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Physics Letters A

Nuclear “anti-stokes” transitions induced by laser radiation

B. Arad, S. Eliezer, Y. Paiss

Published Dec 1, 1979• 23 citations
Publisher
DOI
10.1016/0375-9601(79)90234-2

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Generation of Stokes and Anti-Stokes Radiation in Raman Media

H. A. Haus, Paul L. Kelley, Herbert J. Zeiger

A three-dimensional analysis of stimulated Raman emission is presented for a medium through which a cylindrical laser beam passes. The buildup of the Stokes radiation from the spontaneous fluctuations in the Raman medium is considered. A generalization of the fluctuation-dissipation theorem is derived relating the current-current fluctuations at the Stokes frequency to the laser-induced (negative) conductance at this frequency. The anti-Stokes radiation is treated as arising from the interaction of the laser field and the molecular vibrations accompanying the Stokes radiation. The anti-Stokes radiation emerges in a narrow cone around the familiar phase-matching direction given by ${\mathbf{\ensuremath{\beta}}}_{\ensuremath{-}}=2{\mathbf{k}}_{L}\ensuremath{-}{\mathbf{\ensuremath{\beta}}}_{+}$, where ${\mathbf{\ensuremath{\beta}}}_{\ensuremath{-}}$ and ${\mathbf{\ensuremath{\beta}}}_{+}$ are the (real parts of the) propagation constants of Stokes and anti-Stokes waves in the medium, and ${\mathbf{k}}_{L}$ is the laser propagation vector. The angular width of the anti-Stokes radiation cone is evaluated.

Physical Review•May 17, 1965•11 citations

Theory of the Stimulated Raman and Related Effects

A. David Buckingham

A simple description of the stimulated Raman emission of Stokes radiation, and of the induced absorption found by Stoicheff at the anti-Stokes frequency, is based on the semiclassical theory of radiation. This theory gives the well-known formulas for absorption and stimulated emission when carried to the first order in the time-dependent perturbation due to the interaction of the light beam with the molecules. If there are two light beams of frequencies ωL and ω, the second-order perturbation may be associated with stimulated emission at the Stokes frequency ω=ω−1=ωL—ωR and with induced absorption at the anti-Stokes frequency ω=ω1=ωL+ωR, where ωL is the laser frequency and ωR a Raman-active vibrational frequency; in both cases, there is a molecular transition to the excited vibrational state. The highly directional and very sharp anti-Stokes emission at ω1 arises from the conversion by molecules in intense beams at ωL and ω−1 of two ωL photons into an ω−1, ω1 pair. Like spontaneous emission from excited states, the production of this anti-Stokes radiation requires the full quantum theory of radiation for an adequate description. The emission of ω1 and the observed directional absorption of ω−1 due to the reverse conversion ω−1+ω1→2ωL are explained. The anti-Stokes emission is proportional to the Stokes intensity and to the square of that of the laser, and to the square of the molecular number density; its sharpness is due to the absence of a molecular transition. The generation of photon pairs ω−n+ωn, where ωn=ωL+nωR, can occur for all values of n, but it is most efficient for n=1, due to resonance in the appropriate molecular hyperpolarizability and to the intensity of the Stokes beam at ω−1.

The Journal of Chemical Physics•Jul 1, 1965•24 citations
A three-dimensional analysis of stimulated Raman emission is presented for a medium through which a cylindrical laser beam passes. The buildup of the Stokes radiation from the spontaneous fluctuations in the Raman medium is considered. A generalization of the fluctuation-dissipation theorem is derived relating the current-current fluctuations at the Stokes frequency to the laser-induced (negative) conductance at this frequency. The anti-Stokes radiation is treated as arising from the interaction of the laser field and the molecular vibrations accompanying the Stokes radiation. The anti-Stokes radiation emerges in a narrow cone around the familiar phase-matching direction given by ${\mathbf{\ensuremath{\beta}}}_{\ensuremath{-}}=2{\mathbf{k}}_{L}\ensuremath{-}{\mathbf{\ensuremath{\beta}}}_{+}$, where ${\mathbf{\ensuremath{\beta}}}_{\ensuremath{-}}$ and ${\mathbf{\ensuremath{\beta}}}_{+}$ are the (real parts of the) propagation constants of Stokes and anti-Stokes waves in the medium, and kL{\mathbf{k}}_{L}kL​ is the laser propagation vector. The angular width of the anti-Stokes radiation cone is evaluated.
A simple description of the stimulated Raman emission of Stokes radiation, and of the induced absorption found by Stoicheff at the anti-Stokes frequency, is based on the semiclassical theory of radiation. This theory gives the well-known formulas for absorption and stimulated emission when carried to the first order in the time-dependent perturbation due to the interaction of the light beam with the molecules. If there are two light beams of frequencies ωL and ω, the second-order perturbation may be associated with stimulated emission at the Stokes frequency ω=ω−1=ωL—ωR and with induced absorption at the anti-Stokes frequency ω=ω1=ωL+ωR, where ωL is the laser frequency and ωR a Raman-active vibrational frequency; in both cases, there is a molecular transition to the excited vibrational state. The highly directional and very sharp anti-Stokes emission at ω1 arises from the conversion by molecules in intense beams at ωL and ω−1 of two ωL photons into an ω−1, ω1 pair. Like spontaneous emission from excited states, the production of this anti-Stokes radiation requires the full quantum theory of radiation for an adequate description. The emission of ω1 and the observed directional absorption of ω−1 due to the reverse conversion ω−1+ω1→2ωL are explained. The anti-Stokes emission is proportional to the Stokes intensity and to the square of that of the laser, and to the square of the molecular number density; its sharpness is due to the absence of a molecular transition. The generation of photon pairs ω−n+ωn, where ωn=ωL+nωR, can occur for all values of n, but it is most efficient for n=1, due to resonance in the appropriate molecular hyperpolarizability and to the intensity of the Stokes beam at ω−1.