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Physical Review A

Switching of photon-echo polarization and direction by coherent optical fields

K. Leung, THOMAS W. MOSSBERG, Sven R. Hartmann

Published Jan 1, 1984• 4 citations
Publisher

Abstract

We report a novel method for the observation of photon echoes and other coherent transient effects. In this method, the polarization, direction, and frequency of the polarized coherent radiation emitted by a system are switched by optical pulses. We apply this method to detect photon echoes generated on the $6{P}_{\frac{1}{2}}\ensuremath{-}7{S}_{\frac{1}{2}}$ transition in atomic thallium by two collinear and vertically polarized excitation pulses which are separated by 20 nsec. At the time of the echo, two orthogonally polarized probe pulses resonant with the $6{P}_{\frac{3}{2}}\ensuremath{-}7{S}_{\frac{1}{2}}$ transition of atomic thallium are applied to the sample to switch the photon echo from its original polarization and direction. A horizontally polarized photon echo with its propagation vector turned by about 10 mrad and its axis of polarization rotated by 90\ifmmode^\circ\else\textdegree\fi{} is detected. No electro-optical shutter is used in the experiment. The echo signal disappears either when one of the probe pulses is blocked or when both probe pulses are horizontally or vertically polarized. Echo polarization switching is also demonstrated using an unpolarized probe pulse applied prior to the echo formation time.

DOI
10.1103/physreva.29.225

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Polarization rotation of photon echoes in cesium vapor in a magnetic field

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Coherent Transients by Laser-Acoustical Diffraction Spectroscopy

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Recently we have reported[1] on the measurements of electronic dephasing (T_2) and radiationless decay (T_1) in molecules using emission spectroscopy as a probe for the detection of the photon echo. This right-angle photon echo utilizes a single mode of a narrow-band (~MHz) cw dye laser and an intracavity electro-optical (EO) element that modulates the frequency of the laser.[2] Applying voltage pulses into the EO crystal switches the laser frequency from ω_0 (the peak frequency of the transition resonance) into another frequency ω. This switching procedure introduced by Brewer et al. for the observation of transients in the forward direction of the laser allows one to observe coherent transients in gases,[1,2] solids[3-5] and molecular beams.[6] Typically, the dispersion of the nonlinear EO crystal (e.g., AD*P) gives a 60 MHz frequency shift within the inhomogeneous resonance of the optical transition (width ~GHz or larger). Therefore, to switch the laser frequency further, one must use high-voltage signals that are usually hard to obtain especially for multiple-pulse experiments. Secondly, there is a limit on the frequency shift which is conditioned by the mode spacing of the cavity. Thirdly, because the laser is switched into a new group of molecules some complications may arise in interpreting the transient spectra especially in large molecules. This is because in large molecules the density of excited states is high and thus the buildup of transients of w molecules (which could be complex) will be superimposed on the decay of ω_0 molecules. Finally, off-resonance effects (e.g., beats) between the molecules at frequency ω and ω_0 cannot be avoided.

Journal of the Optical Society of America A•May 1, 1978•1 citation

Theoretical study of photon echoes associated with the coherent nonlinear optical effect in a resonant three-level system

M. Aihara, Humio Inaba

An analytical study of the photon echoes associated with the three-level system interacting resonantly with optical pulses possessing two different frequencies is performed. It is predicted that photon echoes arise at anomalous times corresponding to the correlation between the inhomogeneous broadenings for the different spectral lines as well as at the normal time expected in a simple two-level system. This new effect is caused by the coupling of the two resonant transitions through the common energy level. Furthermore, if the particle does not have inversion symmetry, the echoes with the sum or difference frequency of the exciting optical pulses can be observed in such a system. The quantitative analysis is also given for intensities, direction of propagation and polarizations of the anomalous echoes which depend upon the exciting pulses with different frequency.

