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Optics Letters

Measurement of the hyperfine structure of Pr^3::YAG by quantum-beat free-induction decay, hole burning, and optically detected nuclear quadrupole resonance

Robert M. Shelby, A.C. Tropper, Richard T. Harley, R. M. Macfarlane

Published Jun 1, 1983• 48 citations
Publisher

Abstract

The hyperfine splitting of the ground state and the lowest electronic component of the (1)D(2) excited state have been measured for Pr(3+) in YAG. We show that a particularly simple and powerful technique is the production of sublevel coherence by short-pulse (impact) excitation, which is detected by coherent forward scattering of a weak probe beam and Fourier transformation of the resulting quantum-beat signal. This yielded excited-state splittings of 6.49 and 8.29 MHz. The ground state shows large pseudoquadrupole splittings of 33.4 and 41.6 MHz, which were obtained by optically detected nuclear quadrupole resonance.

DOI
10.1364/ol.8.000304

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Two-pulse photon echo electron-nuclear double resonance of YAl O3 : Pr3+

Robert M. Shelby, R. M. Macfarlane, R. L. Shoemaker

Two-pulse photon echo electron-nuclear double resonance (or PENDOR) has been used to measure the second-order hyperfine splittings in the ground state and the lowest component of the excited $^{1}D_{2}$ state of YAl${\mathrm{O}}_{3}$:${\mathrm{Pr}}^{3+}$. The excited-state splittings are 0.923 and 1.565 MHz and are significantly different from previous hole-burning results because of greatly increased resolution. The mechanism for two-pulse PENDOR involves a modulation of the photon echo decay at the rf Rabi frequency. This modulation has been observed directly. A brief theoretical analysis is given which shows that the echo modulation is a result of phase and amplitude changes in the oscillating opitical dipole moment which are indirectly produced by the rf field.

Physical review. B, Condensed matter•Jun 1, 1982•23 citations

Measurement of nuclear and electronic Zeeman effects using optical hole-burning spectroscopy

R. M. Macfarlane, Robert M. Shelby

The excited-state nuclear Zeeman effect and quadratic-electronic Zeeman effect were studied in Pr(3+):LaF(3) using laser-induced hole burning. Hole burning in an external magnetic field gave values for the excited-state enhanced nuclear g tensor of g(x)beta/h = 2.2, g(y)beta/h = 1.9, and g(z)beta/h = 3.6 kHz/G. By applying the field after hole burning, quadratic-electronic Zeeman coefficients as small as 0.1 Hz/G(2) were measured. The hyperfine coupling constant in the excited (1)D(2) level was found to be A(J) = 600 MHz.

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Hyperfine structure and hyperfine coherent properties of praseodymium in single-crystalline La2(WO4)3 by hole-burning and photon-echo techniques

O. Guillot-Noël, Philippe Goldner, Florian Beaudoux +6 more

We studied the hyperfine structure and hyperfine coherent properties of the ${^{3}\text{H}}_{4}(0)\ensuremath{\rightarrow}{^{1}\text{D}}_{2}(0)$ transition of ${\text{Pr}}^{3+}$ ions in a tungstate single crystal ${\text{La}}_{2}{({\text{WO}}_{4})}_{3}$ by hole-burning and photon-echo techniques. This work is motivated by the search of an efficient three level $\ensuremath{\Lambda}$ system in this new compound with which we could build up a quantum memory. By nonconventional hole-burning experiments, the ordering of the hyperfine splittings in the ${^{3}\text{H}}_{4}(0)$ ground state and in the ${^{1}\text{D}}_{2}(0)$ excited state is obtained. The hyperfine splittings are thus ordered: 24.6 and 14.9 MHz for the ${^{3}\text{H}}_{4}(0)$ level and 5.0 and 7.3 MHz for the ${^{1}\text{D}}_{2}(0)$ level. The relative and absolute transition strengths of individual hyperfine transitions are determined by comparing absorption strengths and by measuring the Rabi flopping frequency as the transition is coherently driven. Free induction and Raman echo decays give inhomogeneous and homogeneous hyperfine linewidths of $57\ifmmode\pm\else\textpm\fi{}2$ and $1.25\ifmmode\pm\else\textpm\fi{}0.1\text{ }\text{kHz}$, respectively.

