A diagrammatic technique is developed to account for the saturation effects which occur when optical coherent transients are generated by broad-bandwidth light pulses. The paper is focused on the calculation of the two-atom, single-time dipole correlation function which originates the signal. In addition to the single-excitation-field situation, we examine the coherent transient generation by overlapping time-delayed correlated pulses. Our approach requires that one of the two correlated pulses be weak. The calculation of the delay dependence of the signal intensity is thoroughly worked out in the case of two-pulse and three-pulse transients in an angled-beam configuration.
A theoretical analysis of the optical coherent transients that arise when a sample of two-level atoms is irradiated by a sequence of three broad-bandwidth pulses is presented. The first two pulses have a relative delay time of order of the correlation time of the pulse fluctuations and are sent into an atomic vapor from different directions. These pulses, whose temporal width is much greater than the delay time, can be correlated with one another and can be strong enough to saturate the two-level atomic transition. The third pulse is weak, noncorrelated with the first two, and is delayed in time so that it does not overlap them. We present a detailed examination of the transient signal that is produced when the third pulse is scattered by the spatial gratings in the population difference of atoms created by the first two pulses. Taking into account the effects of inhomogeneous and homogeneous broadening, we calculate the intensity of the transient signal, emitted in different directions, as a function of delay time. The signal is found to depend dramatically on the intensities of the excitation pulses. It is shown that, for strong excitation pulses, there is a direct dependence of the signal on the cross-correlation time of pulses ${\mathrm{\ensuremath{\tau}}}_{\mathit{c}}^{12}$ that does not exist when the pulses are weak. In particular, the strongest signals exhibit a peak of width of order ${\mathrm{\ensuremath{\tau}}}_{\mathit{c}}^{12}$. This peak can have a very narrow dip near its maximum whose width is much smaller than ${\mathrm{\ensuremath{\tau}}}_{\mathit{c}}^{12}$, if the pulses are fully correlated. We develop a representation of the time evolution of the Bloch vector of a two-level atom, driven by time-delayed pulses, that enables us to explain our results. In this representation, the two time-delayed pulses are replaced by two fully overlapping pulses having some effective amplitudes and atomic field detunings.
This paper deals with the equations of motion of the density matrix of a two-level atom in the presence of an intense multimode radiation field characterizing a multimode laser. Using a simplified treatment of line broadening which does not include correlations between momentum-changing collisions and pressure-broadening collisions, we obtain expressions which show the effect of pressure, laser-pulse length, and intensity on the excitation. We obtain analytic expressions in limiting cases of the pressure which allow prediction of the degree of excitation from a given laser pulse. In our treatment the phase relaxation time of the atoms is assumed to be fast enough so that coherence effects among the atoms can be ignored. Treating the velocity of the atoms statistically, we solve for three cases: constant velocity, velocity changes that are fast compared to the excitation time but slow compared to the dephasing time, and velocity changes that are fast compared to all other processes. The three cases yield the same formal equation for the two-body process of absorption of photons by incoherent atoms; however, the cross sections differ and are calculated explicitly for each case. Also discussed are the range of laboratory conditions and the relationship between these laboratory conditions and the various cases considered to demonstrate that under most circumstances this simple photon-absorption picture is applicable, provided the cross section is calculated correctly.
Coherent excitation of an atomic excited state occurs during the propagation of near-resonant light pulses and is responsible for the induced polarization. Simultaneously, incoherent excitation occurs due to the relaxation processes described by the absorption coefficient. Here, the theory for the coherent and incoherent excitation is initially presented in terms of the traditional vector model. While a complete understanding of the two-level system is provided by the vector model, it is shown to be incomplete when the problem of directly monitoring the coherent and incoherent excitation is considered. This is because this latter problem involves more than two levels. For this more complicated multilevel problem, adiabatic states are introduced to gain further understanding. The adiabatic states are the stationary states of the atom in the presence of the near-resonant laser field; they help to explain the intimate connection between the coherent excitation and the two-photon resonance. Experimental measurements of the coherent and incoherent excitation associated with near-resonant pulse propagation in Rb vapor are presented. The double-resonance technique used a relatively strong pulsed dye laser tuned near the $5{S}_{\frac{1}{2}}\ensuremath{\leftrightarrow}5{P}_{\frac{1}{2}}$ transition (7948 \AA{}A) of Rb to produce the coherent and incoherent excitation, and a weak, tunable cw dye laser tuned in the region of the $5{P}_{\frac{1}{2}}\ensuremath{\leftrightarrow}6{D}_{\frac{3}{2}}$ transition (6206 \AA{}A) to monitor this excitation. In agreement with theory, the experimental results demonstrate that coherent excitation is responsible for two-photon absorption, while the incoherent excitation corresponds to one-photon absorption to the
5P21 state.
Measurements of the relaxation times T1 and T2 of a two-level system by nonlinear transient spectroscopic methods are discussed, where delayed incident pulses are assumed to have correlation times much shorter than T1 or T2 but varied widths. In particular, a delayed degenerate four-wave mixing (photon echoe) and apump-and-probe type transmission measurement with incoherent long pulses are considered in detail, and a principle of their use for ultrafast spectroscopy is clarified. If the field is steady and T1>>T2, the time resolutionof T2measurement by the delayed four-wave mixlng is determined by the field correlation, therefore by the spectral width of the incident light irrespective of the pulse width. The time resoution of the T1 measurement by the pump-and-probe method is determined by the intensity correlation of the incident light, whereasthe one by the delayed four-wave mixing by a higher order correlation.
Using the formalism developed earlier, we treat spontaneous emission from a pair of identical two-level atoms
A1,
A2, whose separation
r21 can be comparable to the wavelength $\ensuremath{\lambda}$. We obtain expressions for time-dependent intensities and damping rates with the initial conditions (a) both atoms inverted, (b) prior excitation by a short $\frac{1}{2}\ensuremath{\pi}$ pulse, and (c) only
A1 inverted. The results in (a) are compared with those obtained for a model consisting of two initially excited harmonic oscillators
O1,
O2. The atoms exhibit superradiant behavior, whereas
O1,
O2 tend to trap radiation. In (a), the intensity pattern $\mathcal{R}(\ensuremath{\theta},t)$ develops lobes in different directions at different times, so that the spatial distribution of photons at time $t\ensuremath{\rightarrow}\ensuremath{\infty}$ is the same as in the independent-atom case ${r}_{21}\ensuremath{\gg}\ensuremath{\lambda}$. For the oscillators, the lobes of $\mathcal{R}(\ensuremath{\theta},t)$ do not change direction, but only become more pronounced as time increases. In (b) and (c), the lobes oscillate back and forth at frequency $2{\ensuremath{\Omega}}_{12}$ corresponding to the shifts $\ifmmode\pm\else\textpm\fi{}{\ensuremath{\Omega}}_{12}$ of the triplet and singlet states due to the ${A}_{1}\ensuremath{-}{A}_{2}$ interaction. The intensity can therefore have a sinusoidal component. Field correlation functions calculated for (a) and (c) show that
A2 and
A2 radiate simultaneously around the frequencies $\ensuremath{\epsilon}\ifmmode\pm\else\textpm\fi{}{\ensuremath{\Omega}}_{12}$, where $\ensuremath{\epsilon}$ is the single-atom resonant frequency. The spectrum is calculated for case (c), and shows the effects of coherent linewidth enhancement in addition to the frequency shifts.