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

Raman heterodyne interference: Observations and analytic theory

Masaharu Mitsunaga, Emily S. Kintzer, Richard G. Brewer

Published Jun 1, 1985• 49 citations
Publisher

Abstract

The recently developed technique of Raman heterodyne detection has unveiled a new interference effect in the Zeeman spectrum of hyperfine transitions of impurity-ion solids. An earlier theory had been developed to explain the basic Raman heterodyne process which involves the resonant interaction of a three-level quantum system with coherent optical-frequency and radiofrequency fields. However, it was not realized that impurity-ion crystals can generate more than one type of Raman heterodyne signal and that these signals can interfere. This article describes two examples of interference where one originates from two or more inequivalent nuclear sites and the other from a single site that exhibits interference among Zeeman transitions. An analytical theory covering these two cases is presented and compared to observations for the impurity-ion crystals ${\mathrm{Pr}}^{3+}$:${\mathrm{YAlO}}_{3}$ and ${\mathrm{Pr}}^{3+}$:${\mathrm{LaF}}_{3}$, the interference behavior in the two being dramatically different.

DOI
10.1103/physrevb.31.6947

Related papers

Interference of scattering pathways in Raman heterodyne spectroscopy of multilevel atoms

Tilo Blasberg, Dieter Suter

Raman heterodyne detection of nuclear magnetic resonance is a sensitive technique for optical detection of an NMR transition, which is driven by a resonant radio-frequency field. The observed signal is linear in the transition matrix elements of the magnetic resonance transition and two optical transitions. This linearity is the reason that signal contributions from different sites or different rf transitions can interfere, in many cases destructively. In this article, we discuss such an interference effect, which appears to have been overlooked in the past. It occurs between signal contributions that originate from the same magnetic resonance transition of atoms with different positions within the inhomogeneously broadened optical resonance line. These atoms contribute to the coherent Raman scattering through different scattering paths, which involve optical transitions to different nuclear spin states of the same electronic state. We show that the interference between all possible scattering paths leads to complete signal cancellation, if the atoms that are involved in the different scattering paths are equally polarized. To study the effect and to eliminate the interference, we used a pump-and-probe technique with two laser beams. With two independent laser frequencies, it becomes possible to separate the individual scattering paths. We calculate the dependence of the signal on the frequency of both laser beams as well as on the radio frequency and compare the results to experimental data from ${\mathrm{Pr}}^{3+}$:${\mathrm{YAlO}}_{3}$. Our results show that the interference reduces the signal amplitude of the conventional Raman heterodyne experiment but can be eliminated in the new experiment.

Physical review. B, Condensed matter•May 1, 1995•5 citations

Raman heterodyne detection of nuclear magnetic resonance

N. C. Wong, Emily S. Kintzer, J. Mlynek +2 more

A novel coherent Raman effect induced by a laser and a radio-frequency (rf) field is used to detect cw and pulsed nuclear magnetic resonance (NMR) in ground and excited electronic states. The effect is illustrated in the impurity-ion solid ${\mathrm{Pr}}^{3+}$: La${\mathrm{F}}_{3}$ at 1.6 K utilizing the ${\mathrm{Pr}}^{3+}$ optical transition $^{3}H_{4}({\ensuremath{\Gamma}}_{1})\ensuremath{\rightarrow}^{1}D_{2}({\ensuremath{\Gamma}}_{1})$. The laser field of frequency ${\ensuremath{\omega}}_{E}$ and the rf field (${\ensuremath{\omega}}_{H}$) induce a light wave at the sum ${\ensuremath{\omega}}_{E}+{\ensuremath{\omega}}_{H}$ (anti-Stokes) and difference ${\ensuremath{\omega}}_{E}\ensuremath{-}{\ensuremath{\omega}}_{H}$ (Stokes) frequencies, generating an absorptive or dispersive heterodyne beat signal (${\ensuremath{\omega}}_{H}$) with the laser field at a photodetector. The theory of this effect is characterized in a new three-level perturbation calculation which requires, unlike the usual stimulated Raman effect, that all three transitions be electric- or magnetic-dipole allowed. Detailed predictions are confirmed by cw measurements of the ${\mathrm{Pr}}^{3+}$: La${\mathrm{F}}_{3}$ hyperfine splittings where the optical heterodyne signals are shot-noise limited. The ${\mathrm{Pr}}^{3+}$ nuclear quadrupole parameters are obtained for the $^{3}H_{4}$ and $^{1}D_{2}$ states where the line centers are determined with kilohertz precision. The corresponding wave functions show significant hyperfine-state mixing, as required for all three transitions to be dipole allowed. The cw line shapes are narrow (30-160 kHz), inhomogeneously broadened by nuclear magnetic interactions, and reveal either a Gaussian or an anomalous second-derivative---like line shape. The spin-echo measurements for the $^{3}H_{4}$ and $^{1}D_{2}$ hyperfine transitions yield homogeneous line shapes which are Lorentzian, and rather surprisingly, linewidths in the narrow range 10-20 kHz, a result which tests current line-broadening theories.

