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 A

Theory of two-photon multiwave mixing

Murray Sargent, Shlomo Ovadia, Mao Hong Lu

Published Sep 1, 1985• 24 citations
Publisher

Abstract

Steady-state interactions of one, two, and three waves with two-photon two-level media are treated semiclassically. Dynamic Stark shifts as well as dynamic Stark splittings are included in the theory. The intermediate levels are assumed to be nonresonant, and one wave is allowed to have arbitrarily large intensity. The theory parallels the one-photon theory of multiwave mixing couched in terms of population pulsations. We find the one-, two-, and three-wave two-photon absorption coefficients and the three-wave coupling coefficients. We find similarities and significant differences between the one- and two-photon polarizations of the medium. The work treats two-photon saturation spectroscopy, laser- and optical-bistability instabilities, and phase conjugation with a unified formalism.

DOI
10.1103/physreva.32.1596

Related papers

Theory of two-photon multiwave mixing

Shlomo Ovadia, Murray Sargent, Mao Hong Lu

Two-photon transitions have provided the basis for numerous useful nonlinear interactions with radiation. In this paper we calculate the absorption and coupling coefficients for one-, two-, and three-wave mixing in two-photon homogeneously broadened media. The resulting field equations form the basis for understanding saturation spectroscopy, phase conjugation,1 and single-mode instabilities2 in lasers and optical bistability in two-photon media. We assume that the wave frequencies are not resonant with any intermediate state j and that the probe and conjugate waves cannot saturate the two-photon transition. This allows us to use the two-photon two-level model and to transfer much of our knowledge of the one-photon two-level systems to the two-photon case. Two major differences occur between the two models. First, dynamic Stark shifts of the active levels play an important role in generating asymmetric spectra and nonzero dispersion (≃ω s T1) at line center. Second, high pump intensities do not bleach the absorption coefficient at the Rabi sidebands.

Annual Meeting Optical Society of America•Jan 1, 1985•0 citations

Quantum theory of multiwave mixing in two-photon two-level media

David A. Holm, Murray Sargent

Multiphoton transitions are of great interest in laser spectroscopy because they permit the study of new physical phenomena and because of their potential applications. Malcuit et al.1 studied two-photon transitions in atomic sodium and showed that for appropriate phase-matching four-wave mixing can overcome the usual spontaneous decay processes. We have recently developed a quantum theory2 to treat such multiwave mixing processes in two-photon media. Because of the greater complexity of two-photon transitions, many effects arise that are absent in the one-photon case, some of which have important consequences in the generation of squeezed states. For the two-photon two-level model, the field modes have frequencies approximately one-half the frequency difference between the levels. We find that our coefficients differ from the corresponding one-photon theory in that dynamic Stark shifts have a major effect and that the pump-induced coherence between the two levels has a new term in the conjugate coupling terms, which leads to improved squeezing.

Annual Meeting Optical Society of America•Jan 1, 1986•0 citations

QUANTUM THEORY OF MULTIWAVE MIXING (RESONANCE FLUORESCENCE, SATURATION SPECTROSCOPY, MODULATION, PHASE CONJUGATION, QUANTUM NOISE).

David A. Holm

This dissertation formulates and applies a theory describing how one or two strong classical waves and one or two weak quantum mechanical waves interact in a two-level medium. The theory unifies many topics in quantum optics, such as resonance fluorescence, saturation spectroscopy, modulation spectroscopy, the build up of laser and optical bistability instabilities, and phase conjugation. The theory is based on a quantum population pulsation approach that resembles the semiclassical theories, but is substantially more detailed. Calculations are performed to include the effects of inhomogeneous broadening, spatial hole burning, and Gaussian transverse variations. The resonance fluorescence spectrum in a high finesse optical cavity is analyzed in detail, demonstrating how stimulated emission and multiwave processes alter the spectrum from the usual three peaks. The effects of quantum noise during the propagation of weak signal and conjugate fields in phase conjugation and modulation spectroscopy are studied. Our analysis demonstrates that quantum noise affects not only the intensities of the signal and conjugate, but also their relative phase, and in particular we determine a quantum limit to the semiclassical theory of FM modulation spectroscopy. Finally, we derive the corresponding theory for the two-photon, two-level medium. This yields the first calculation of the two-photon resonance fluorescence spectrum. Because of the greater number of possible interactions in the two-photon two-level model, the theoretical formalism is considerably more complex, and many effects arise that are absent in the one-photon problem. We discuss the role of the Stark shifts on the emission spectrum and show how the Rayleigh scattering is markedly different.