Physical Review B•Apr 27, 2009•30 citations

Coherent raman scattering for optical detection of NMR in Pr³⁺:YAIO₃

Tilo Blasberg

T. Blasberg: Coherent Raman scattering for optical detecti¬ on of NMR in Pr3+:YA103. Nuclear magnetic resonance (NMR) is a powerful and versatile spec¬ troscopic technique. However, conventional NMR requires samples, which has to consist of at least 1017 nuclear spins. One of the most promising approaches to increase the sensitivity of this method relies on the resonant interaction of laser fields with atoms. The main goal of this thesis was the investigation and the improvement of coherent Raman scattering techniques for an optical heterodyne detection of NMR. All ex¬ periments were performed at cryogenic temperatures on Pr3+-ions, which were added to the host lattice YAIO3 (YAP). The coherent Raman scattering experiments consist of two distinct stages: firstly, the transient or continuous excitation of a coherent superposition between two nuclear spin states and secondly, its optical detection through coherent Raman scattering of a resonant, frequency-tunable test laser field from this sublevel coherence. For the theoretical description of the experiments, coherent Raman scattering in multilevel atoms is discussed in detail and a common solution for the Raman heterodyne beat signal in pump-and-probe experiments is derived. The dynamics of a three-level atom that interacts with two resonant electromagnetic fields is treated making use of the density-matrix formalism. The method of Raman heterodyne detection of NMR uses a resonant radio frequency field to drive the magnetic-dipole transition between two nuclear spin states. This technique was used to determine the orientation of the nuclear quadrupole tensors of Pr3+ at its two non-equivalent lattice sites in YAP by measuring the dependence of the transition frequencies on the orientation of an external magnetic field. In the electronic ground state 3H4, the quantization axes of the nuclear spin eigenfunctions are ro¬ tated by po=±56.4° relative to the crystal b-axis. The corresponding rota¬ tion angle in the electronically excited state !D2 is Po=±105.2°. With this new value for the relative orientation of the quantization axes in both electronic states, the relative strengths of all 3H4 1D2 transitions could be calculated. The different orientation of the quantization axes in the two electronic states gives rise to a strong state mixing of the nuclear spin eigenfunctions and is the reason, why most of the optical transitions be¬ tween nuclear spin substates of different electronic states have similar oscillator strengths. Pr:YAP is therefore an ideal model system for the investigation of coherent Raman scattering. A new rf-optical triple-resonance experiment was developed that is a combination of Raman heterodyne detection of NMR and spectral holeburning. This technique allows the unambiguous determination of the ab¬ solute sign of nuclear quadrupole coupling constants. In the electronic ground state of PnYAP, the quadrupole coupling constant was found to be negative (D=-3.5289 MHz) being the result of dominant pseudoquadrupole contributions. The pump-and-probe technique, which uses a frequency-tunable test laser beam, was used to investigate the influence of an inhomogeneous broadening of the optical resonance line on Raman heterodyne detection of NMR. A hitherto unknown interference effect could be predicted and verified by the experiments. A prerequisite for this interference effect is that coherent Raman scattering in different opti¬ cal transitions can contribute to the total Raman heterodyne beat signal. These optical transitions represent different 'scattering pathways', whose contributions to the total beat signal can interfere destructively with each other, since the heterodyne beat signal depends linearly on the relevant transition matrix elements. The rf-optical triple resonance technique al¬ lows to circumvent this interference effect, since the frequency-tunable test laser field can be used to select only one of the various scattering pathways. A new and efficient excitation scheme was developed, which allows the observation of coherent Raman beats in systems with arbitrary wide sublevel spectra and small oscillator strengths. The method utilizes a bichromatic laser field for the purely optical excitation of a coherent superposition between two nuclear spin substates. For the preparation of the sublevel coherence, the two frequency components couple two different nuclear spin substates of the same electronic state to a different electronic state. With the help of the density-matrix formalism, the dyna¬ mics of a three-level atom during the bichromatic excitation were calcu¬ lated. Those experimental parameters could be identified that determine the excitation efficiency. While in the purely optical method of coherent Raman beats almost 10_1 of the incident test laser photons were coherent¬ ly Raman scattered, the corresponding figure of merit of Raman hetero¬ dyne detection of NMR was less man 10-3. From the decay of hole-burning spectra in the presence of a saturating rf-field the temperature-dependence of the nuclear spin relaxation rates of Pr:YAP was determined in the temperature range 3-9 K. At low tem¬ peratures, the relaxation is dominated by mutual spin flips whereas at higher temperatures Orbach and Raman relaxation become of importan¬ ce. A simple rate-equation model allowed to calculate the entire hole-bur¬ ning spectrum of the crystal.

