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Physical Review A

Polarization of signal wave radiation generated by parametric four-wave mixing in rubidium vapor: Ultrafast (∼150−fs) and nanosecond time scale excitation

Chang Jun Zhu, Andrey A. Senin, Zhongling Lu, Ju Gao, Y. Xiao, James Gary Eden

Published Aug 10, 2005• 24 citations
Publisher

Abstract

The polarization characteristics of the signal wave produced in Rb vapor by difference-frequency, parametric four-wave mixing (FWM) has been investigated for either ultrafast $(\ensuremath{\sim}150\phantom{\rule{0.3em}{0ex}}\mathrm{fs})$ or nanosecond time-scale excitation of the $5s\ensuremath{\rightarrow}\ensuremath{\rightarrow}5d$, $7s$ two photon transitions. The electronic configurations of the $5d\phantom{\rule{0.2em}{0ex}}^{2}D_{5∕2}$ and $7s\phantom{\rule{0.2em}{0ex}}^{2}S_{1∕2}$ states of Rb, as well as their energy separation $(\ensuremath{\sim}608\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1})$, offers the opportunity to examine separately the resonantly enhanced $5s\ensuremath{\rightarrow}\ensuremath{\rightarrow}7s$, $5d\ensuremath{\rightarrow}6p\ensuremath{\rightarrow}5s$ FWM pathways on the nanosecond time scale and then to drive both channels simultaneously with an ultrafast pulse of sufficient spectral width. As expected, dye laser $(\ensuremath{\sim}10\phantom{\rule{0.3em}{0ex}}\mathrm{ns})$ excitation of the $5s\ensuremath{\rightarrow}\ensuremath{\rightarrow}5d$ $(J=5∕2)$ transition produces a signal wave $({\ensuremath{\lambda}}_{s}\ensuremath{\sim}420\phantom{\rule{0.3em}{0ex}}\mathrm{nm})$ having the same ellipticity as the driving optical field. Two photon excitation of Rb $(7s)$ on the same time scale, however, generates an elliptically polarized signal when the pump is linearly polarized $(\ensuremath{\epsilon}=1)$, a result attributed to $7s\ensuremath{\rightarrow}6p$, $5p$ amplified spontaneous emission at $\ensuremath{\sim}4\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{m}$ and $\ensuremath{\sim}741\phantom{\rule{0.3em}{0ex}}\mathrm{nm}$, respectively. Simultaneous excitation of the $5s\ensuremath{\rightarrow}\ensuremath{\rightarrow}7s$, $5d$ transitions with $\ensuremath{\sim}150\phantom{\rule{0.3em}{0ex}}\mathrm{fs}$ pulses centered at $\ensuremath{\sim}770\phantom{\rule{0.3em}{0ex}}\mathrm{nm}$ yields polarization characteristics that can be approximated as a superposition of those for the individual transitions, thus displaying weak coupling between the two FWM channels. Also, the influence of molecular contributions to the FWM signal is observed for Rb number densities above $\ensuremath{\sim}5\ifmmode\times\else\texttimes\fi{}{10}^{14}\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}3}$.

DOI
10.1103/physreva.72.023811

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INTERFERENCE BETWEEN THE 5d5/2 – 5p3/2 AND 5p3/2 – 5s1/2 COHERENCES (386.4 AND 384.1 THz) IN Rb OBSERVED BY ULTRAFAST FOUR-WAVE MIXING SPECTROSCOPY

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\begin{wrapfigure}{r}{0pt} \includegraphics[scale=0.32]{Fig1.eps} \end{wrapfigure} Coherences at 386.2 THz and 384.1 THz, corresponding to the 5d$_{5/2}$ – 5p$_{3/2}$ and 5p$_{3/2}$ – 5s$_{1/2}$ difference frequencies, respectively, have been established in the Rb atom during pump-probe experiments involving pairs of identical ~150 fs pulses produced by a Ti:\chem{Al_2O_3} laser and a Michelson interferometer. The interference between the two coherences within the atom is observed through a parametric four-wave mixing process in Rb and detection of the signal wave intensity at 420 nm. Scanning the time delay between the pump and probe pulses over a 600 ps interval produces a sampling rate over 300 THz and allows for a spectral domain resolution of 0.05 cm$^{-1}$ to be achieved. The figure at right shows several spectra recorded near 2.1 THz, the (5d$_{5/2}$ – 5p$_{3/2}$) - (5p$_{3/2}$ – 5s$_{1/2}$) difference frequency, with varying angle between the pump and probe pulses (i.e., the phase matching angle) and varying Rb background density. A Fano interference window is clearly observed, and analysis of these and similar spectra demonstrates that the amplitude and phase of the coherently-coupled, three Rb state system can be controlled precisely.

