Physical review. B, Condensed matter

Hyperfine structures of praseodymium ions in solids using stimulated-photon-echo modulation

M. K. Kim, Ravinder Kachru

Published Nov 1, 1991• 13 citations

Abstract

We report a systematic study of the stimulated-photon-echo relaxation on the $^{3}$${\mathit{P}}_{0}$${\mathrm{\ensuremath{-}}}^{3}$${\mathit{H}}_{4}$ transition of ${\mathrm{Pr}}^{3+}$:${\mathrm{LaF}}_{3}$ and the $^{3}$${\mathit{P}}_{0}$${\mathrm{\ensuremath{-}}}^{3}$${\mathit{H}}_{4}$ and $^{1}$${\mathit{D}}_{2}$${\mathrm{\ensuremath{-}}}^{3}$${\mathit{H}}_{4}$ transitions of ${\mathrm{Pr}}^{3+}$:YAG (yttrium aluminum garnet). The stimulated-echo intensity is measured as a function of the delay between the first and the second pulses and the delay between the second and the third pulses. The stimulated-echo relaxation is modulated by the hyperfine interaction in the ground and the excited electronic states. We find that the modulation patterns can be quite distinct from those for two-pulse photon-echo relaxation and give complementary information about the hyperfine structures. We use the density-matrix theory of stimulated-photon-echo modulation, and the resulting simulation shows satisfactory agreement with the experimental data.

DOI: 10.1103/physrevb.44.9826

Related papers

Stimulated photon echo modulation in praseodymium-doped crystals

P. Talagala, M. K. Kim, Ravinder Kachru

Annual Meeting Optical Society of AmericaJan 1, 19900 citations

Hyperfine measurements of the D21 −3 H4 transition in Pr3+ : Yttrium aluminum garnet using photon echo

M. K. Kim, Ravinder Kachru

Physical review. B, Condensed matterAug 1, 198910 citations

Stimulated-photon-echo spectroscopy. II. Echo modulation in Pr3+ : YAlO3

Masaharu Mitsunaga, Ryuzi Yano, Naoshi Uesugi

Physical review. B, Condensed matterJun 1, 199227 citations

Intensity-dependent photon-echo relaxation in rare-earth-doped crystals

Stefan Kröll, E. Y. Xu, M. K. Kim +2 more

Physical review. B, Condensed matterJun 1, 199033 citations

Spectroscopic and relaxation character of the P03−H43 transition in La F3 : Pr3+ measured by photon echoes

Y.C. Chen, Kophu P. Chiang, Sven R. Hartmann

Physical review. B, Condensed matterJan 1, 198064 citations

Hyperfine structure of the D21−H43 levels of Pr3+ : La F3 with the use of photon echo modulation spectroscopy

Edward A. Whittaker, Sven R. Hartmann

Physical review. B, Condensed matterOct 1, 198226 citations

Physical review. B, Condensed matter

Hyperfine structures of praseodymium ions in solids using stimulated-photon-echo modulation

M. K. Kim, Ravinder Kachru

Published Nov 1, 1991• 13 citations

Publisher

Abstract

We report a systematic study of the stimulated-photon-echo relaxation on the

^{3}$${\mathit{P}}_{0}$${\mathrm{\ensuremath{-}}}^{3}$${\mathit{H}}_{4}

transition of

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

{\mathrm{LaF}}_{3}

and the

^{3}$${\mathit{P}}_{0}$${\mathrm{\ensuremath{-}}}^{3}$${\mathit{H}}_{4}

and

^{1}$${\mathit{D}}_{2}$${\mathrm{\ensuremath{-}}}^{3}$${\mathit{H}}_{4}

transitions of

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

:YAG (yttrium aluminum garnet). The stimulated-echo intensity is measured as a function of the delay between the first and the second pulses and the delay between the second and the third pulses. The stimulated-echo relaxation is modulated by the hyperfine interaction in the ground and the excited electronic states. We find that the modulation patterns can be quite distinct from those for two-pulse photon-echo relaxation and give complementary information about the hyperfine structures. We use the density-matrix theory of stimulated-photon-echo modulation, and the resulting simulation shows satisfactory agreement with the experimental data.