•Jan 1, 1995•0 citations

Hyperfine structure and homogeneous broadening in Pr3+:KY(WO4)2

H. L. Xu, M. Nilsson, S. Ohser +4 more

As part of a search for suitable materials for coherent quantum operations, relaxation times and hyperfine structure of the $^{1}D_{2}(1)\text{\ensuremath{-}}^{3}H_{4}(1)$ transition in ${\mathrm{Pr}}^{3+}:\mathrm{KY}{({\mathrm{WO}}_{4})}_{2}$ (0.29 at. %) at 4 K have been obtained using photon-echo and spectral hole burning techniques. The homogeneous linewidth and the effect of excitation-induced dephasing were measured using two-pulse photon-echo techniques. Linewidths of $23.4\ifmmode\pm\else\textpm\fi{}1.0$ and $17.6\ifmmode\pm\else\textpm\fi{}0.9\phantom{\rule{0.3em}{0ex}}\mathrm{kHz}$ were obtained in the absence and presence of an external magnetic field of about 9 mT. The radiative lifetime $({T}_{1})$ of the $^{1}D_{2}$ state was measured to be $43\ifmmode\pm\else\textpm\fi{}2\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{s}$ using time-resolved laser-induced fluorescence and three-pulse photon-echo measurements. The transmission hole spectra were measured and directly yielded the quadrupole level splitting in the $^{1}D_{2}$ ($3.77\ifmmode\pm\else\textpm\fi{}0.03$ and $4.58\ifmmode\pm\else\textpm\fi{}0.04\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$) and $^{3}H_{4}$ ($17.1\ifmmode\pm\else\textpm\fi{}0.1$ and $33.2\ifmmode\pm\else\textpm\fi{}0.3\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$) states. The spectral hole lifetime due to population redistribution between the ground-state nuclear levels was also determined to be $70\ifmmode\pm\else\textpm\fi{}10\phantom{\rule{0.3em}{0ex}}\mathrm{ms}$. A strong dipole-dipole interaction observed in this crystal opens for potential applications in quantum computing schemes for performing quantum logic operations, but the short dephasing time makes it less useful in data storage applications.

Physical Review B•Dec 30, 2004•8 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.