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A dense sample of atomic Rb vapor excited by a 4 ps laser pulse two-photon resonant with the $5S\ensuremath{-}5D$ transition in a large Fresnel number geometry emits a delayed coherent omnidirectional ir pulse on the $5D\ensuremath{-}6P$ transition. This superfluorescence emission involves a coherent population transfer to the $6P$ level and results in simultaneous directional uv emission and coherent population transfer back to the ground $5S$ state. This uv emission is a manifestation of parametric time-delayed four-wave mixing. For a composite noncollinear, $|{\stackrel{\ensuremath{\rightarrow}}{k}}_{1}|\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}|{\stackrel{\ensuremath{\rightarrow}}{k}}_{2}|$, excitation, the uv radiation pattern is conical and the cone angle depends on the angle between the excitation pulses.

Physical Review Letters•May 31, 1999•48 citations
The polarization characteristics of the signal wave produced in Rb vapor by difference-frequency, parametric four-wave mixing (FWM) has been investigated for either ultrafast (\ensuremath∼150fs)(\ensuremath{\sim}150\phantom{\rule{0.3em}{0ex}}\mathrm{fs})(\ensuremath∼150fs) or nanosecond time-scale excitation of the 5s\ensuremath→\ensuremath→5d5s\ensuremath{\rightarrow}\ensuremath{\rightarrow}5d5s\ensuremath→\ensuremath→5d, 7s7s7s two photon transitions. The electronic configurations of the 5d2D5∕25d\phantom{\rule{0.2em}{0ex}}^{2}D_{5∕2}5d2D5∕2​ and 7s2S1∕27s\phantom{\rule{0.2em}{0ex}}^{2}S_{1∕2}7s2S1∕2​ states of Rb, as well as their energy separation (\ensuremath∼608cm\ensuremath−1)(\ensuremath{\sim}608\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1})(\ensuremath∼608cm\ensuremath−1), offers the opportunity to examine separately the resonantly enhanced 5s\ensuremath→\ensuremath→7s5s\ensuremath{\rightarrow}\ensuremath{\rightarrow}7s5s\ensuremath→\ensuremath→7s, 5d\ensuremath→6p\ensuremath→5s5d\ensuremath{\rightarrow}6p\ensuremath{\rightarrow}5s5d\ensuremath→6p\ensuremath→5s FWM pathways on the nanosecond time scale and then to drive both channels simultaneously with an ultrafast pulse of sufficient spectral width. As expected, dye laser (\ensuremath∼10ns)(\ensuremath{\sim}10\phantom{\rule{0.3em}{0ex}}\mathrm{ns})(\ensuremath∼10ns) excitation of the 5s\ensuremath→\ensuremath→5d5s\ensuremath{\rightarrow}\ensuremath{\rightarrow}5d5s\ensuremath→\ensuremath→5d (J=5∕2)(J=5∕2)(J=5∕2) transition produces a signal wave (\ensuremathλs\ensuremath∼420nm)({\ensuremath{\lambda}}_{s}\ensuremath{\sim}420\phantom{\rule{0.3em}{0ex}}\mathrm{nm})(\ensuremathλs​\ensuremath∼420nm) having the same ellipticity as the driving optical field. Two photon excitation of Rb (7s)(7s)(7s) on the same time scale, however, generates an elliptically polarized signal when the pump is linearly polarized (\ensuremathϵ=1)(\ensuremath{\epsilon}=1)(\ensuremathϵ=1), a result attributed to 7s\ensuremath→6p7s\ensuremath{\rightarrow}6p7s\ensuremath→6p, 5p5p5p amplified spontaneous emission at \ensuremath∼4\ensuremathμm\ensuremath{\sim}4\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{m}\ensuremath∼4\ensuremathμm and \ensuremath∼741nm\ensuremath{\sim}741\phantom{\rule{0.3em}{0ex}}\mathrm{nm}\ensuremath∼741nm, respectively. Simultaneous excitation of the 5s\ensuremath→\ensuremath→7s5s\ensuremath{\rightarrow}\ensuremath{\rightarrow}7s5s\ensuremath→\ensuremath→7s, 5d5d5d transitions with \ensuremath∼150fs\ensuremath{\sim}150\phantom{\rule{0.3em}{0ex}}\mathrm{fs}\ensuremath∼150fs pulses centered at \ensuremath∼770nm\ensuremath{\sim}770\phantom{\rule{0.3em}{0ex}}\mathrm{nm}\ensuremath∼770nm yields polarization characteristics that can be approximated as a superposition of those for the individual transitions, thus displaying weak coupling between the two FWM channels. Also, the influence of molecular contributions to the FWM signal is observed for Rb number densities above \ensuremath∼5\ifmmode×\else\texttimes\fi1014cm\ensuremath−3\ensuremath{\sim}5\ifmmode\times\else\texttimes\fi{}{10}^{14}\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}3}\ensuremath∼5\ifmmode×\else\texttimes\fi1014cm\ensuremath−3.
