study is based on the assumption that the cross relaxation between Pr ions dominates the nonradiative process. The ion-ion interaction has been directly probed by the two-ion cooperative absorption process under which a 3P0^{3}P_{0}3P0​ level lifetime dilation has been observed. The dilation effect can be suppressed when the spectral energy transfer is switched on by raising the temperature of the host crystal. The temporal behavior of the fluorescence line shape of the 1D2^{1}D_{2}1D2​ level has been systematically investigated. The "inhomogeneous" linewidth is found to be composed of a main central peak and a series of ion-pair satellites. The shorter decay lifetime of the ion-pair states results in the narrowing of the emission line shape at later times. The energy positions of the ion-pair states have been measured from the 1D2^{1}D_{2}1D2​ ion pairs up-conversion fluorescence process. The lifetime of the ion-pair states is determined by the coupling strength of the cross relaxation from an excited ion to its partner ion and hence varies according to the ion-pair separation. The decay under the inhomogeneous width is nonexponential in general. Based on the number of the distinguished ion pair levels, a concept of the sphere of influence is introduced. Following this model, an approach has been developed which allows us to study the decay characteristics. Systematical trends emerge from such analysis. The cross-relaxation coupling constants for ion pairs have been extracted from the decay curves and profiles of the ion-pairs line shape have been mapped out. Their peak positions agree with those obtained from 1D2^{1}D_{2}1D2​ ion-pair up-conversion fluorescence measurements.
We have investigated the process of quenching of fluorescence from the 3P0^{3}P_{0}3P0​ excited state of Pr3+{\mathrm{Pr}}^{3+}Pr3+ in LaF3{\mathrm{F}}_{3}F3​ 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{} 104{10}^{4}104 ${\mathrm{s}}^{\ensuremath{-}1}$ which is independent of temperature for T<32T<32T<32 K and which successfully predicts the observed decay rate in PrF3{\mathrm{F}}_{3}F3​. 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>35T>35T>35 K an activation process becomes dominant consistent with the onset of cross relaxation involving the 1D2(5)^{1}D_{2}(5)1D2​(5) and 3H6(1)^{3}H_{6}(1)3H6​(1) states in which a 190-${\mathrm{cm}}^{\ensuremath{-}1}$ phonon is created.
Time-resolved fluorescence line narrowing is used to study spectral energy transfer in PrF3{\mathrm{F}}_{3}F3​ and PrCl3{\mathrm{Cl}}_{3}Cl3​. The excitation spectrum of PrF3{\mathrm{F}}_{3}F3​ in the region of the ${(^{3}H_{4})}_{1}\ensuremath{\rightarrow}^{3}P_{0}$ absorption indicates that several strong satellite lines accompany the main transition, their origin being ascribed to different Pr3+{\mathrm{Pr}}^{3+}Pr3+ ions lying in strongly perturbed lattice sites. The spectral transfer within the inhomogeneously broadened main transiton is measured, where the energy mismatch is about 2 ${\mathrm{cm}}^{\ensuremath{-}1}$. This process is characterized by a strong ($\ensuremath{\sim}{T}^{4.3}$) dependence of the transfer probability on sample temperature. The growth of the full inhomogeneous emission profile accompanies a uniform decay of the donor line shape. A transfer process between the lowest-energy satellite ions is also measured. Here the energy mismatch is 32 ${\mathrm{cm}}^{\ensuremath{-}1}$ resulting in a weak temperature dependence for the transfer rate. Both the intraline and intersatellite transfer are characterized by simple exponential rate equations. Recent calculations of phonon-assisted transfer probabilities are compared to our measurements, with the intersatellite transfer ascribed to a "one-phonon direct" process whereas the transfer within the main transition occurs by a "one-phonon second-order" mechanism. In PrCl3{\mathrm{Cl}}_{3}Cl3​ the transfer times are faster than the 15-nsec response time of our detection system indicating a much stronger ion-ion coupling.
The nature of inhomogeneous broadening in rare earth systems plays an important role in the dynamical optical properties of ions in crystals. For this reason much of the work on the nature of the inhomogeneous broadening in rare earth doped systems has concentrated on the investigation of ion-ion interactions such as spectral transfer and up conversion processes.1,3 Variations in homogeneous optical dephasing times across the inhomogeneous optical line have also been reported.4 These studies concentrate on the variations of collective effects of ion- ion interactions at different positions in the inhomogeneous optical line in relatively heavily doped rare earth systems. We report variations in optically detected NQR (ODNQR) linewidths and shifts of Pr3+ hyperfme transitions in the optical ground state as a function of position in the inhomogeneous optical line and for satellite transitions of the 1D2-3H4 transition in lightly doped (0.5 at. %) Pr3+:LaF3.
We report nuclear quadrupole resonance (NQR) frequency and linewidth variations of the Pr3+ ground-state hyperfine levels for various positions within the 3H4(Γ1)–1D2(Γ1) inhomogeneous optical line and satellite transitions of Pr3+:LaF3. A linear increase in the broadening of the Pr3+ hyperfine transitions, without a shift of central frequency, is measured by the Stark modulated optical pumping hole-burning technique as the laser is tuned toward the wings of the inhomogeneous optical transition. The linear variation is attributed to electric quadrupole broadening caused by changes in the local density of point defects across the Stark-broadened optical transition. The optically detected NQR spectra of the satellite transitions associated with Pr ion pairs are shifted in frequency and for most satellites are narrower than the NQR spectra found in the wings of the main inhomogeneous optical line.