Physical review. B, Condensed matter

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

Published Oct 1, 1982• 26 citations

Abstract

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.

DOI: 10.1103/physrevb.26.3617

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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

Photon-echo nuclear double resonance in La F3 : Pr3+

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

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Optical measurement of the hyperfine splitting of the D 2 1 metastable state of Pr 3 + in La F 3 by enhanced and saturated absorption spectroscopy

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

M. K. Kim, Ravinder Kachru

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Optically Detected Coherent Transients in Nuclear Hyperfine Levels

Robert M. Shelby, Constantino S. Yannoni, R. M. Macfarlane

Physical Review LettersDec 18, 197891 citations

Physical review. B, Condensed matter

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

Published Oct 1, 1982• 26 citations

Publisher

Abstract

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.

DOI: 10.1103/physrevb.26.3617

Related papers

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

Photon-echo nuclear double resonance in La F3 : Pr3+

Kophu P. Chiang, Edward A. Whittaker, Sven R. Hartmann

Using the photon-echo-nuclear-double-resonance technique, we have measured the nuclear hyperfine splittings in the excited $^{1}D_{2}$ state of La ${\mathrm{F}}_{3}$ : ${\mathrm{Pr}}^{3+}$ . Our measurements are in agreement with the results obtained by Erickson from his saturated-and-enhanced-absorption study of the $^{3}H_{4}\ensuremath{-}^{1}D_{2}$ transition in La ${\mathrm{F}}_{3}$ : ${\mathrm{Pr}}^{3+}$ .Using the photon-echo-nuclear-double-resonance technique, we have measured the nuclear hyperfine splittings in the excited $^{1}D_{2}$ state of La${\mathrm{F}}_{3}$:${\mathrm{Pr}}^{3+}$. Our measurements are in agreement with the results obtained by Erickson from his saturated-and-enhanced-absorption study of the $^{3}H_{4}\ensuremath{-}^{1}D_{2}$ transition in La${\mathrm{F}}_{3}$:${\mathrm{Pr}}^{3+}$.

Physical review. B, Condensed matterJun 1, 198122 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

Optical measurement of the hyperfine splitting of the D 2 1 metastable state of Pr 3 + in La F 3 by enhanced and saturated absorption spectroscopy

L. E. Erickson

The sizable ground-state nuclear polarization which accompanies the optical pumping of the $^{3}H_{4}\ensuremath{-}^{1}D_{2}$ (16 872-${\mathrm{cm}}^{\ensuremath{-}1}$) $\ensuremath{\sigma}$ transition of ${\mathrm{Pr}}^{3+}$ in La ${\mathrm{F}}_{3}$ was utilized to observe enhanced and saturated absorptions within the inhomogeneously broadened spectral line. The observed hyperfine splittings of the lowest $^{1}D_{2}$ state are 3.7 and 4.7 MHz at 2.0\ifmmode^\circ\else\textdegree\fi{}K. These splittings were fitted by a spin Hamiltonian $\mathcal{H}=D[{I}_{z}^{2}\ensuremath{-}\frac{I(I+1)}{3}]+(\frac{E}{2})({I}_{+}^{2}+{I}_{\ensuremath{-}}^{2})$, where $D=\ensuremath{-}1.10\ifmmode\pm\else\textpm\fi{}0.05$ and $E=\ensuremath{-}0.48\ifmmode\pm\else\textpm\fi{}0.05$ MHz. The observed linewidths (including the exciting laser linewidth) were 0.8 MHz. The deconvoluted optical transition linewidths (full widths at half-maximum) are 0.20\ifmmode\pm\else\textpm\fi{}0.05 MHz.The sizable ground-state nuclear polarization which accompanies the optical pumping of the $^{3}H_{4}\ensuremath{-}^{1}D_{2}$ (16 872-${\mathrm{cm}}^{\ensuremath{-}1}$) $\ensuremath{\sigma}$ transition of ${\mathrm{Pr}}^{3+}$ in La${\mathrm{F}}_{3}$ was utilized to observe enhanced and saturated absorptions within the inhomogeneously broadened spectral line. The observed hyperfine splittings of the lowest $^{1}D_{2}$ state are 3.7 and 4.7 MHz at 2.0\ifmmode^\circ\else\textdegree\fi{}K. These splittings were fitted by a spin Hamiltonian $\mathcal{H}=D[{I}_{z}^{2}\ensuremath{-}\frac{I(I+1)}{3}]+(\frac{E}{2})({I}_{+}^{2}+{I}_{\ensuremath{-}}^{2})$, where $D=\ensuremath{-}1.10\ifmmode\pm\else\textpm\fi{}0.05$ and $E=\ensuremath{-}0.48\ifmmode\pm\else\textpm\fi{}0.05$ MHz. The observed linewidths (including the exciting laser linewidth) were 0.8 MHz. The deconvoluted optical transition linewidths (full widths at half-maximum) are 0.20\ifmmode\pm\else\textpm\fi{}0.05 MHz.

