Physical review. B, Solid state

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

Published Dec 1, 1977• 114 citations

Abstract

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.

DOI: 10.1103/physrevb.16.4731

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Physical review. B, Solid state

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

Published Dec 1, 1977• 114 citations

Publisher

Abstract

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.

DOI: 10.1103/physrevb.16.4731

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${\mathrm{F}}_{3}$:${\mathrm{Pr}}^{3+}$.

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Physical Review LettersDec 18, 197891 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

Ultraslow Optical Dephasing of La F3 : Pr3+

Ralph G. DeVoe, A. Szabó, Stephen Colby Rand +1 more

Optical free-induction dephasing times as long as 16 \ensuremath{\mu}sec, corresponding to an optical homogenous linewidth of 10 kHz, have been observed for the $^{3}H_{4}\ensuremath{\leftrightarrow}^{1}D_{2}$ transition of ${\mathrm{Pr}}^{3+}$ ions in La ${\mathrm{F}}_{3}$ at 2\ifmmode^\circ\else\textdegree\fi{}K. Measurements are facilitated by a frequency-locked cw dye laser and a new form of laser frequency switching. Zeeman studies reveal a Pr-F dipole-dipole dephasing mechanism where the Pr nuclear moment is enhanced in both $^{1}D_{2}$ and $^{3}H_{4}$ .Optical free-induction dephasing times as long as 16 \ensuremath{\mu}sec, corresponding to an optical homogenous linewidth of 10 kHz, have been observed for the $^{3}H_{4}\ensuremath{\leftrightarrow}^{1}D_{2}$ transition of ${\mathrm{Pr}}^{3+}$ ions in La${\mathrm{F}}_{3}$ at 2\ifmmode^\circ\else\textdegree\fi{}K. Measurements are facilitated by a frequency-locked cw dye laser and a new form of laser frequency switching. Zeeman studies reveal a Pr-F dipole-dipole dephasing mechanism where the Pr nuclear moment is enhanced in both $^{1}D_{2}$ and $^{3}H_{4}$.

Physical Review LettersJun 4, 197970 citations

Homogeneous broadening and hyperfine structure of optical transitions in Pr 3 + : Y 2 SiO 5

Randy W. Equall, R. L. Cone, R. M. Macfarlane

Contributions to the homogeneous linewidth of the $^{3}$ ${\mathit{H}}_{4}$ (1)${\ensuremath{\rightarrow}}^{1}$ ${\mathit{D}}_{2}$ (1) transition for the two crystallographic sites of ${\mathrm{Pr}}^{3+}$ in ${\mathrm{Y}}_{2}$ ${\mathrm{SiO}}_{5}$ have been investigated using photon echoes. The effects of excitation-intensity-dependent dephasing or instantaneous diffusion were systematically studied to allow accurate determination of the optical resonance widths. Homogeneous linewidths of 2.8 kHz (site 1) and 1 kHz (site 2) were measured with no applied magnetic field and with sufficiently low laser intensity to minimize the effects of instantaneous diffusion. Using the same excitation intensity, widths of 2.1 kHz (site 1) and 0.85 kHz (site 2) were obtained with an applied magnetic field of 77 G, demonstrating a significant contribution of $^{89}\mathrm{Y}$ nuclear-spin fluctuations to the zero-field homogeneous linewidth. Extrapolation to zero excitation intensity yielded optical resonance widths that were only slightly narrower than the measured values. Optically detected nuclear magnetic resonance measurements determined the hyperfine structure of the $^{3}$ ${\mathit{H}}_{4}$ ground state for each site; the hyperfine levels of the lowest component of the $^{1}$ ${\mathit{D}}_{2}$ manifold for each site were determined using photon echo nuclear double resonance. The relatively large oscillator strength of 3\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}7}$ for a rare-earth ion, in conjunction with long dephasing times makes this material a useful candidate for demonstration of time-domain signal processing and optical data storage.Contributions to the homogeneous linewidth of the $^{3}$${\mathit{H}}_{4}$(1)${\ensuremath{\rightarrow}}^{1}$${\mathit{D}}_{2}$(1) transition for the two crystallographic sites of ${\mathrm{Pr}}^{3+}$ in ${\mathrm{Y}}_{2}$${\mathrm{SiO}}_{5}$ have been investigated using photon echoes. The effects of excitation-intensity-dependent dephasing or instantaneous diffusion were systematically studied to allow accurate determination of the optical resonance widths. Homogeneous linewidths of 2.8 kHz (site 1) and 1 kHz (site 2) were measured with no applied magnetic field and with sufficiently low laser intensity to minimize the effects of instantaneous diffusion. Using the same excitation intensity, widths of 2.1 kHz (site 1) and 0.85 kHz (site 2) were obtained with an applied magnetic field of 77 G, demonstrating a significant contribution of $^{89}\mathrm{Y}$ nuclear-spin fluctuations to the zero-field homogeneous linewidth. Extrapolation to zero excitation intensity yielded optical resonance widths that were only slightly narrower than the measured values. Optically detected nuclear magnetic resonance measurements determined the hyperfine structure of the $^{3}$${\mathit{H}}_{4}$ ground state for each site; the hyperfine levels of the lowest component of the $^{1}$${\mathit{D}}_{2}$ manifold for each site were determined using photon echo nuclear double resonance. The relatively large oscillator strength of 3\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}7}$ for a rare-earth ion, in conjunction with long dephasing times makes this material a useful candidate for demonstration of time-domain signal processing and optical data storage.

Physical review. B, Condensed matterAug 1, 1995213 citations

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

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+}

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.

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.

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

ions in La

{\mathrm{F}}_{3}

at 2\ifmmode^\circ\else\textdegree\fi{}K. Measurements are facilitated by a frequency-locked cw dye laser and a new form of laser frequency switching. Zeeman studies reveal a Pr-F dipole-dipole dephasing mechanism where the Pr nuclear moment is enhanced in both

^{1}D_{2}

and

^{3}H_{4}

Contributions to the homogeneous linewidth of the

^{3}

{\mathit{H}}_{4}

(1)${\ensuremath{\rightarrow}}^{1}$

{\mathit{D}}_{2}

(1) transition for the two crystallographic sites of

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

{\mathrm{Y}}_{2}

{\mathrm{SiO}}_{5}

have been investigated using photon echoes. The effects of excitation-intensity-dependent dephasing or instantaneous diffusion were systematically studied to allow accurate determination of the optical resonance widths. Homogeneous linewidths of 2.8 kHz (site 1) and 1 kHz (site 2) were measured with no applied magnetic field and with sufficiently low laser intensity to minimize the effects of instantaneous diffusion. Using the same excitation intensity, widths of 2.1 kHz (site 1) and 0.85 kHz (site 2) were obtained with an applied magnetic field of 77 G, demonstrating a significant contribution of

^{89}\mathrm{Y}

nuclear-spin fluctuations to the zero-field homogeneous linewidth. Extrapolation to zero excitation intensity yielded optical resonance widths that were only slightly narrower than the measured values. Optically detected nuclear magnetic resonance measurements determined the hyperfine structure of the

^{3}

{\mathit{H}}_{4}

ground state for each site; the hyperfine levels of the lowest component of the

^{1}

{\mathit{D}}_{2}

manifold for each site were determined using photon echo nuclear double resonance. The relatively large oscillator strength of 3\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}7}$ for a rare-earth ion, in conjunction with long dephasing times makes this material a useful candidate for demonstration of time-domain signal processing and optical data storage.