DOI: 10.1103/physrevb.44.9826

Related papers

Stimulated photon echo modulation in praseodymium-doped crystals

P. Talagala, M. K. Kim, Ravinder Kachru

When the intensity of photon echo in a two-level system is measured as a function of delay time of the two input pulses, one obtains a simple exponential decay with the characteristic phase relaxation time. When the two levels contain hyperfine structures, the interference among the hyperfine levels gives rise to modulation of the decay envelope. The Fourier transform of the modulation pattern reveals the hyperfine structure of the rare-earth ions. The hyperfine structure, and therefore the modulation pattern, are both sensitively affected by the crystal environment of the ionic site. We extend photon-echo modulation spectroscopy to three-pulse, stimulated photon-echo modulation, and we find that the stimulated echo modulation patterns are quite distinct from the two-pulse, photon-echo case and are affected by a different set of atomic and crystal interaction parameters. The modulation is measured, in several photon-echo transitions of praseodymium ions in lanthanum trifluoride and yttrium aluminum garnet crystals, as functions of delay times between first and second pulses and between first and third pulses. Comparison of the experimental results with density-matrix calculations allows us to determine hyperfine parameters that are not easily observed with two-pulse echo modulation.When the intensity of photon echo in a two-level system is measured as a function of delay time of the two input pulses, one obtains a simple exponential decay with the characteristic phase relaxation time. When the two levels contain hyperfine structures, the interference among the hyperfine levels gives rise to modulation of the decay envelope. The Fourier transform of the modulation pattern reveals the hyperfine structure of the rare-earth ions. The hyperfine structure, and therefore the modulation pattern, are both sensitively affected by the crystal environment of the ionic site. We extend photon-echo modulation spectroscopy to three-pulse, stimulated photon-echo modulation, and we find that the stimulated echo modulation patterns are quite distinct from the two-pulse, photon-echo case and are affected by a different set of atomic and crystal interaction parameters. The modulation is measured, in several photon-echo transitions of praseodymium ions in lanthanum trifluoride and yttrium aluminum garnet crystals, as functions of delay times between first and second pulses and between first and third pulses. Comparison of the experimental results with density-matrix calculations allows us to determine hyperfine parameters that are not easily observed with two-pulse echo modulation.

Annual Meeting Optical Society of AmericaJan 1, 19900 citations

Hyperfine measurements of the D21 −3 H4 transition in Pr3+ : Yttrium aluminum garnet using photon echo

M. K. Kim, Ravinder Kachru

The hyperfine structure of the $^{1}\mathrm{D}_{2}$ ${\mathrm{\ensuremath{-}}}^{3}$ ${\mathrm{H}}_{4}$ transition of ${\mathrm{Pr}}^{3+}$ : yttrium aluminum garnet (YAG) is studied using a photon echo modulation technique. The Fourier transform of modulation data gives hyperfine frequencies of the $^{1}\mathrm{D}_{2}$ state as 3.42 and 5.96 MHz. The photon echo modulation is a very sensitive function of the atomic environment, and we find that the site symmetry of ${\mathrm{Pr}}^{3+}$ impurity ions in YAG is lowered to ${C}_{2}$ from the ${D}_{2}$ symmetry of ${\mathrm{Y}}^{3+}$ ions.The hyperfine structure of the $^{1}\mathrm{D}_{2}$${\mathrm{\ensuremath{-}}}^{3}$${\mathrm{H}}_{4}$ transition of ${\mathrm{Pr}}^{3+}$: yttrium aluminum garnet (YAG) is studied using a photon echo modulation technique. The Fourier transform of modulation data gives hyperfine frequencies of the $^{1}\mathrm{D}_{2}$ state as 3.42 and 5.96 MHz. The photon echo modulation is a very sensitive function of the atomic environment, and we find that the site symmetry of ${\mathrm{Pr}}^{3+}$ impurity ions in YAG is lowered to ${C}_{2}$ from the ${D}_{2}$ symmetry of ${\mathrm{Y}}^{3+}$ ions.

