We address the distinction between resonance Raman scattering and fluorescence as the excitation source is continuously tuned through resonance. The experiments are performed in iodine vapor using a cw laser, whose intensity is electrooptically modulated in the 0.1-50-MHz frequency range. A lock-in amplifier is used to detect both the in-phase and out-of-phase response of the emission. The modulated signal is found to be the sum of two components. One component varies with angular modulation frequency ω, as (1 + ω2τ2)-1/2, where τ is the lifetime of the excited state. The other is found to be flat within the range of modulation frequency used in the experiment. Since the results of the modulation experiment are the Fourier transform of the response to pulsed excitation, the first component corresponds to exponential decay with the fluorescence lifetime and the second corresponds to a prompt response. A density matrix calculation shows that the prompt response would be absent if the absorption were independent of laser frequency. It exists as a result of the finite inhomogeneous linewidth and the laser detuning from the center of the transition. The amplitude of the delayed and prompt components is a function of laser frequency. This gives a full description of the dynamical response to the emission to linear excitation as the laser is tuned continuously through resonance. The response of the sample to nonlinear excitation is also discussed.
The steady-state absorption of a beam of sodium atoms irradiated by a train of pulses from a mode-locked dye laser has been measured. The sodium atoms were prepared as two-level systems by optical pumping with a two-mode laser. Absorption spectra on the 589.0-nm D2 line were recorded over 20 GHz with a frequency-stabilized, tunable, mode-locked dye laser having a bandwidth of 3.7 GHz and a mode spacing of 82 MHz. The laser-pulse profile was determined from the spectral profile assuming transform-limited pulses and was incorporated in theoretical calculations of excitation spectra obtained by numerical integration of the optical Bloch equations. By comparison of measured absorption spectra and theoretical excitation spectra the validity of the weak-field solution as well as the predicted saturation behavior were fully verified by the experimental results. For the highest level of irradiation applied, the laser pulses were identified as π pulses.
levels of atomic sodium using ultrashort laser pulses in a stepwise excitation scheme. Two broadband femtosecond laser pulses are used to excite the 6S level from the 3S ground level in sodium vapor. The first one is simultaneously resonant with the D1 and D2 lines of the 3S→3P transition, and the second one with the 3P→6S transition. The delay between the two pulses is scanned in order to probe the dephasing between the two excited intermediate levels. Quantum beating is observed by monitoring the fluorescence signals at 330 nm and 515 nm, namely transition 4P→3S and 6S→3P, respectively. Signals are compared to a semi-classical model that reproduces the oscillations with a very good agreement.
A technique for producing phase-related picosecond optical pulses is described. A sequence of two phase-related pulses, well separated in time, is applied to the D1 line in Na vapor. When the phase between the two pulses is scanned, oscillations in the incoherent fluorescence are observed. This demonstrates the well-defined phase relationship between the pulses. Measuring the amplitude of the oscillations as a function of pulse separation yields the Na optical coherence decay. A beat arising from the ground-state hyperfine splitting is observed, and the results agree well with calculation.
Calcium vapor has been excited by two-photon absorption of a mode-locked dye-laser pulse, and emission from a coherent superposition state of the $4{s}^{2}^{1}S_{0}$ and
4s3d1D2 levels has been observed using a delayed off-resonant interrogation pulse in the picosecond regime. The emission signal intensity was measured as a function of the delay time of the interrogation pulse, and showed a peak well delayed from that of the dye-laser pulse. This reflects the fact that the induced coherence is expressed by a time integral of the excitation. The emission signal was then found to decay as a result of the Doppler effect. The above process is analyzed by Bloch and Maxwell equations. This is the first reported observation of the coherence of an atomic system induced by two-photon absorption, a coherence which persists after the passage of the excitation pulse and decays inhomogeneously as a result of thermal motion. In carrying out the experiment, deformation of the input dye-laser pulse during propagation through the two-photon resonant medium was carefully avoided.
Sodium vapor, in the density range
1013 to 5 \ifmmode\times\else\texttimes\fi{}
1014 ${\mathrm{cm}}^{\ensuremath{-}3}$, was excited by a cw dye laser, tuned 20-150 GHz from either the
D1 or
D2 resonance line. We observed a three-peak scattered spectrum, consisting of the Rayleigh component at the laser frequency, and the two fluorescence components (direct and sensitized) at the atomic resonance-line frequencies. Corrections to the Rayleigh signals for anisotropy and polarization effects, and to the fluorescence signals for radiation trapping, were made in order to obtain the ratio of the sum of the total intensities of the two fluorescence components to that of the Rayleigh component. This ratio combined with a measurement of the line-wing absorption coefficient yields the sodium density and the
D-line self-broadening rate coefficients [${k}_{\mathrm{br}}=4.67\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}7}$
cm3${\mathrm{s}}^{\ensuremath{-}1}$ (\ifmmode\pm\else\textpm\fi{}15%) for the
D2 line and ${k}_{\mathrm{br}}=3.07\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}7}$
cm3${\mathrm{s}}^{\ensuremath{-}1}$ (\ifmmode\pm\else\textpm\fi{}15%) for the
D1 line]. Asymmetry in the self-broadened line wings due to fine-structure recoupling was observed. The measured intensity ratio of the
D lines, combined with pulsed measurements of the effective radiative decay rates in the presence of radiation trapping, yields the fine-structure collisional-mixing cross section [$\ensuremath{\sigma}(3{P}_{\frac{3}{2}}\ensuremath{\rightarrow}3{P}_{\frac{1}{2}})=172$
A˚2(\ifmmode\pm\else\textpm\fi{}18%)] at $T\ensuremath{\cong}300\ifmmode^\circ\else\textdegree\fi{}$ C. Our results are compared to other experiments and to theory.