Journal of Physics A Mathematical Nuclear and General•Nov 1, 1973•21 citations
We report a novel method for the observation of photon echoes and other coherent transient effects. In this method, the polarization, direction, and frequency of the polarized coherent radiation emitted by a system are switched by optical pulses. We apply this method to detect photon echoes generated on the 6P12\ensuremath−7S126{P}_{\frac{1}{2}}\ensuremath{-}7{S}_{\frac{1}{2}}6P21​​\ensuremath−7S21​​ transition in atomic thallium by two collinear and vertically polarized excitation pulses which are separated by 20 nsec. At the time of the echo, two orthogonally polarized probe pulses resonant with the 6P32\ensuremath−7S126{P}_{\frac{3}{2}}\ensuremath{-}7{S}_{\frac{1}{2}}6P23​​\ensuremath−7S21​​ transition of atomic thallium are applied to the sample to switch the photon echo from its original polarization and direction. A horizontally polarized photon echo with its propagation vector turned by about 10 mrad and its axis of polarization rotated by 90\ifmmode^\circ\else\textdegree\fi{} is detected. No electro-optical shutter is used in the experiment. The echo signal disappears either when one of the probe pulses is blocked or when both probe pulses are horizontally or vertically polarized. Echo polarization switching is also demonstrated using an unpolarized probe pulse applied prior to the echo formation time.
We report observations of the rotation of the plane of polarization of photon echoes by a weak axial magnetic field. The echoes are generated on the 6S126{S}_{\frac{1}{2}}6S21​​ to 7P127{P}_{\frac{1}{2}}7P21​​ transition in cesium (4593 \AA{}) by a sequence of two collinear laser pulses polarized in the same direction. When a magnetic field is applied along the propagation axis the polarization vector of the echo is rotated from that of the exciting pulses. We measure the intensity of the photon echo signal polarized orthogonal to the excitation pulse polarization as a function of magnetic field and pulse separation. The theoretical analysis decribes cesium atoms as a nondegenerate multilevel system, consisting of ground and excited Zeeman-split hyperfine-structure levels. The theory presented predicts the observed dependence on magnetic field strength, pulse separation, and excited- and ground-state ggg factors. A novel method of observing photon echoes is described which uses the polarization rotation effect to replace electro-optical shutters often employed in photon echo experiments.
Detailed experimental analysis of photon echo polarization in a longitudinal magnetic field is performed for the first time at the simplest quantum transition J = 1 ↔ J = 0 for which the non-Faraday rotation of photon echo polarization plane was predicted. The echo was generated at the intercombination transition (6s6p) 3P1 → (6s2) 1S0 of 174Yb by two resonant laser pulses of linear (parallel or mutually orthogonal) polarization, and the angled echo optical scheme was applied for the detection. At the magnetic field strength ℬ ⩽ 5 G the photon echo has polarization very close to linear one; its polarization plane rotates around magnetic field vector, and photon echo polarization components and integral echo power oscillate versus ℬ from its maximum value to zero, in agreement with theory. At a stronger magnetic field ℬ ∼ 40 G photon echo power oscillations disappear, no preferable orientation of polarization vector is observed; the fluctuations of exciting radiation spectrum are supposed to be responsible for this "non-polarized" echo.
Coherent transient effects are the optical analogs of the many transient phenomena seen in pulsed nuclear magnetic resonance experiments on spin systems. For example, photon-echo and optical nutation are the respective optical equivalents of spin echo and transient nutation of nuclear magnetic resonance. In Stark-switching and frequency-switching techniques the laser field and the molecules are brought into resonance in a sequence of pulses, the rest of the time they remain well off-resonance. So far it has been assumed that the off-resonance field does not have any measureable influence on the experimental results and is utilized to implement a very efficient detection scheme. This work discusses how the off-resonance field affects the coherent transient effects. It is shown here how this field, by inducing changes in the index of refraction as small as 10⁻⁶ produces easily observable effects in photon echo and delayed optical nutation.
Each of three basic coherent transient phenomena (optical nutation, free polarization decay photon echo) can be generated by sufficiently abrupt modulation of the interaction between the matter and radiation. This can be performed by rapid commutation of either radiation parameters, or the parameters of the matter. I present here comparative analysis of these two approaches (the first one, using electro-optical switching of the resonant laser power to create the pulses for the gas excitation and the second one, based on the Stark switching of vibro-rotational levels in a gas, excited by CW laser radiation), used in our experiments in molecular gases, from the point of view of both their capability to generate various coherent transients and their sensitivity to the intensity of laser radiation.
Recently we have reported[1] on the measurements of electronic dephasing (T_2) and radiationless decay (T_1) in molecules using emission spectroscopy as a probe for the detection of the photon echo. This right-angle photon echo utilizes a single mode of a narrow-band (~MHz) cw dye laser and an intracavity electro-optical (EO) element that modulates the frequency of the laser.[2] Applying voltage pulses into the EO crystal switches the laser frequency from ω_0 (the peak frequency of the transition resonance) into another frequency ω. This switching procedure introduced by Brewer et al. for the observation of transients in the forward direction of the laser allows one to observe coherent transients in gases,[1,2] solids[3-5] and molecular beams.[6] Typically, the dispersion of the nonlinear EO crystal (e.g., AD*P) gives a 60 MHz frequency shift within the inhomogeneous resonance of the optical transition (width ~GHz or larger). Therefore, to switch the laser frequency further, one must use high-voltage signals that are usually hard to obtain especially for multiple-pulse experiments. Secondly, there is a limit on the frequency shift which is conditioned by the mode spacing of the cavity. Thirdly, because the laser is switched into a new group of molecules some complications may arise in interpreting the transient spectra especially in large molecules. This is because in large molecules the density of excited states is high and thus the buildup of transients of w molecules (which could be complex) will be superimposed on the decay of ω_0 molecules. Finally, off-resonance effects (e.g., beats) between the molecules at frequency ω and ω_0 cannot be avoided.
An analytical study of the photon echoes associated with the three-level system interacting resonantly with optical pulses possessing two different frequencies is performed. It is predicted that photon echoes arise at anomalous times corresponding to the correlation between the inhomogeneous broadenings for the different spectral lines as well as at the normal time expected in a simple two-level system. This new effect is caused by the coupling of the two resonant transitions through the common energy level. Furthermore, if the particle does not have inversion symmetry, the echoes with the sum or difference frequency of the exciting optical pulses can be observed in such a system. The quantitative analysis is also given for intensities, direction of propagation and polarizations of the anomalous echoes which depend upon the exciting pulses with different frequency.