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The Review of Laser Engineering

Polarization Properties of the Photon Echo in Solids

T. Kohmoto, M. Nido, Yukio Fukuda, Masahiro Matsuoka

Published Jan 1, 1982• 1 citation
Publisher

Abstract

The behavior of the photon-echo polarization in solids is discussed. The photon echo in La F3: Pr3+ is considered in some details as a typical example. The echo is induced by linearly polarized pulses propagating along the c axis of the crystal, with an angle between their electric vectors. The polarization direction and the intensity of the echo in the case of small-area exciting pulses are calculated both for the twopulse echo and the three-pulse echo. An experiment on La F3: Pr3+ is also performed and the result is well interpreted by the calculation.

DOI
10.2184/lsj.10.378

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The behavior of the photon echo produced by an inhomogeneously broadened spectral line is analyzed, with particular emphasis on the effect of spatial degeneracy of the molecular energy levels. The theoretical results are used to aid in the identification of the states involved in the echoes produced from gaseous S${\mathrm{F}}_{6}$ excited by pulses of C${\mathrm{O}}_{2}$ laser radiation near 10.6 \ensuremath{\mu}. The analysis demonstrates that for the $|{\ensuremath{\Delta}}_{j}|=1$ transitions ($P$ and $R$ branches) the echo induced by two linearly polarized pulses propagating along the same direction, with an angle $\ensuremath{\psi}$ between their electric vectors, is polarized at an angle greater than $\ensuremath{\psi}$ with respect to the first pulse, and the echo intensity decreases to a minimum, but not zero, as $\ensuremath{\psi}$ approaches $\frac{\ensuremath{\pi}}{2}$. An exception is the $j=1\ensuremath{\leftrightarrow}j=0$ transition, for which the echo is always polarized along the second pulse and the intensity varies as ${cos}^{2}\ensuremath{\psi}$. For ${\ensuremath{\Delta}}_{j}=0$ transitions ($Q$ branch) the echo polarization generally lies at an angle smaller than $\ensuremath{\psi}$, i.e., between the first two pulses, and its intensity also decreases as $|\ensuremath{\psi}|$ approaches $\frac{\ensuremath{\pi}}{2}$. The exceptions for the ${\ensuremath{\Delta}}_{j}=0$ transitions are the cases $j=\frac{1}{2}\ensuremath{\leftrightarrow}j=\frac{1}{2}$ and $j=1\ensuremath{\leftrightarrow}j=1$. In the former case, the echo is polarized at an angle $2\ensuremath{\psi}$ with respect to the electric field vector of the first pulse, and the echo intensity is independent of $\ensuremath{\psi}$; whereas in the latter case, the echo behaves like that for $j=1\ensuremath{\leftrightarrow}j=0$. The dependence of the echo behavior on the angular momentum of states involved in the transition can serve to identify the transitions when measurements of the echo polarization and intensity are possible.