Physical review. B, Solid stateDec 1, 1977114 citations

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

M. K. Kim, Ravinder Kachru

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.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.

Physical review. B, Condensed matterNov 1, 199113 citations

Optically Detected Coherent Transients in Nuclear Hyperfine Levels

Robert M. Shelby, Constantino S. Yannoni, R. M. Macfarlane

Using optical detection, we have observed rf nutation, free-induction decay, and echoes, on the 16.70-MHz nuclear hyperfine transition of dilute ${\mathrm{Pr}}^{3+}$ in La ${\mathrm{F}}_{3}$ at 2 K. From a comparison of free-induction decay and echo decay we find that the previously observed linewidth of 200 kHz is inhomogeneous and that the homogeneous width is 19 kHz. On the basis of these measurements it is suggested that optical dephasing times for the $^{1}D_{2}\ensuremath{\leftrightarrow}^{3}H_{4}$ and $^{3}P_{0}\ensuremath{\leftrightarrow}^{3}H_{4}$ transitions are as long as \ensuremath{\sim}20 \ensuremath{\mu} sec.Using optical detection, we have observed rf nutation, free-induction decay, and echoes, on the 16.70-MHz nuclear hyperfine transition of dilute ${\mathrm{Pr}}^{3+}$ in La${\mathrm{F}}_{3}$ at 2 K. From a comparison of free-induction decay and echo decay we find that the previously observed linewidth of 200 kHz is inhomogeneous and that the homogeneous width is 19 kHz. On the basis of these measurements it is suggested that optical dephasing times for the $^{1}D_{2}\ensuremath{\leftrightarrow}^{3}H_{4}$ and $^{3}P_{0}\ensuremath{\leftrightarrow}^{3}H_{4}$ transitions are as long as \ensuremath{\sim}20 \ensuremath{\mu} sec.

Physical Review LettersDec 18, 197891 citations

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.

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.

Using the photon-echo-nuclear-double-resonance technique, we have measured the nuclear hyperfine splittings in the excited

^{1}D_{2}

state of La

{\mathrm{F}}_{3}

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

. Our measurements are in agreement with the results obtained by Erickson from his saturated-and-enhanced-absorption study of the $^{3}H_{4}\ensuremath{-}^{1}D_{2}$ transition in La

{\mathrm{F}}_{3}

{\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.

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

in La

{\mathrm{F}}_{3}

was utilized to observe enhanced and saturated absorptions within the inhomogeneously broadened spectral line. The observed hyperfine splittings of the lowest

^{1}D_{2}

state are 3.7 and 4.7 MHz at 2.0\ifmmode^\circ\else\textdegree\fi{}K. These splittings were fitted by a spin Hamiltonian $\mathcal{H}=D[{I}_{z}^{2}\ensuremath{-}\frac{I(I+1)}{3}]+(\frac{E}{2})({I}_{+}^{2}+{I}_{\ensuremath{-}}^{2})$, where $D=\ensuremath{-}1.10\ifmmode\pm\else\textpm\fi{}0.05$ and $E=\ensuremath{-}0.48\ifmmode\pm\else\textpm\fi{}0.05$ MHz. The observed linewidths (including the exciting laser linewidth) were 0.8 MHz. The deconvoluted optical transition linewidths (full widths at half-maximum) are 0.20\ifmmode\pm\else\textpm\fi{}0.05 MHz.

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.

Using optical detection, we have observed rf nutation, free-induction decay, and echoes, on the 16.70-MHz nuclear hyperfine transition of dilute

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

in La

{\mathrm{F}}_{3}

at 2 K. From a comparison of free-induction decay and echo decay we find that the previously observed linewidth of 200 kHz is inhomogeneous and that the homogeneous width is 19 kHz. On the basis of these measurements it is suggested that optical dephasing times for the $^{1}D_{2}\ensuremath{\leftrightarrow}^{3}H_{4}$ and $^{3}P_{0}\ensuremath{\leftrightarrow}^{3}H_{4}$ transitions are as long as \ensuremath{\sim}20 \ensuremath{\mu} sec.