Three-photon Molecular Scattering of Light

A review is given of experimental and theoretical achievements in studies of multiphoton spontaneous scattering processes in atomic and molecular media. An analysis is made of integral multiphoton scattering, particularly of scattering in statistically inhomogeneous media with short-range quasiorder. A study of the intensity of the noncoherent multiphoton scattering component provides direct information on the nonlinear polarizability of atoms and molecules whilst the coherent component is associated with various atomic and molecular correlation mechanisms. An analysis of the spectra of elastic and inelastic multiphoton scattering processes yields information on the translational and rotational motion of the molecules. In particular, it is possible to measure the higher-order rotational relaxation times and to verify the adequacy of the various stochastic models of molecular motion. Observations of the spectral lines of three- or more-photon scattering, which obeys new selection rules, yield detail on the fine structure of the molecules and their linear and nonlinear vibrations. Examples are given of the most interesting spectra of three- or more-photon scattering in gases, liquids, and crystals obtained in singleand multichannel systems. The stochastic theory of multiphoton scattering in liquids is discussed, using the spherical tensor concept. The derived general expression reduces to known results for certain cases.A review is given of experimental and theoretical achievements in studies of multiphoton spontaneous scattering processes in atomic and molecular media. An analysis is made of integral multiphoton scattering, particularly of scattering in statistically inhomogeneous media with short-range quasiorder. A study of the intensity of the noncoherent multiphoton scattering component provides direct information on the nonlinear polarizability of atoms and molecules whilst the coherent component is associated with various atomic and molecular correlation mechanisms. An analysis of the spectra of elastic and inelastic multiphoton scattering processes yields information on the translational and rotational motion of the molecules. In particular, it is possible to measure the higher-order rotational relaxation times and to verify the adequacy of the various stochastic models of molecular motion. Observations of the spectral lines of three- or more-photon scattering, which obeys new selection rules, yield detail on the fine structure of the molecules and their linear and nonlinear vibrations. Examples are given of the most interesting spectra of three- or more-photon scattering in gases, liquids, and crystals obtained in singleand multichannel systems. The stochastic theory of multiphoton scattering in liquids is discussed, using the spherical tensor concept. The derived general expression reduces to known results for certain cases.

Soviet Journal of Quantum ElectronicsDec 31, 19770 citations

Multiphoton resonance in a three-level system with nearly degenerate excited states

Michał Berent, R. Parzyński

An analytic study is presented of the efficient multiphoton excitation and strong harmonic generation in three-level systems specified by a pair of nearly degenerate, strongly dipole-coupled excited states. Such systems are physically formed by the three lowest states in, e.g., the hydrogen atom or evenly charged homonuclear diatomic molecular ions under reasonably chosen laser intensities. As a detailed analytic result, we found that the laser pulse of photon energy $2.05\text{eV}$ , duration $0.23\text{ps}$ , and intensity $5\ifmmode\times\else\texttimes\fi{}{10}^{13}\frac{\mathrm{W}}{{\mathrm{cm}}^{2}}$ is able to produce complete inversion of the initial population in the hydrogen atom through the five-photon excitation. At the same photon energy, the pulse of duration $0.41\text{ps}$ and intensity $3.44\ifmmode\times\else\texttimes\fi{}{10}^{14}\frac{\mathrm{W}}{{\mathrm{cm}}^{2}}$ was found to produce the same effect in the molecular ion but through the nine-photon excitation. We show that the accompanying scattering of light has very rich spectrum differing substantially from that of the two-level system.An analytic study is presented of the efficient multiphoton excitation and strong harmonic generation in three-level systems specified by a pair of nearly degenerate, strongly dipole-coupled excited states. Such systems are physically formed by the three lowest states in, e.g., the hydrogen atom or evenly charged homonuclear diatomic molecular ions under reasonably chosen laser intensities. As a detailed analytic result, we found that the laser pulse of photon energy $2.05\text{eV}$, duration $0.23\text{ps}$, and intensity $5\ifmmode\times\else\texttimes\fi{}{10}^{13}\frac{\mathrm{W}}{{\mathrm{cm}}^{2}}$ is able to produce complete inversion of the initial population in the hydrogen atom through the five-photon excitation. At the same photon energy, the pulse of duration $0.41\text{ps}$ and intensity $3.44\ifmmode\times\else\texttimes\fi{}{10}^{14}\frac{\mathrm{W}}{{\mathrm{cm}}^{2}}$ was found to produce the same effect in the molecular ion but through the nine-photon excitation. We show that the accompanying scattering of light has very rich spectrum differing substantially from that of the two-level system.

arXiv:1007.0371Physical Review AAug 10, 20106 citations

Lifetimes for resonance fluorescence and near resonance Raman scattering

Shaul Mukamel, Joshua Jortner

In this paper we present a quantum mechanical treatment of time resolved resonant and near resonant light scattering from a molecular system. The time resolved decay pattern is characterized by just two types of lifetimes, those specifying the molecular system and those characterizing the light pulse, while the off resonance energy parameter affects the total intensity and, in some cases, the relative intensities of the different decay components. The theoretical results for the ’’isolated’’ molecule are confronted with the recent experimental data of Williams, Rousseau, and Dworetzky [Phys. Rev. Lett. 32, 196 (1974)] for resonance and near resonance photon scattering from I2. Finally, we present a general scheme for handling photon scattering from a multilevel molecular system.In this paper we present a quantum mechanical treatment of time resolved resonant and near resonant light scattering from a molecular system. The time resolved decay pattern is characterized by just two types of lifetimes, those specifying the molecular system and those characterizing the light pulse, while the off resonance energy parameter affects the total intensity and, in some cases, the relative intensities of the different decay components. The theoretical results for the ’’isolated’’ molecule are confronted with the recent experimental data of Williams, Rousseau, and Dworetzky [Phys. Rev. Lett. 32, 196 (1974)] for resonance and near resonance photon scattering from I2. Finally, we present a general scheme for handling photon scattering from a multilevel molecular system.

The Journal of Chemical PhysicsMay 1, 197595 citations

2.05\text{eV}

, duration

0.23\text{ps}

, and intensity $5\ifmmode\times\else\texttimes\fi{}{10}^{13}\frac{\mathrm{W}}{{\mathrm{cm}}^{2}}$ is able to produce complete inversion of the initial population in the hydrogen atom through the five-photon excitation. At the same photon energy, the pulse of duration

0.41\text{ps}

and intensity $3.44\ifmmode\times\else\texttimes\fi{}{10}^{14}\frac{\mathrm{W}}{{\mathrm{cm}}^{2}}$ was found to produce the same effect in the molecular ion but through the nine-photon excitation. We show that the accompanying scattering of light has very rich spectrum differing substantially from that of the two-level system.