•Jan 1, 1985•0 citations

Nondegenerate two-photon phase conjugation

Barbara A. Capron, Murray Sargent

Our semiclassical theory of two-photon multiwave mixing1 is a generalization of the degenerate four-wave mixing case2 to treat nondegenerate pump/signal/conjugate frequencies. We apply that theory to four-wave mixing in two-photon media. We present explicit formulas for the nondegenerate signal/conjugate absorption and coupling coefficients for cases for which the two-photon Stark shifts are sufficiently small compared to the homogeneous linewidths. More general cases require that the spatial hole burning averages be performed numerically. We find intricate dependencies of the transmission and reflection spectra on the pump intensity and on dynamic Stark shifts. In particular, the reflection coefficients do not necessarily bleach to zero as the pump intensity is increased indefinitely, and interferences occur between pure index and mixed absorption/index contributions

Annual Meeting Optical Society of America•Jan 1, 1987•1 citation

Quantum theory of multiwave mixing. V. Two-photon two-level model

David A. Holm, Murray Sargent

We extend our theoretical formalism describing how one strong classical wave and one or two weak quantum-mechanical waves interact in a nonlinear medium to the ``two-photon two-level'' model. In this model, field transitions between two levels not connected by an electric dipole occur by means of a two-photon transition using off-resonant intermediate levels. This model has many similarities with, as well as significant differences from, the corresponding one-photon two-level model that has been treated in the previous papers in this series. The theory yields the first detailed calculation of the two-photon resonance fluorescence spectrum, as well as the complete set of four coefficients that describe the quantum theory of two-, three-, and four-wave mixing.

Physical Review A•Feb 1, 1986•19 citations

Polarization properties of optical phase conjugation by two-photon resonant degenerate four-wave mixing

Martti Olavi Kauranen, Daniel J. Gauthier, Michelle S. Malcuit +1 more

We develop a semiclassical theory of the polarization properties of phase conjugation by two-photon resonant degenerate four-wave mixing. The theory includes the effects of saturation by the pump waves. We solve the density-matrix equations of motion in steady state for a nonlinear medium consisting of stationary atoms with a ground and excited state connected by two-photon transitions. As an illustration of the general results, we consider an ${S}_{0}$\ensuremath{\rightarrow}${S}_{0}$ two-photon transition, which is known to lead to perfect polarization conjugation in the limit of third-order theory. We show that the fidelity of the polarization-conjugation process is degraded for excessively large pump intensities. The degradation can occur both due to transfer of population to the excited state and due to nonresonant Stark shifts. Theoretical results are compared to those of a recent experiment [Malcuit, Gauthier, and Boyd, Opt. Lett. 13, 663 (1988)].

