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Quantum Electronics and Laser Science Conference

Higher-order collision enhanced wave mixing; theory and experiment

Rick P. Trebino, Larry A. Rahn

Published Apr 24, 1989• 0 citations
OpenAlex

Abstract

Collision enhanced resonances represent an interesting class of nonlinear-optical processes. They occur because collisional dephasing can rephase quantum mechanical amplitudes that ordinarily cancel out exactly, thereby allowing otherwise unobservable wave-mixing resonances to be seen. This is an especially interesting phenomenon because these resonances are coherent effects that are induced by an incoherent process (collisional dephasing). First predicted1 in the late 1970s and eventually observed2 in 1981, these novel effects have now been seen in a wide variety of four-wave-mixing experiments, ranging from self-focusing to coherent anti-Stokes Raman spectroscopy.

Related papers

Collisionally induced phenomena in nonlinear optics

E. Giacobino, P. R. Berman, M. Pinard +1 more

Collisional perturbation of atoms in a vapor is well known to induce additional resonances in degenerate or nearly degenerate four-wave mixing.1,2 Actually the effect of collisions in nonlinear optics includes a much broader class of phenomenon, in which the dephasing of the wave functions during the collisions modifies the response of the medium to the input waves. Two examples of such effects are described: coherent emission of radiation induced by collisions and collisionally aided amplification.

Journal of the Optical Society of America B•Jan 1, 1986•0 citations

Observation of Higher-Order Dephasing-Induced Coherences in a Flame in a Magnetic Field

Rick P. Trebino, Larry A. Rahn

Dephasieg-induced phenomena are a novel class of effects that are ordinarily forbidden because the two or more relevant quantum-mechanical amplitudes add coherently and cancel out.1 When dephasing is present, however, these amplitudes no longer cancel, and previously unseen effects can be observed. Indeed, a number of novel dephasing-induced phenomena have been seen.2-5 Of particular interest, both for fundamental reasons and for diagnostic purposes, are (third-order) dephasing-induced resonances between equally populated levels of a ground electronic state,6,7 specifically, Zeeman and hyperfine coherences. Working with a sodium-seeded flame, we8 have observed these latter effects and, at higher intensities, subharmonics of them.

•Jul 18, 1988•1 citation

Time-Delayed Four-Wave Mixing: The Interplay Between Iaser Field Fluctuations and the Atomic Memory Time

J.V. Gomes, Michael Scott Belsley, M. Kaczmarck +1 more

Coherent signals induced by fundamentally incoherent phenomena through a four-wave mixing process are among the most intriguing and subtle effects in nonlinear spectroscopy. These effects were initially observed by Bloembergen and his co-workers in the form of pressure-induced extra resonances in four-wave mixing. Using standard perturbance techniques based on the optical Bloch equations, they suggested that these collision induced resonances were the result of a destruction of the destructive interference existent between two alternate time-ordered pathways. Subsequently, Prior et al realised that fluctuations in the incident radiation fields could play essentially the same role as the collisionally induced dephasing. In practice, of course, both collisional dephasing and field fluctuations are present in a typical atomic vapor pulsed four-wave mixing experiment. If the timescales governing these two effects approach one another, one can expect to gain valuable new insight into this fascinating process of incoherently inducing a coherent signal

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Nonlinear optical processes are strongly dominated by phase relationships among electromagnetic fields involved. In this paper, we theoretically and experimentally show that in a Raman-resonant four-wave-mixing process, the first anti-Stokes and Stokes generations can be tailored in a variety of ways by manipulating the phase relationships among the relevant electromagnetic fields.

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Nonlinear Optical Processes With Incoherent Light And Their Applications For Studies Of Ultrafast Dephasing

Peixian Ye

In recent years, a series of nonlinear optical processes with incoherent light, such as time-delay four-wave mixing, optical Kerr effect and coherent Stokes Raman scattering, were developed and attracted much attention. It has been demonstrated that these processes can be used to measure the ultrafast dephasing times of excitations (shorter than 1 psec.) with nanosecond pulse lasers or even CW lasers. In this talk, after a short review of the works done by others previously theoretical and experimental investigations in this field in my laboratory are presented.

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Multiple resonance-enhanced four-wave-mixing processes in I2

Ilse Aben, Wim Ubachs, Pieternel Felicitas Levelt +2 more

Resonance-enhanced four-wave-mixing processes were studied in molecular iodine by detection of a wave generated at frequency ${\mathrm{\ensuremath{\omega}}}_{3}$=2${\mathrm{\ensuremath{\omega}}}_{1}$-${\mathrm{\ensuremath{\omega}}}_{2}$ for a wide range of Raman frequencies (${\mathrm{\ensuremath{\omega}}}_{1}$-${\mathrm{\ensuremath{\omega}}}_{2}$). On the basis of known spectroscopic constants of the two electronic states involved, the electronic ground state ${\mathit{X}}^{1}$${\mathrm{\ensuremath{\Sigma}}}_{\mathit{g}}^{+}$ and the electronic excited state ${\mathit{B}}^{3}$${\mathrm{\ensuremath{\Pi}}}_{\mathit{u}0}^{+}$, an interpretation of the spectral features in terms of three essentially different four-wave-mixing processes is given. Resonance enhancement through bound states with discrete energy levels and the enhancement effect by dissociative continuum states are considered. In addition to resonance-enhanced coherent anti-Stokes Raman-scattering (CARS) processes, in which the Raman resonances are in the electronic ground state, two resonant schemes are identified in ${\mathrm{I}}_{2}$, in which Raman resonances in an excited state are probed: excited-state parametric and nonparametric CARS. The latter process is an example of electronic population transfer in a four-wave-mixing cycle.

