Photon echo and free induction decay, i.e., representative coherent optical transients, are described for two level system whose transition frequency is modulated by the Gaussian-Markoffian process. Photon echo signal is shown to decay biexponentially and to be effective in fixing the magnitude and the correlation time of the frequency modulation. Then we present the transition of the free induction decay rate against laser intensity from the Bloch type at the weak laser field into the Redfield one at the strong laser field.Photon echo and free induction decay, i.e., representative coherent optical transients, are described for two level system whose transition frequency is modulated by the Gaussian-Markoffian process. Photon echo signal is shown to decay biexponentially and to be effective in fixing the magnitude and the correlation time of the frequency modulation. Then we present the transition of the free induction decay rate against laser intensity from the Bloch type at the weak laser field into the Redfield one at the strong laser field.

Journal of the Physical Society of JapanJun 1, 198379 citations

Multiple phase-coherent laser pulses in optical spectroscopy. II. Applications to multilevel systems

W. S. Warren, Ahmed H. Zewail

The effects of intense laser pulse trains in coupled multilevel systems (such as pure or mixed molecular crystals) are analyzed by calculating exact density matrix evolutions. It is shown that two-level approximations are inadequate. The contributions of exchange couplings, inhomogeneous broadening, permanent multipole interactions and transition multipole interactions to absorption and photon echo line shapes are calculated. The absorption line shape of 1,4-dibromonaphthalene (DBN) is shown to be predominantly an isotopic substitution effect, as our Monte Carlo results give quantitative agreement with experiment for this model. Average t-matrix approximations to the Green’s function, which have been used to propose a different mechanism for the DBN line shape are shown to be qualitatively inadequate. Dipole–dipole interactions are shown to be an important photon echo decay mechanism in mixed crystals, with the relative importance of permanent and transition multipole interactions dependent on the resonance frequency distribution. Multiple pulse trains, including multiple pulse echoes and optical multiple-quantum sequences, are shown to be capable of distinguishing different types of interactions in the molecular Hamiltonian and reducing optical density effects. Specific pulse sequences are proposed and their effects are calculated.The effects of intense laser pulse trains in coupled multilevel systems (such as pure or mixed molecular crystals) are analyzed by calculating exact density matrix evolutions. It is shown that two-level approximations are inadequate. The contributions of exchange couplings, inhomogeneous broadening, permanent multipole interactions and transition multipole interactions to absorption and photon echo line shapes are calculated. The absorption line shape of 1,4-dibromonaphthalene (DBN) is shown to be predominantly an isotopic substitution effect, as our Monte Carlo results give quantitative agreement with experiment for this model. Average t-matrix approximations to the Green’s function, which have been used to propose a different mechanism for the DBN line shape are shown to be qualitatively inadequate. Dipole–dipole interactions are shown to be an important photon echo decay mechanism in mixed crystals, with the relative importance of permanent and transition multipole interactions dependent on the resonance frequency distribution. Multiple pulse trains, including multiple pulse echoes and optical multiple-quantum sequences, are shown to be capable of distinguishing different types of interactions in the molecular Hamiltonian and reducing optical density effects. Specific pulse sequences are proposed and their effects are calculated.

The Journal of Chemical PhysicsMar 1, 198363 citations

Stochastic Optical Signals and Photon Fluctuations

WORLD SCIENTIFIC eBooksJun 1, 20080 citations

Photo Echo and Optical Nutation in Molecules

Richard G. Brewer, R. L. Shoemaker

Photon echo and optical nutation have been easily observed in ${\mathrm{C}}^{13}$ ${\mathrm{H}}_{3}$ F and N ${\mathrm{H}}_{2}$ D by applying Stark pulses which shift the molecular levels into resonance with cw laser radiation. Numerical computations of the nutation effect agree with observation, and echo characteristics closely follow predictions of existing theories. The $T_{2}^{}{}_{}{}^{\ensuremath{'}}$ pressure dependence, from infrared-echo measurements, indicates that ${\mathrm{C}}^{13}$ ${\mathrm{H}}_{3}$ F relaxes primarily by rotational energy transfer.Photon echo and optical nutation have been easily observed in ${\mathrm{C}}^{13}$${\mathrm{H}}_{3}$F and N${\mathrm{H}}_{2}$D by applying Stark pulses which shift the molecular levels into resonance with cw laser radiation. Numerical computations of the nutation effect agree with observation, and echo characteristics closely follow predictions of existing theories. The $T_{2}^{}{}_{}{}^{\ensuremath{'}}$ pressure dependence, from infrared-echo measurements, indicates that ${\mathrm{C}}^{13}$${\mathrm{H}}_{3}$F relaxes primarily by rotational energy transfer.

Physical Review LettersSep 6, 1971338 citations

Photon echo and optical nutation have been easily observed in

{\mathrm{C}}^{13}

{\mathrm{H}}_{3}

F and N

{\mathrm{H}}_{2}

D by applying Stark pulses which shift the molecular levels into resonance with cw laser radiation. Numerical computations of the nutation effect agree with observation, and echo characteristics closely follow predictions of existing theories. The $T_{2}^{}{}_{}{}^{\ensuremath{'}}$ pressure dependence, from infrared-echo measurements, indicates that

{\mathrm{C}}^{13}

{\mathrm{H}}_{3}

F relaxes primarily by rotational energy transfer.