Physical Review A•Aug 1, 1989•13 citations
Steady-state interactions of one, two, and three waves with two-photon two-level media are treated semiclassically. Dynamic Stark shifts as well as dynamic Stark splittings are included in the theory. The intermediate levels are assumed to be nonresonant, and one wave is allowed to have arbitrarily large intensity. The theory parallels the one-photon theory of multiwave mixing couched in terms of population pulsations. We find the one-, two-, and three-wave two-photon absorption coefficients and the three-wave coupling coefficients. We find similarities and significant differences between the one- and two-photon polarizations of the medium. The work treats two-photon saturation spectroscopy, laser- and optical-bistability instabilities, and phase conjugation with a unified formalism.
Two-photon transitions have provided the basis for numerous useful nonlinear interactions with radiation. In this paper we calculate the absorption and coupling coefficients for one-, two-, and three-wave mixing in two-photon homogeneously broadened media. The resulting field equations form the basis for understanding saturation spectroscopy, phase conjugation,1 and single-mode instabilities2 in lasers and optical bistability in two-photon media. We assume that the wave frequencies are not resonant with any intermediate state j and that the probe and conjugate waves cannot saturate the two-photon transition. This allows us to use the two-photon two-level model and to transfer much of our knowledge of the one-photon two-level systems to the two-photon case. Two major differences occur between the two models. First, dynamic Stark shifts of the active levels play an important role in generating asymmetric spectra and nonzero dispersion (≃ω s T1) at line center. Second, high pump intensities do not bleach the absorption coefficient at the Rabi sidebands.
Multiphoton transitions are of great interest in laser spectroscopy because they permit the study of new physical phenomena and because of their potential applications. Malcuit et al.1 studied two-photon transitions in atomic sodium and showed that for appropriate phase-matching four-wave mixing can overcome the usual spontaneous decay processes. We have recently developed a quantum theory2 to treat such multiwave mixing processes in two-photon media. Because of the greater complexity of two-photon transitions, many effects arise that are absent in the one-photon case, some of which have important consequences in the generation of squeezed states. For the two-photon two-level model, the field modes have frequencies approximately one-half the frequency difference between the levels. We find that our coefficients differ from the corresponding one-photon theory in that dynamic Stark shifts have a major effect and that the pump-induced coherence between the two levels has a new term in the conjugate coupling terms, which leads to improved squeezing.
This dissertation formulates and applies a theory describing how one or two strong classical waves and one or two weak quantum mechanical waves interact in a two-level medium. The theory unifies many topics in quantum optics, such as resonance fluorescence, saturation spectroscopy, modulation spectroscopy, the build up of laser and optical bistability instabilities, and phase conjugation. The theory is based on a quantum population pulsation approach that resembles the semiclassical theories, but is substantially more detailed. Calculations are performed to include the effects of inhomogeneous broadening, spatial hole burning, and Gaussian transverse variations. The resonance fluorescence spectrum in a high finesse optical cavity is analyzed in detail, demonstrating how stimulated emission and multiwave processes alter the spectrum from the usual three peaks. The effects of quantum noise during the propagation of weak signal and conjugate fields in phase conjugation and modulation spectroscopy are studied. Our analysis demonstrates that quantum noise affects not only the intensities of the signal and conjugate, but also their relative phase, and in particular we determine a quantum limit to the semiclassical theory of FM modulation spectroscopy. Finally, we derive the corresponding theory for the two-photon, two-level medium. This yields the first calculation of the two-photon resonance fluorescence spectrum. Because of the greater number of possible interactions in the two-photon two-level model, the theoretical formalism is considerably more complex, and many effects arise that are absent in the one-photon problem. We discuss the role of the Stark shifts on the emission spectrum and show how the Rayleigh scattering is markedly different.
Our semiclassical theory of two-photon multiwave mixing1 is a generalization of the degenerate four-wave mixing case2 to treat nondegenerate pump/signal/conjugate frequencies. We apply that theory to four-wave mixing in two-photon media. We present explicit formulas for the nondegenerate signal/conjugate absorption and coupling coefficients for cases for which the two-photon Stark shifts are sufficiently small compared to the homogeneous linewidths. More general cases require that the spatial hole burning averages be performed numerically. We find intricate dependencies of the transmission and reflection spectra on the pump intensity and on dynamic Stark shifts. In particular, the reflection coefficients do not necessarily bleach to zero as the pump intensity is increased indefinitely, and interferences occur between pure index and mixed absorption/index contributions
We extend our theoretical formalism describing how one strong classical wave and one or two weak quantum-mechanical waves interact in a nonlinear medium to the ``two-photon two-level'' model. In this model, field transitions between two levels not connected by an electric dipole occur by means of a two-photon transition using off-resonant intermediate levels. This model has many similarities with, as well as significant differences from, the corresponding one-photon two-level model that has been treated in the previous papers in this series. The theory yields the first detailed calculation of the two-photon resonance fluorescence spectrum, as well as the complete set of four coefficients that describe the quantum theory of two-, three-, and four-wave mixing.
We develop a semiclassical theory of the polarization properties of phase conjugation by two-photon resonant degenerate four-wave mixing. The theory includes the effects of saturation by the pump waves. We solve the density-matrix equations of motion in steady state for a nonlinear medium consisting of stationary atoms with a ground and excited state connected by two-photon transitions. As an illustration of the general results, we consider an S0{S}_{0}S0​\ensuremath{\rightarrow}S0{S}_{0}S0​ two-photon transition, which is known to lead to perfect polarization conjugation in the limit of third-order theory. We show that the fidelity of the polarization-conjugation process is degraded for excessively large pump intensities. The degradation can occur both due to transfer of population to the excited state and due to nonresonant Stark shifts. Theoretical results are compared to those of a recent experiment [Malcuit, Gauthier, and Boyd, Opt. Lett. 13, 663 (1988)].