Physical review. B, Condensed matterAug 1, 198910 citations

Stimulated-photon-echo spectroscopy. II. Echo modulation in Pr3+ : YAlO3

Masaharu Mitsunaga, Ryuzi Yano, Naoshi Uesugi

Stimulated-photon-echo measurements as a function of both the first-to-second (\ensuremath{\tau}) and the second-to-third (T) pulse separations were conducted to study the echo-modulation behavior for the $^{3}$ ${\mathit{H}}_{4}$ ${\mathrm{\ensuremath{-}}}^{1}$ ${\mathit{D}}_{2}$ transition of a cryogenic ${\mathrm{Pr}}^{3+}$ : ${\mathrm{YAlO}}_{3}$ sample. When T is shorter than the excited-state lifetime ${\mathit{T}}_{1}$ , deep echo modulations along both the \ensuremath{\tau} and T axes are observed, the frequencies of which correspond to the excited-state sublevel splittings. When T exceeds ${\mathit{T}}_{1}$ , the modulation is still observed, although only along the \ensuremath{\tau} axis. A density-matrix theory is developed in a perturbative manner to explain these coherent dynamical properties. The numerically simulated three-dimensional plots of the echo intensity versus \ensuremath{\tau} and T are presented, predicting quite satisfactorily the seemingly complicated experimental modulation patterns.Stimulated-photon-echo measurements as a function of both the first-to-second (\ensuremath{\tau}) and the second-to-third (T) pulse separations were conducted to study the echo-modulation behavior for the $^{3}$${\mathit{H}}_{4}$${\mathrm{\ensuremath{-}}}^{1}$${\mathit{D}}_{2}$ transition of a cryogenic ${\mathrm{Pr}}^{3+}$:${\mathrm{YAlO}}_{3}$ sample. When T is shorter than the excited-state lifetime ${\mathit{T}}_{1}$, deep echo modulations along both the \ensuremath{\tau} and T axes are observed, the frequencies of which correspond to the excited-state sublevel splittings. When T exceeds ${\mathit{T}}_{1}$, the modulation is still observed, although only along the \ensuremath{\tau} axis. A density-matrix theory is developed in a perturbative manner to explain these coherent dynamical properties. The numerically simulated three-dimensional plots of the echo intensity versus \ensuremath{\tau} and T are presented, predicting quite satisfactorily the seemingly complicated experimental modulation patterns.

Physical review. B, Condensed matterJun 1, 199227 citations

Intensity-dependent photon-echo relaxation in rare-earth-doped crystals

Stefan Kröll, E. Y. Xu, M. K. Kim +2 more

Photon-echo-relaxation measurements made on the $^{3}\mathrm{H}_{4}$ ${\mathrm{\ensuremath{-}}}^{3}$ ${\mathrm{P}}_{0}$ transition of 0.01 at. % ${\mathrm{Pr}}^{3+}$ :YAG (where YAG represents yttrium aluminum garnet), $^{3}\mathrm{H}_{4}$ ${\mathrm{\ensuremath{-}}}^{1}$ ${\mathrm{D}}_{2}$ transition in 0.1 at. % ${\mathrm{Pr}}^{3+}$ : ${\mathrm{YAlO}}_{3}$ , and $^{7}\mathrm{F}_{0}$ ${\mathrm{\ensuremath{-}}}^{5}$ ${\mathrm{D}}_{0}$ transition in 0.25 at. % ${\mathrm{Eu}}^{3+}$ : ${\mathrm{YAlO}}_{3}$ show that the photon-echo relaxation rate increases when the intensities of the excitation pulses are increased. Although a part of the relaxation-rate increase in ${\mathrm{Pr}}^{3+}$ :YAG may be attributed to an instantaneous spectral diffusion (ISD) in which the presence of excited neighboring ${\mathrm{Pr}}^{3+}$ ions change the local field and the absorption frequency of the rare-earth ions, our data deviate significantly from the ISD-model predictions. An additional intensity-dependent relaxation mechanism is required to explain the results.Photon-echo-relaxation measurements made on the $^{3}\mathrm{H}_{4}$${\mathrm{\ensuremath{-}}}^{3}$${\mathrm{P}}_{0}$ transition of 0.01 at. % ${\mathrm{Pr}}^{3+}$:YAG (where YAG represents yttrium aluminum garnet), $^{3}\mathrm{H}_{4}$${\mathrm{\ensuremath{-}}}^{1}$${\mathrm{D}}_{2}$ transition in 0.1 at. % ${\mathrm{Pr}}^{3+}$:${\mathrm{YAlO}}_{3}$, and $^{7}\mathrm{F}_{0}$${\mathrm{\ensuremath{-}}}^{5}$${\mathrm{D}}_{0}$ transition in 0.25 at. % ${\mathrm{Eu}}^{3+}$:${\mathrm{YAlO}}_{3}$ show that the photon-echo relaxation rate increases when the intensities of the excitation pulses are increased. Although a part of the relaxation-rate increase in ${\mathrm{Pr}}^{3+}$:YAG may be attributed to an instantaneous spectral diffusion (ISD) in which the presence of excited neighboring ${\mathrm{Pr}}^{3+}$ ions change the local field and the absorption frequency of the rare-earth ions, our data deviate significantly from the ISD-model predictions. An additional intensity-dependent relaxation mechanism is required to explain the results.