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Physical Review A•Aug 1, 1977•13 citations
The behavior of the photon-echo polarization in solids is discussed. The photon echo in La F3: Pr3+ is considered in some details as a typical example. The echo is induced by linearly polarized pulses propagating along the c axis of the crystal, with an angle between their electric vectors. The polarization direction and the intensity of the echo in the case of small-area exciting pulses are calculated both for the twopulse echo and the three-pulse echo. An experiment on La F3: Pr3+ is also performed and the result is well interpreted by the calculation.
With regard to the depolarizing collisions the polarization properties of the photon echo formed by two exciting pulses linearly polarized at an angle ψ to each other with arbitrary values of their areas and arbitrary ratios of the durations and the time of reversible Doppler relaxation are obtained. The case of the small area of the first exciting pulse is examined. It is shown that the polarization properties of the photon echo can be described by equations obtained in the limit of small areas for both the first and the second exciting pulses up to the area of the second exciting pulse of the order of unity.
The polarization properties of the photon echo generated by two linearly polarized pulses of resonant radiation at the (6s6p)3 P 1 ↔ (6s 2)1 S 0 transition of 174Yb are investigated. A complicated polarization behavior of the photon echo versus an angle between the polarization vectors of the excitation pulses is revealed in a mixture of ytterbium vapor with inert gas. For the angles ranging from 0° to 75°, a conventional echo with its linear polarization coinciding with the second excitation pulse dominates and the echo amplitude decreases with an increasing angle. For the angles ranging from 75° to 89°, the photon echo is elliptically polarized. Finally, for an angle of 90°, the conventional echo disappears and the collision echo becomes linearly polarized along the first excitation pulse.
The polarization properties of photon echoes in strong magnetic field, when the action of this field during the time of propagation of the exciting pulses and the echo signal through the resonant gaseous medium cannot be neglected, are studied theoretically. The photon echo polarization in strong magnetic field cannot be described by the polarization vector but rather by the polarization matrix. The degree of the photon echo polarization decreases with the increase of the magnetic field strength. The dependence of the photon echo intensity on the magnetic field strength was also analyzed numerically. In strong magnetic field the fast oscillations of this intensity appear to be damping and modulated by the slower ones. The spectrum of these oscillations depend also on the spectra of the exciting pulses, so that in case of small area of the first exciting pulse its temporal shape may be reconstructed from the oscillations of the echo intensity versus the magnetic field strength.
The behavior of the photon echo produced by an inhomogeneously broadened spectral line is analyzed, with particular emphasis on the effect of spatial degeneracy of the molecular energy levels. The theoretical results are used to aid in the identification of the states involved in the echoes produced from gaseous SF6{\mathrm{F}}_{6}F6​ excited by pulses of CO2{\mathrm{O}}_{2}O2​ laser radiation near 10.6 \ensuremath{\mu}. The analysis demonstrates that for the $|{\ensuremath{\Delta}}_{j}|=1$ transitions (PPP and RRR branches) the echo induced by two linearly polarized pulses propagating along the same direction, with an angle $\ensuremath{\psi}$ between their electric vectors, is polarized at an angle greater than $\ensuremath{\psi}$ with respect to the first pulse, and the echo intensity decreases to a minimum, but not zero, as $\ensuremath{\psi}$ approaches $\frac{\ensuremath{\pi}}{2}$. An exception is the $j=1\ensuremath{\leftrightarrow}j=0$ transition, for which the echo is always polarized along the second pulse and the intensity varies as ${cos}^{2}\ensuremath{\psi}$. For ${\ensuremath{\Delta}}_{j}=0$ transitions (QQQ branch) the echo polarization generally lies at an angle smaller than $\ensuremath{\psi}$, i.e., between the first two pulses, and its intensity also decreases as $|\ensuremath{\psi}|$ approaches $\frac{\ensuremath{\pi}}{2}$. The exceptions for the ${\ensuremath{\Delta}}_{j}=0$ transitions are the cases $j=\frac{1}{2}\ensuremath{\leftrightarrow}j=\frac{1}{2}$ and $j=1\ensuremath{\leftrightarrow}j=1$. In the former case, the echo is polarized at an angle $2\ensuremath{\psi}$ with respect to the electric field vector of the first pulse, and the echo intensity is independent of $\ensuremath{\psi}$; whereas in the latter case, the echo behaves like that for $j=1\ensuremath{\leftrightarrow}j=0$. The dependence of the echo behavior on the angular momentum of states involved in the transition can serve to identify the transitions when measurements of the echo polarization and intensity are possible.
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.
The polarization of photon echoes stimulated by linear-linear, circular-linear, and linear-circular excitation sequences has been studied in SF6{\mathrm{F}}_{6}F6​ with the P(12)P(12)P(12) through P(26)P(26)P(26) laser lines of CO2{\mathrm{O}}_{2}O2​ near 10.6 \ensuremath{\mu}m and in SiF4{\mathrm{F}}_{4}F4​ with the P(28)P(28)P(28) through P(34)P(34)P(34) lines near 9.6 \ensuremath{\mu}m. A linear-linear pulse sequence with angle $\ensuremath{\beta}$ between the linear polarizations produces an echo at angle $\ensuremath{\phi}$ with respect to the second pulse. $\ensuremath{\phi}$ rotates in the same sense as $\ensuremath{\beta}$ with P(16)P(16)P(16) in SF6{\mathrm{F}}_{6}F6​ and in the opposite sense as $\ensuremath{\beta}$ with the other lines in SF6{\mathrm{F}}_{6}F6​, and with the lines in SiF4{\mathrm{F}}_{4}F4​. A left-circular-linear sequence produces a right-elliptic echo with P(16)P(16)P(16) in SF6{\mathrm{F}}_{6}F6​, and a left-elliptic echo in the other cases. A linear-left-circular sequence produces a left-circular echo in all cases. These results are in accord with the large-JJJ polarization theory of Heer and Nordstrom. For a linear-linear excitation sequence, this theory predicts an unnormalized echo electric field $\stackrel{\ensuremath{\rightarrow}}{\mathrm{E}}\ensuremath{\cong}\ensuremath{\mp}\stackrel{^}{X}(\frac{1}{2}sin\ensuremath{\beta})+\stackrel{^}{Z}cos\ensuremath{\beta}$, where the negative sign applies to a PPP- or RRR-branch transition, and the plus sign to a QQQ-branch transition. For a left-circular-linear sequence, the theory predicts an unnormalized echo electric field $\stackrel{\ensuremath{\rightarrow}}{\mathrm{E}}\ensuremath{\cong}\ifmmode\pm\else\textpm\fi{}\frac{1}{2}i\stackrel{^}{X}+\stackrel{^}{Z}$, where the plus sign refers to a PPP- or RRR-branch transition, and the negative sign to a QQQ-branch transition. Echo decay rates determined from relaxation measurements are used to calculate molecular cross sections, and these cross sections are compared with calculations based on the refractive indices and the Slater-Kirkwood equation. Experimental cross sections are in general smaller than those found from the Slater-Kirkwood equation.