Axially phase-matched parametric six-wave mixing (PSWM) has been observed in Rb vapor by two-photon excitation of the atom $(5s\ensuremath{\rightarrow}\ensuremath{\rightarrow}7s,5d)$ with $\ensuremath{\sim}150\phantom{\rule{0.3em}{0ex}}\mathrm{fs}$ pulses, centered at $\ensuremath{\lambda}\ensuremath{\sim}769\phantom{\rule{0.3em}{0ex}}\mathrm{nm}$ and generated by a Ti:Al2O3\mathrm{Ti}:{\mathrm{Al}}_{2}{\mathrm{O}}_{3}Ti:Al2​O3​ laser system. For a peak laser pulse intensity of $30\phantom{\rule{0.3em}{0ex}}\mathrm{GW}\phantom{\rule{0.2em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}2}$, PSWM is observed for Rb number densities $([\mathrm{Rb}])>2.5\ifmmode\times\else\texttimes\fi{}{10}^{15}\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}3}$ whereas, for $[\mathrm{Rb}]=2.2\ifmmode\times\else\texttimes\fi{}{10}^{16}\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}3}$, the PSWM process is detectable for pump intensities above $\ensuremath{\sim}3\phantom{\rule{0.3em}{0ex}}\mathrm{GW}\phantom{\rule{0.2em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}2}$. Upconversion of the $1.367\phantom{\rule{0.3em}{0ex}}\mathrm{\ensuremath{\mu}}\mathrm{m}$ and $1.323\phantom{\rule{0.3em}{0ex}}\mathrm{\ensuremath{\mu}}\mathrm{m}$ signal waves into the visible $(\ensuremath{\lambda}\ensuremath{\sim}494\phantom{\rule{0.3em}{0ex}}\mathrm{nm})$ has been accomplished by sum frequency generation in LiIO3{\mathrm{LiIO}}_{3}LiIO3​, and quantum beating in Rb at 18.3THz18.3\phantom{\rule{0.3em}{0ex}}\mathrm{THz}18.3THz $(\ensuremath{\sim}608\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1})$ has been observed by monitoring the upconverted signal wave intensity produced in pump-probe experiments. These results broaden the scope of the wave packet detection scheme reported by Tran et al. [Opt. Lett. 23, 70 (1998)] in that a variety of coherent nonlinear optical processes $({\ensuremath{\chi}}^{(3)},{\ensuremath{\chi}}^{(5)},\dots{})$ appear to be suitable for observing the amplitude and phase of atomic (or molecular) wave packets.
Wavepackets are excited in rubidium vapor by intense ultrashort (∼100 fs) pulses centered at a wavelength of 620 nm or 770 nm. The generated atomic wavepackets are optically detected via a pump-probe experiment based on axially phase-matched parametric four-wave mixing (FWM). This nonlinear process results in coherent ultraviolet (UV) or violet emission that carries information about the relative number densities of the excited states. The frequency spectrum of the UV/violet signal intensity, recorded while varying the pump-probe time delay, shows the presence of quantum beats between energy levels involved in the FWM process. The time-frequency analysis of that temporal UV/violet data is done by means of the short-time Fourier transform that leads to retrieval of the temporal evolution of amplitude and phase of the quantum beats. The observed dynamics suggest that not only atomic but also molecular ( Rb*2 ) wavepackets are generated, and that the temporal history of the amplitude of the quantum beats reflects the production of the excited atomic fragments of Rb*2 dissociation. More precisely, changes in the Rb excited state number densities alter the third-order nonlinear susceptibility chi(3) of the Rb vapor, which affects generation of the output signal wave by FWM. Dissociation into several product states is detected, and their branching ratios are estimated. Thus, atomic wavepackets, combined with FWM, appear to be a sensitive new multichannel spectroscopic means to study the fundamental process of molecular dissociation.