Physical review. B, Condensed matterJun 1, 199033 citations

Spectroscopic and relaxation character of the P03−H43 transition in La F3 : Pr3+ measured by photon echoes

Y.C. Chen, Kophu P. Chiang, Sven R. Hartmann

The hyperfine structure and relaxation character of the terminal levels of the $^{3}P_{0}\ensuremath{-}^{3}H_{4}$ (4777 \AA{}) transition in La ${\mathrm{F}}_{3}$ : ${\mathrm{Pr}}^{3+}$ (0.03 at.%) were studied using the photon-echo technique. Using two independent nitrogen-laser pumped dye lasers we have observed modulated photon echoes for pulse separations over a \ensuremath{\sim}10-\ensuremath{\mu}sec range. In this interval our modulated photon echoes decay in a simple exponential manner by a factor of ${10}^{5}$ and yield a homogeneous linewidth of 70 kHz [full width at half maximum (FWHM)]. Fourier transformation of the echo-modulation data yields directly the nuclear level splittings and their associated linewidths in the $^{3}P_{0}$ and $^{3}H_{4}$ states. In the $^{3}P_{0}(^{3}H_{4})$ state the nuclear splittings are 0.73 and 1.12 MHz (8.48 and 16.68 MHz). The measurements for the nuclear level splittings and associated linewidths in the $^{3}H_{4}$ state are in excellent agreement with those obtained from the optical-rf double-resonance experiments of Erickson. We find that the calculated echo modulation is a sensitive function of the relative orientation of the principal axes associated with the ground-and excited-state Hamiltonians. By comparing our experimental and calculated echo-modulation patterns we are able to determine their relative orientations.The hyperfine structure and relaxation character of the terminal levels of the $^{3}P_{0}\ensuremath{-}^{3}H_{4}$ (4777 \AA{}) transition in La${\mathrm{F}}_{3}$: ${\mathrm{Pr}}^{3+}$ (0.03 at.%) were studied using the photon-echo technique. Using two independent nitrogen-laser pumped dye lasers we have observed modulated photon echoes for pulse separations over a \ensuremath{\sim}10-\ensuremath{\mu}sec range. In this interval our modulated photon echoes decay in a simple exponential manner by a factor of ${10}^{5}$ and yield a homogeneous linewidth of 70 kHz [full width at half maximum (FWHM)]. Fourier transformation of the echo-modulation data yields directly the nuclear level splittings and their associated linewidths in the $^{3}P_{0}$ and $^{3}H_{4}$ states. In the $^{3}P_{0}(^{3}H_{4})$ state the nuclear splittings are 0.73 and 1.12 MHz (8.48 and 16.68 MHz). The measurements for the nuclear level splittings and associated linewidths in the $^{3}H_{4}$ state are in excellent agreement with those obtained from the optical-rf double-resonance experiments of Erickson. We find that the calculated echo modulation is a sensitive function of the relative orientation of the principal axes associated with the ground-and excited-state Hamiltonians. By comparing our experimental and calculated echo-modulation patterns we are able to determine their relative orientations.

Physical review. B, Condensed matterJan 1, 198064 citations

Hyperfine structure of the D21−H43 levels of Pr3+ : La F3 with the use of photon echo modulation spectroscopy

Edward A. Whittaker, Sven R. Hartmann

We have performed a photon echo modulation measurement of the $^{1}D_{2}\ensuremath{-}^{3}H_{4}$ levels of ${\mathrm{Pr}}^{3+}$ : La ${\mathrm{F}}_{3}$ . This time-domain method yields a precise determination of the $^{1}D_{2}$ excited-state hyperfine splittings and linewidths. New information on the relative orientation of the principal axes of the excited- and ground-state hyperfine Hamiltonians is presented.We have performed a photon echo modulation measurement of the $^{1}D_{2}\ensuremath{-}^{3}H_{4}$ levels of ${\mathrm{Pr}}^{3+}$: La${\mathrm{F}}_{3}$. This time-domain method yields a precise determination of the $^{1}D_{2}$ excited-state hyperfine splittings and linewidths. New information on the relative orientation of the principal axes of the excited- and ground-state hyperfine Hamiltonians is presented.