Physical Review A•Nov 1, 1991•11 citations
Collision enhanced resonances represent an interesting class of nonlinear-optical processes. They occur because collisional dephasing can rephase quantum mechanical amplitudes that ordinarily cancel out exactly, thereby allowing otherwise unobservable wave-mixing resonances to be seen. This is an especially interesting phenomenon because these resonances are coherent effects that are induced by an incoherent process (collisional dephasing). First predicted1 in the late 1970s and eventually observed2 in 1981, these novel effects have now been seen in a wide variety of four-wave-mixing experiments, ranging from self-focusing to coherent anti-Stokes Raman spectroscopy.
Collisional perturbation of atoms in a vapor is well known to induce additional resonances in degenerate or nearly degenerate four-wave mixing.1,2 Actually the effect of collisions in nonlinear optics includes a much broader class of phenomenon, in which the dephasing of the wave functions during the collisions modifies the response of the medium to the input waves. Two examples of such effects are described: coherent emission of radiation induced by collisions and collisionally aided amplification.
Dephasieg-induced phenomena are a novel class of effects that are ordinarily forbidden because the two or more relevant quantum-mechanical amplitudes add coherently and cancel out.1 When dephasing is present, however, these amplitudes no longer cancel, and previously unseen effects can be observed. Indeed, a number of novel dephasing-induced phenomena have been seen.2-5 Of particular interest, both for fundamental reasons and for diagnostic purposes, are (third-order) dephasing-induced resonances between equally populated levels of a ground electronic state,6,7 specifically, Zeeman and hyperfine coherences. Working with a sodium-seeded flame, we8 have observed these latter effects and, at higher intensities, subharmonics of them.
Coherent signals induced by fundamentally incoherent phenomena through a four-wave mixing process are among the most intriguing and subtle effects in nonlinear spectroscopy. These effects were initially observed by Bloembergen and his co-workers in the form of pressure-induced extra resonances in four-wave mixing. Using standard perturbance techniques based on the optical Bloch equations, they suggested that these collision induced resonances were the result of a destruction of the destructive interference existent between two alternate time-ordered pathways. Subsequently, Prior et al realised that fluctuations in the incident radiation fields could play essentially the same role as the collisionally induced dephasing. In practice, of course, both collisional dephasing and field fluctuations are present in a typical atomic vapor pulsed four-wave mixing experiment. If the timescales governing these two effects approach one another, one can expect to gain valuable new insight into this fascinating process of incoherently inducing a coherent signal
In recent years, a series of nonlinear optical processes with incoherent light, such as time-delay four-wave mixing, optical Kerr effect and coherent Stokes Raman scattering, were developed and attracted much attention. It has been demonstrated that these processes can be used to measure the ultrafast dephasing times of excitations (shorter than 1 psec.) with nanosecond pulse lasers or even CW lasers. In this talk, after a short review of the works done by others previously theoretical and experimental investigations in this field in my laboratory are presented.
Resonance-enhanced four-wave-mixing processes were studied in molecular iodine by detection of a wave generated at frequency ${\mathrm{\ensuremath{\omega}}}_{3}$=2${\mathrm{\ensuremath{\omega}}}_{1}$-${\mathrm{\ensuremath{\omega}}}_{2}$ for a wide range of Raman frequencies (${\mathrm{\ensuremath{\omega}}}_{1}$-${\mathrm{\ensuremath{\omega}}}_{2}$). On the basis of known spectroscopic constants of the two electronic states involved, the electronic ground state X1{\mathit{X}}^{1}X1${\mathrm{\ensuremath{\Sigma}}}_{\mathit{g}}^{+}$ and the electronic excited state B3{\mathit{B}}^{3}B3${\mathrm{\ensuremath{\Pi}}}_{\mathit{u}0}^{+}$, an interpretation of the spectral features in terms of three essentially different four-wave-mixing processes is given. Resonance enhancement through bound states with discrete energy levels and the enhancement effect by dissociative continuum states are considered. In addition to resonance-enhanced coherent anti-Stokes Raman-scattering (CARS) processes, in which the Raman resonances are in the electronic ground state, two resonant schemes are identified in I2{\mathrm{I}}_{2}I2​, in which Raman resonances in an excited state are probed: excited-state parametric and nonparametric CARS. The latter process is an example of electronic population transfer in a four-wave-mixing cycle.