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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Population and nonlinear polarization coherent changes on Raman transition due to two-photon pulse excitation

S. V. Anikeev, V. N. Kulyasov, Viacheslav B. Morozov, A. N. Olenin, Vladimir G. Tunkin

Published Mar 15, 1999• 0 citations
Publisher

Abstract

Population and third order nonlinear polarization coherent changes on Raman electronic transition of thallium atoms excited by a couple of 30 ps pulses of dye- and Nd:YAG lasers were observed. Collimated exciting and probing beams propagated through a heated cell of one centimeter length with thallium vapor. Population and nonlinear polarization dependences as functions of exciting pulses energy product were monitored using permanently delayed probing pulses.

DOI
10.1117/12.342336

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Population and third order nonlinear polarization coherent changes on Raman electronic transition of thallium atoms excited by a couple of 30 ps pulses of dye- and Nd:YAG lasers were observed. Collimated exciting and probing beams propagated through a heated cell of one centimeter length with thallium vapor. Population and nonlinear polarization dependences as functions of exciting pulses energy product were monitored using permanently delayed probing pulses.
Optical nutation under Raman excitation accompanied by considerable (up to inverted) population changes was observed. The Raman-active 6P1/2–6P3/2 transition of thallium atoms was excited by picosecond pulses of a dye and an Nd : YAG laser. Transition polarization and upper level population were probed by delayed pulses at a fixed time by means of coherent Raman scattering and third harmonic generation schemes, respectively. Optical nutation manifested itself in corresponding changes of anti-Stokes and third harmonic signal energies as functions of the product of the pump pulses energies. As a result of the a.c. Stark shift, the nutation picture strongly depended on the sign of wavenumber detuning from the transition wavenumber. Copyright © 2000 John Wiley & Sons, Ltd.
Summary form only given. Optical nutation at pulse biharmonic excitation of Raman transition accompanied by considerable, up to inverse, population changes was observed. The optical nutation manifested itself in corresponding changes of polarization and upper level population of the thallium 6P/sub 1/2/-6P/sub 3/2/ transition excited by picosecond pulses of a dye and a Nd:YAG lasers and probed by delayed pulses by means of coherent Raman scattering and third harmonic generation schemes. As a result of the AC Stark shift, the nutation picture strongly depended on the sign of frequency detuning from the transition frequency.
Optical nutation at the Raman-active transition 6P 1/2−6P 3/2 of thallium atoms (ω R /2πc=7793 cm −1) under resonant Raman excitation by a biharmonic picosecond pulsed field, giving rise to substantial motion of the population, is detected. Optical nutation appears as an oscillatory behavior of the energy of the anti-Stokes scattering of probe pulses, which follow with a fixed delay, as a function of the product of the energies of the excitation pulses. As a result of the dynamic Stark effect, which decreases the frequency of the transition under study, resonance excitation conditions are satisfied for negative initial detunings of the Raman excitation frequency from resonance. The Raman scattering cross section for the transition under study is estimated by comparing the experimental data with the calculations.
A coherent superposition state of 5S and 5D levels of Rb vapor, when it was excited by two-photon resonant transition between these levels, was observed by applying an interrogation pulse which was non-resonant to the system. The emphasis is laid on this coherence in the atomic excitation, instead of just the population inversion, in explaining the origin of various strong collimated emissions observed by many authors. Saturation of the off diagonal density matrix element between 5S and 5D levels was observed at higher excitation level due to the population change. An analysis of the saturation is given using a simple model for the coherence of the dye laser beam.
The recently demonstrated technique of optically phase-locked pulse-pair (PLPP) excited spontaneous emission is described by a third-order perturbative density matrix approach. A nonlinear polarization description shows how PLPP spectroscopy depends on all the relevant material dephasing time scales. The time and frequency integrated resonance spontaneous emission consists entirely of resonance fluorescence, and is derived exclusively from excited-state population decay terms, i.e., diagonal second-order density-matrix elements. These third-order polarization results are proportional to the previously derived linear polarization expressions found to describe the observed PLPP I2 vapor emission. The nonlinear treatment allows a comparison of this technique to other forms of ultrafast pump–probe spectroscopies such as transient absorption and photon echo techniques. The role of impulsively prepared coherences is clearly described by this analysis. The effect of pulse duration, relative to material dephasing times, is explored for relaxation given by the optical Bloch equations. The most significant differences between a linear and nonlinear polarization treatment occur for pulse durations greater than the optical dephasing time or when excited state population and coherence decays are of the order of rovibrational periods. A fluorescence line narrowing effect, due to short pulse excitation, is predicted.
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.