The observation of an atomic wave packet by use of a coherent, nonlinear-optical process is reported. Wave packets formed in K or Rb vapor by two-photon excitation of ns and (n-2)dstates (n=8 for K; n=11 , 12 for Rb) with red (~620-nm) , 80-100-fs pulses were detected by four-wave mixing in pump-probe experiments. The temporal behavior of the wave packet is observed by monitoring the coherent UV radiation generated near the alkali mp(2)P? (2)S(1/2) (7</=m</=12 for Rb; 5</=m</=7 for K) resonance transitions when a probe pulse is scattered by the wave packet established by the earlier (identical) pump pulse. The spatial and spectral characteristics of the UV emission are well described by axially phase-matched four-wave mixing, and all the prominent frequency components of the wave packets are associated with energy differences between pairs of excited states for which Diota=0 or Diota=2 . These results demonstrate that the wave packet modulates chi((3))of the medium, thus rendering the wave packet detectable.
We investigate the transient response of the generated light from four-wave mixing (FWM) in the diamond configuration using a step-down field excitation. The transients show fast decay times and oscillations that depend on the detunings and intensities of the fields. A simplified model taking into account the thermal motion of the atoms, propagation, absorption, and dispersion effects shows qualitative agreement with the experimental observations with the energy levels in rubidium (5S1/25{S}_{1/2}5S1/2​, 5P1/25{P}_{1/2}5P1/2​, 5P3/25{P}_{3/2}5P3/2​, and 6S1/26{S}_{1/2}6S1/2​). The atomic polarization comes from all the contributions of different velocity classes of atoms in the ensemble modifying dramatically the total transient behavior of the light from FWM.
\begin{wrapfigure}{r}{0pt} \includegraphics[scale=0.32]{Fig1.eps} \end{wrapfigure} Coherences at 386.2 THz and 384.1 THz, corresponding to the 5d5/2_{5/2}5/2​ – 5p3/2_{3/2}3/2​ and 5p3/2_{3/2}3/2​ – 5s1/2_{1/2}1/2​ difference frequencies, respectively, have been established in the Rb atom during pump-probe experiments involving pairs of identical ~150 fs pulses produced by a Ti:\chem{Al_2O_3} laser and a Michelson interferometer. The interference between the two coherences within the atom is observed through a parametric four-wave mixing process in Rb and detection of the signal wave intensity at 420 nm. Scanning the time delay between the pump and probe pulses over a 600 ps interval produces a sampling rate over 300 THz and allows for a spectral domain resolution of 0.05 cm−1^{-1}−1 to be achieved. The figure at right shows several spectra recorded near 2.1 THz, the (5d5/2_{5/2}5/2​ – 5p3/2_{3/2}3/2​) - (5p3/2_{3/2}3/2​ – 5s1/2_{1/2}1/2​) difference frequency, with varying angle between the pump and probe pulses (i.e., the phase matching angle) and varying Rb background density. A Fano interference window is clearly observed, and analysis of these and similar spectra demonstrates that the amplitude and phase of the coherently-coupled, three Rb state system can be controlled precisely.
A dense sample of atomic Rb vapor excited by a 4 ps laser pulse two-photon resonant with the $5S\ensuremath{-}5D$ transition in a large Fresnel number geometry emits a delayed coherent omnidirectional ir pulse on the $5D\ensuremath{-}6P$ transition. This superfluorescence emission involves a coherent population transfer to the 6P6P6P level and results in simultaneous directional uv emission and coherent population transfer back to the ground 5S5S5S state. This uv emission is a manifestation of parametric time-delayed four-wave mixing. For a composite noncollinear, $|{\stackrel{\ensuremath{\rightarrow}}{k}}_{1}|\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}|{\stackrel{\ensuremath{\rightarrow}}{k}}_{2}|$, excitation, the uv radiation pattern is conical and the cone angle depends on the angle between the excitation pulses.