Physical review. B, Condensed matterOct 1, 198226 citations

We report a systematic study of the stimulated-photon-echo relaxation on the

^{3}$${\mathit{P}}_{0}$${\mathrm{\ensuremath{-}}}^{3}$${\mathit{H}}_{4}

transition of

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

{\mathrm{LaF}}_{3}

and the

^{3}$${\mathit{P}}_{0}$${\mathrm{\ensuremath{-}}}^{3}$${\mathit{H}}_{4}

and

^{1}$${\mathit{D}}_{2}$${\mathrm{\ensuremath{-}}}^{3}$${\mathit{H}}_{4}

transitions of

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

The hyperfine structure of the

^{1}\mathrm{D}_{2}

${\mathrm{\ensuremath{-}}}^{3}$

{\mathrm{H}}_{4}

transition of

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

: yttrium aluminum garnet (YAG) is studied using a photon echo modulation technique. The Fourier transform of modulation data gives hyperfine frequencies of the

^{1}\mathrm{D}_{2}

state as 3.42 and 5.96 MHz. The photon echo modulation is a very sensitive function of the atomic environment, and we find that the site symmetry of

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

impurity ions in YAG is lowered to

{C}_{2}

from the

{D}_{2}

symmetry of

{\mathrm{Y}}^{3+}

ions.

^{3}

{\mathit{H}}_{4}

${\mathrm{\ensuremath{-}}}^{1}$

{\mathit{D}}_{2}

transition of a cryogenic

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

{\mathrm{YAlO}}_{3}

sample. When T is shorter than the excited-state lifetime

{\mathit{T}}_{1}

, deep echo modulations along both the \ensuremath{\tau} and T axes are observed, the frequencies of which correspond to the excited-state sublevel splittings. When T exceeds

{\mathit{T}}_{1}

, the modulation is still observed, although only along the \ensuremath{\tau} axis. A density-matrix theory is developed in a perturbative manner to explain these coherent dynamical properties. The numerically simulated three-dimensional plots of the echo intensity versus \ensuremath{\tau} and T are presented, predicting quite satisfactorily the seemingly complicated experimental modulation patterns.

Photon-echo-relaxation measurements made on the

^{3}\mathrm{H}_{4}

${\mathrm{\ensuremath{-}}}^{3}$

{\mathrm{P}}_{0}

transition of 0.01 at. %

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

:YAG (where YAG represents yttrium aluminum garnet),

^{3}\mathrm{H}_{4}

${\mathrm{\ensuremath{-}}}^{1}$

{\mathrm{D}}_{2}

transition in 0.1 at. %

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

{\mathrm{YAlO}}_{3}

, and

^{7}\mathrm{F}_{0}

${\mathrm{\ensuremath{-}}}^{5}$

{\mathrm{D}}_{0}

transition in 0.25 at. %

{\mathrm{Eu}}^{3+}

{\mathrm{YAlO}}_{3}

show that the photon-echo relaxation rate increases when the intensities of the excitation pulses are increased. Although a part of the relaxation-rate increase in

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

:YAG may be attributed to an instantaneous spectral diffusion (ISD) in which the presence of excited neighboring

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

ions change the local field and the absorption frequency of the rare-earth ions, our data deviate significantly from the ISD-model predictions. An additional intensity-dependent relaxation mechanism is required to explain the results.

The hyperfine structure and relaxation character of the terminal levels of the $^{3}P_{0}\ensuremath{-}^{3}H_{4}$ (4777 \AA{}) transition in La

{\mathrm{F}}_{3}

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

(0.03 at.%) were studied using the photon-echo technique. Using two independent nitrogen-laser pumped dye lasers we have observed modulated photon echoes for pulse separations over a \ensuremath{\sim}10-\ensuremath{\mu}sec range. In this interval our modulated photon echoes decay in a simple exponential manner by a factor of

{10}^{5}

and yield a homogeneous linewidth of 70 kHz [full width at half maximum (FWHM)]. Fourier transformation of the echo-modulation data yields directly the nuclear level splittings and their associated linewidths in the

^{3}P_{0}

and

^{3}H_{4}

states. In the

^{3}P_{0}(^{3}H_{4})

state the nuclear splittings are 0.73 and 1.12 MHz (8.48 and 16.68 MHz). The measurements for the nuclear level splittings and associated linewidths in the

^{3}H_{4}

state are in excellent agreement with those obtained from the optical-rf double-resonance experiments of Erickson. We find that the calculated echo modulation is a sensitive function of the relative orientation of the principal axes associated with the ground-and excited-state Hamiltonians. By comparing our experimental and calculated echo-modulation patterns we are able to determine their relative orientations.

We have performed a photon echo modulation measurement of the $^{1}D_{2}\ensuremath{-}^{3}H_{4}$ levels of

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

: La

{\mathrm{F}}_{3}

. This time-domain method yields a precise determination of the

^{1}D_{2}

excited-state hyperfine splittings and linewidths. New information on the relative orientation of the principal axes of the excited- and ground-state hyperfine Hamiltonians is presented.