Physical review. B, Condensed matter•Nov 1, 1983•110 citations

Raman heterodyne interference: Symmetry analysis

Emily S. Kintzer, Masaharu Mitsunaga, Richard G. Brewer

The Raman heterodyne interference phenomenon observed recently in the impurity-ion crystals ${\mathrm{Pr}}^{3+}$:${\mathrm{YAlO}}_{3}$ and ${\mathrm{Pr}}^{3+}$:${\mathrm{LaF}}_{3}$ is examined from the viewpoint of symmetry analysis of the nonlinear susceptibility tensor. General Raman heterodyne signals are derived for all crystal symmetries and for all optical-frequency and radiofrequency polarizations. An example of the utility of this approach resolves a controversy over the crystal symmetry of ${\mathrm{LaF}}_{3}$, establishing that it is trigonal rather than hexagonal.

Physical review. B, Condensed matter•Jun 1, 1985•22 citations

Raman Heterodyne Detection of Nuclear Magnetic Resonance

J. Mlynek, N. C. Wong, Ralph G. DeVoe +2 more

An optical heterodyne technique based on the coherent Raman effect is demonstrated for detecting nuclear magnetic resonances (NMR) and coherent spin transients in normal and optically excited impurity-ion solids at low temperature. Initial measurements on ${\mathrm{Pr}}^{3+}$: La${\mathrm{F}}_{3}$ provide the first spin-echo studies of an electronically excited state, and cw resonances yield NMR line centers and shapes with kilohertz precision.

Physical Review Letters•Mar 28, 1983•154 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

Dipole interference for optical transitions of ions in crystals in a transverse Zeeman field

Clinton DeW. Van Siclen

An ion is located in a crystal at a site that is not a centre of inversion, with a Zeeman field directed at right angles to the crystal axis c. Periodic intensity variations in the optical spectrum that occur when the crystal is rotated about c are due to magnetic dipole transitions between levels of different type and to electric dipole transitions between levels having admixed opposite-parity parts of different type. Use of an antiunitary operator that commutes with the total Hamiltonian demonstrates that interference between electric and magnetic dipole radiation (or interference between any opposite-parity multipole radiation) does not occur for transitions appearing in the axial spectrum, but does occur for those appearing in the pi or sigma transverse spectrum. Depending on the site symmetry, two or four of the Zeeman components of a doublet-doublet transition have an additional periodicity as a result of this interference. Eigenstates are constructed that show the relationship between the M values of a Zeeman level, the crystal quantum number that labels it, and its type, and are used to calculate the angular dependence of certain doublet-doublet dipole transitions for ions at sites of point symmetries D 2d and C 3h . With explicit expressions for dipole matrix elements, it is discovered that two Zeeman components having the same angular dependence when interference is neglected exhibit dissimilar angular behaviour when the interference cross-term is included.