Physical review. B, Solid state•Dec 1, 1977•114 citations
The hyperfine splitting of the ground state and the lowest electronic component of the (1)D(2) excited state have been measured for Pr(3+) in YAG. We show that a particularly simple and powerful technique is the production of sublevel coherence by short-pulse (impact) excitation, which is detected by coherent forward scattering of a weak probe beam and Fourier transformation of the resulting quantum-beat signal. This yielded excited-state splittings of 6.49 and 8.29 MHz. The ground state shows large pseudoquadrupole splittings of 33.4 and 41.6 MHz, which were obtained by optically detected nuclear quadrupole resonance.
Two-pulse photon echo electron-nuclear double resonance (or PENDOR) has been used to measure the second-order hyperfine splittings in the ground state and the lowest component of the excited 1D2^{1}D_{2}1D2​ state of YAlO3{\mathrm{O}}_{3}O3​:Pr3+{\mathrm{Pr}}^{3+}Pr3+. The excited-state splittings are 0.923 and 1.565 MHz and are significantly different from previous hole-burning results because of greatly increased resolution. The mechanism for two-pulse PENDOR involves a modulation of the photon echo decay at the rf Rabi frequency. This modulation has been observed directly. A brief theoretical analysis is given which shows that the echo modulation is a result of phase and amplitude changes in the oscillating opitical dipole moment which are indirectly produced by the rf field.
The excited-state nuclear Zeeman effect and quadratic-electronic Zeeman effect were studied in Pr(3+):LaF(3) using laser-induced hole burning. Hole burning in an external magnetic field gave values for the excited-state enhanced nuclear g tensor of g(x)beta/h = 2.2, g(y)beta/h = 1.9, and g(z)beta/h = 3.6 kHz/G. By applying the field after hole burning, quadratic-electronic Zeeman coefficients as small as 0.1 Hz/G(2) were measured. The hyperfine coupling constant in the excited (1)D(2) level was found to be A(J) = 600 MHz.
We studied the hyperfine structure and hyperfine coherent properties of the ${^{3}\text{H}}_{4}(0)\ensuremath{\rightarrow}{^{1}\text{D}}_{2}(0)$ transition of Pr3+{\text{Pr}}^{3+}Pr3+ ions in a tungstate single crystal La2(WO4)3{\text{La}}_{2}{({\text{WO}}_{4})}_{3}La2​(WO4​)3​ by hole-burning and photon-echo techniques. This work is motivated by the search of an efficient three level $\ensuremath{\Lambda}$ system in this new compound with which we could build up a quantum memory. By nonconventional hole-burning experiments, the ordering of the hyperfine splittings in the 3H4(0){^{3}\text{H}}_{4}(0)3H4​(0) ground state and in the 1D2(0){^{1}\text{D}}_{2}(0)1D2​(0) excited state is obtained. The hyperfine splittings are thus ordered: 24.6 and 14.9 MHz for the 3H4(0){^{3}\text{H}}_{4}(0)3H4​(0) level and 5.0 and 7.3 MHz for the 1D2(0){^{1}\text{D}}_{2}(0)1D2​(0) level. The relative and absolute transition strengths of individual hyperfine transitions are determined by comparing absorption strengths and by measuring the Rabi flopping frequency as the transition is coherently driven. Free induction and Raman echo decays give inhomogeneous and homogeneous hyperfine linewidths of $57\ifmmode\pm\else\textpm\fi{}2$ and $1.25\ifmmode\pm\else\textpm\fi{}0.1\text{ }\text{kHz}$, respectively.
T. Blasberg: Coherent Raman scattering for optical detecti¬ on of NMR in Pr3+:YA103. Nuclear magnetic resonance (NMR) is a powerful and versatile spec¬ troscopic technique. However, conventional NMR requires samples, which has to consist of at least 1017 nuclear spins. One of the most promising approaches to increase the sensitivity of this method relies on the resonant interaction of laser fields with atoms. The main goal of this thesis was the investigation and the improvement of coherent Raman scattering techniques for an optical heterodyne detection of NMR. All ex¬ periments were performed at cryogenic temperatures on Pr3+-ions, which were added to the host lattice YAIO3 (YAP). The coherent Raman scattering experiments consist of two distinct stages: firstly, the transient or continuous excitation of a coherent superposition between two nuclear spin states and secondly, its optical detection through coherent Raman scattering of a resonant, frequency-tunable test laser field from this sublevel coherence. For the theoretical description of the experiments, coherent Raman scattering in multilevel atoms is discussed in detail and a common solution for the Raman heterodyne beat signal in pump-and-probe experiments is derived. The dynamics of a three-level atom that interacts with two resonant electromagnetic fields is treated making use of the density-matrix formalism. The method of Raman heterodyne detection of NMR uses a resonant radio frequency field to drive the magnetic-dipole transition between two nuclear spin states. This technique was used to determine the orientation of the nuclear quadrupole tensors of Pr3+ at its two non-equivalent lattice sites in YAP by measuring the dependence of the transition frequencies on the orientation of an external magnetic field. In the electronic ground state 3H4, the quantization axes of the nuclear spin eigenfunctions are ro¬ tated by po=±56.4° relative to the crystal b-axis. The corresponding rota¬ tion angle in the electronically excited state !D2 is Po=±105.2°. With this new value for the relative orientation of the quantization axes in both electronic states, the