Journal of Physics C Solid State Physics•Nov 10, 1981•3 citations
The recently developed technique of Raman heterodyne detection has unveiled a new interference effect in the Zeeman spectrum of hyperfine transitions of impurity-ion solids. An earlier theory had been developed to explain the basic Raman heterodyne process which involves the resonant interaction of a three-level quantum system with coherent optical-frequency and radiofrequency fields. However, it was not realized that impurity-ion crystals can generate more than one type of Raman heterodyne signal and that these signals can interfere. This article describes two examples of interference where one originates from two or more inequivalent nuclear sites and the other from a single site that exhibits interference among Zeeman transitions. An analytical theory covering these two cases is presented and compared to observations for the impurity-ion crystals Pr3+{\mathrm{Pr}}^{3+}Pr3+:YAlO3{\mathrm{YAlO}}_{3}YAlO3​ and Pr3+{\mathrm{Pr}}^{3+}Pr3+:LaF3{\mathrm{LaF}}_{3}LaF3​, the interference behavior in the two being dramatically different.
Raman heterodyne detection of nuclear magnetic resonance is a sensitive technique for optical detection of an NMR transition, which is driven by a resonant radio-frequency field. The observed signal is linear in the transition matrix elements of the magnetic resonance transition and two optical transitions. This linearity is the reason that signal contributions from different sites or different rf transitions can interfere, in many cases destructively. In this article, we discuss such an interference effect, which appears to have been overlooked in the past. It occurs between signal contributions that originate from the same magnetic resonance transition of atoms with different positions within the inhomogeneously broadened optical resonance line. These atoms contribute to the coherent Raman scattering through different scattering paths, which involve optical transitions to different nuclear spin states of the same electronic state. We show that the interference between all possible scattering paths leads to complete signal cancellation, if the atoms that are involved in the different scattering paths are equally polarized. To study the effect and to eliminate the interference, we used a pump-and-probe technique with two laser beams. With two independent laser frequencies, it becomes possible to separate the individual scattering paths. We calculate the dependence of the signal on the frequency of both laser beams as well as on the radio frequency and compare the results to experimental data from Pr3+{\mathrm{Pr}}^{3+}Pr3+:YAlO3{\mathrm{YAlO}}_{3}YAlO3​. Our results show that the interference reduces the signal amplitude of the conventional Raman heterodyne experiment but can be eliminated in the new experiment.
A novel coherent Raman effect induced by a laser and a radio-frequency (rf) field is used to detect cw and pulsed nuclear magnetic resonance (NMR) in ground and excited electronic states. The effect is illustrated in the impurity-ion solid Pr3+{\mathrm{Pr}}^{3+}Pr3+: LaF3{\mathrm{F}}_{3}F3​ at 1.6 K utilizing the Pr3+{\mathrm{Pr}}^{3+}Pr3+ optical transition $^{3}H_{4}({\ensuremath{\Gamma}}_{1})\ensuremath{\rightarrow}^{1}D_{2}({\ensuremath{\Gamma}}_{1})$. The laser field of frequency ${\ensuremath{\omega}}_{E}$ and the rf field (${\ensuremath{\omega}}_{H}$) induce a light wave at the sum ${\ensuremath{\omega}}_{E}+{\ensuremath{\omega}}_{H}$ (anti-Stokes) and difference ${\ensuremath{\omega}}_{E}\ensuremath{-}{\ensuremath{\omega}}_{H}$ (Stokes) frequencies, generating an absorptive or dispersive heterodyne beat signal (${\ensuremath{\omega}}_{H}$) with the laser field at a photodetector. The theory of this effect is characterized in a new three-level perturbation calculation which requires, unlike the usual stimulated Raman effect, that all three transitions be electric- or magnetic-dipole allowed. Detailed predictions are confirmed by cw measurements of the Pr3+{\mathrm{Pr}}^{3+}Pr3+: LaF3{\mathrm{F}}_{3}F3​ hyperfine splittings where the optical heterodyne signals are shot-noise limited. The Pr3+{\mathrm{Pr}}^{3+}Pr3+ nuclear quadrupole parameters are obtained for the 3H4^{3}H_{4}3H4​ and 1D2^{1}D_{2}1D2​ states where the line centers are determined with kilohertz precision. The corresponding wave functions show significant hyperfine-state mixing, as required for all three transitions to be dipole allowed. The cw line shapes are narrow (30-160 kHz), inhomogeneously broadened by nuclear magnetic interactions, and reveal either a Gaussian or an anomalous second-derivative---like line shape. The spin-echo measurements for the 3H4^{3}H_{4}3H4​ and 1D2^{1}D_{2}1D2​ hyperfine transitions yield homogeneous line shapes which are Lorentzian, and rather surprisingly, linewidths in the narrow range 10-20 kHz, a result which tests current line-broadening theories.
The Raman heterodyne interference phenomenon observed recently in the impurity-ion crystals Pr3+{\mathrm{Pr}}^{3+}Pr3+:YAlO3{\mathrm{YAlO}}_{3}YAlO3​ and Pr3+{\mathrm{Pr}}^{3+}Pr3+:LaF3{\mathrm{LaF}}_{3}LaF3​ is examined from the viewpoint of symmetry analysis of the nonlinear susceptibility tensor. General Raman heterodyne signals are derived for all crystal symmetries and for all optical-frequency and radiofrequency polarizations. An example of the utility of this approach resolves a controversy over the crystal symmetry of LaF3{\mathrm{LaF}}_{3}LaF3​, establishing that it is trigonal rather than hexagonal.
An optical heterodyne technique based on the coherent Raman effect is demonstrated for detecting nuclear magnetic resonances (NMR) and coherent spin transients in normal and optically excited impurity-ion solids at low temperature. Initial measurements on Pr3+{\mathrm{Pr}}^{3+}Pr3+: LaF3{\mathrm{F}}_{3}F3​ provide the first spin-echo studies of an electronically excited state, and cw resonances yield NMR line centers and shapes with kilohertz precision.
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.
An ion is located in a crystal at a site that is not a centre of inversion, with a Zeeman field directed at right angles to the crystal axis c. Periodic intensity variations in the optical spectrum that occur when the crystal is rotated about c are due to magnetic dipole transitions between levels of different type and to electric dipole transitions between levels having admixed opposite-parity parts of different type. Use of an antiunitary operator that commutes with the total Hamiltonian demonstrates that interference between electric and magnetic dipole radiation (or interference between any opposite-parity multipole radiation) does not occur for transitions appearing in the axial spectrum, but does occur for those appearing in the pi or sigma transverse spectrum. Depending on the site symmetry, two or four of the Zeeman components of a doublet-doublet transition have an additional periodicity as a result of this interference. Eigenstates are constructed that show the relationship between the M values of a Zeeman level, the crystal quantum number that labels it, and its type, and are used to calculate the angular dependence of certain doublet-doublet dipole transitions for ions at sites of point symmetries D 2d and C 3h . With explicit expressions for dipole matrix elements, it is discovered that two Zeeman components having the same angular dependence when interference is neglected exhibit dissimilar angular behaviour when the interference cross-term is included.