relative strengths of all 3H4 1D2 transitions could be calculated. The different orientation of the quantization axes in the two electronic states gives rise to a strong state mixing of the nuclear spin eigenfunctions and is the reason, why most of the optical transitions be¬ tween nuclear spin substates of different electronic states have similar oscillator strengths. Pr:YAP is therefore an ideal model system for the investigation of coherent Raman scattering. A new rf-optical triple-resonance experiment was developed that is a combination of Raman heterodyne detection of NMR and spectral holeburning. This technique allows the unambiguous determination of the ab¬ solute sign of nuclear quadrupole coupling constants. In the electronic ground state of PnYAP, the quadrupole coupling constant was found to be negative (D=-3.5289 MHz) being the result of dominant pseudoquadrupole contributions. The pump-and-probe technique, which uses a frequency-tunable test laser beam, was used to investigate the influence of an inhomogeneous broadening of the optical resonance line on Raman heterodyne detection of NMR. A hitherto unknown interference effect could be predicted and verified by the experiments. A prerequisite for this interference effect is that coherent Raman scattering in different opti¬ cal transitions can contribute to the total Raman heterodyne beat signal. These optical transitions represent different 'scattering pathways', whose contributions to the total beat signal can interfere destructively with each other, since the heterodyne beat signal depends linearly on the relevant transition matrix elements. The rf-optical triple resonance technique al¬ lows to circumvent this interference effect, since the frequency-tunable test laser field can be used to select only one of the various scattering pathways. A new and efficient excitation scheme was developed, which allows the observation of coherent Raman beats in systems with arbitrary wide sublevel spectra and small oscillator strengths. The method utilizes a bichromatic laser field for the purely optical excitation of a coherent superposition between two nuclear spin substates. For the preparation of the sublevel coherence, the two frequency components couple two different nuclear spin substates of the same electronic state to a different electronic state. With the help of the density-matrix formalism, the dyna¬ mics of a three-level atom during the bichromatic excitation were calcu¬ lated. Those experimental parameters could be identified that determine the excitation efficiency. While in the purely optical method of coherent Raman beats almost 10_1 of the incident test laser photons were coherent¬ ly Raman scattered, the corresponding figure of merit of Raman hetero¬ dyne detection of NMR was less man 10-3. From the decay of hole-burning spectra in the presence of a saturating rf-field the temperature-dependence of the nuclear spin relaxation rates of Pr:YAP was determined in the temperature range 3-9 K. At low tem¬ peratures, the relaxation is dominated by mutual spin flips whereas at higher temperatures Orbach and Raman relaxation become of importan¬ ce. A simple rate-equation model allowed to calculate the entire hole-bur¬ ning spectrum of the crystal.
As part of a search for suitable materials for coherent quantum operations, relaxation times and hyperfine structure of the $^{1}D_{2}(1)\text{\ensuremath{-}}^{3}H_{4}(1)$ transition in Pr3+:KY(WO4)2{\mathrm{Pr}}^{3+}:\mathrm{KY}{({\mathrm{WO}}_{4})}_{2}Pr3+:KY(WO4​)2​ (0.29 at. %) at 4 K have been obtained using photon-echo and spectral hole burning techniques. The homogeneous linewidth and the effect of excitation-induced dephasing were measured using two-pulse photon-echo techniques. Linewidths of $23.4\ifmmode\pm\else\textpm\fi{}1.0$ and $17.6\ifmmode\pm\else\textpm\fi{}0.9\phantom{\rule{0.3em}{0ex}}\mathrm{kHz}$ were obtained in the absence and presence of an external magnetic field of about 9 mT. The radiative lifetime (T1)({T}_{1})(T1​) of the 1D2^{1}D_{2}1D2​ state was measured to be $43\ifmmode\pm\else\textpm\fi{}2\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{s}$ using time-resolved laser-induced fluorescence and three-pulse photon-echo measurements. The transmission hole spectra were measured and directly yielded the quadrupole level splitting in the 1D2^{1}D_{2}1D2​ ($3.77\ifmmode\pm\else\textpm\fi{}0.03$ and $4.58\ifmmode\pm\else\textpm\fi{}0.04\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$) and 3H4^{3}H_{4}3H4​ ($17.1\ifmmode\pm\else\textpm\fi{}0.1$ and $33.2\ifmmode\pm\else\textpm\fi{}0.3\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$) states. The spectral hole lifetime due to population redistribution between the ground-state nuclear levels was also determined to be $70\ifmmode\pm\else\textpm\fi{}10\phantom{\rule{0.3em}{0ex}}\mathrm{ms}$. A strong dipole-dipole interaction observed in this crystal opens for potential applications in quantum computing schemes for performing quantum logic operations, but the short dephasing time makes it less useful in data storage applications.
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 Pr3+{\mathrm{Pr}}^{3+}Pr3+ in LaF3{\mathrm{F}}_{3}F3​ was utilized to observe enhanced and saturated absorptions within the inhomogeneously broadened spectral line. The observed hyperfine splittings of the lowest 1D2^{1}D_{2}1D2​ 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.