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The Journal of Chemical Physics

Propagation of complex shaped ultrafast pulses in highly optically dense samples

J. C. Davis, Matthew R. Fetterman, W. S. Warren, Debabrata Goswami

Published Apr 17, 2008• 5 citations
Publisher

Abstract

We examine the propagation of shaped (amplitude- and frequency-modulated) ultrafast laser pulses through optically dense rubidium vapor. Pulse reshaping, stimulated emission dynamics, and residual electronic excitation all strongly depend on the laser pulse shape. For example, frequency swept pulses, which produce adiabatic passage in the optically thin limit (independent of the sign of the frequency sweep), behave unexpectedly in optically dense samples. Paraxial Maxwell optical Bloch equations can model our ultrafast pulse propagation results well and provide insight.

DOI
10.1063/1.2894871

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We examine the propagation of shaped (amplitude- and frequency-modulated) ultrafast laser pulses through optically dense rubidium vapor. Pulse reshaping, stimulated emission dynamics, and residual electronic excitation all strongly depend on the laser pulse shape. For example, frequency swept pulses, which produce adiabatic passage in the optically thin limit (independent of the sign of the frequency sweep), behave unexpectedly in optically dense samples. Paraxial Maxwell optical Bloch equations can model our ultrafast pulse propagation results well and provide insight.
Ultrafast laser pulses with complex envelopes (amplitude and frequency modulated) are used to excite an optically dense column of rubidium vapor. Pulse reshaping, stimulated emission dynamics, and residual electronic excitation in the Rb vapor are all shown to depend strongly on the laser pulse shape. Pulses that produce adiabatic passage in the optically thin limit exhibit more complex behavior in optically thick samples, including an unexpected dependence on the sign of the frequency sweep. Numerical solutions of the Maxwell-Bloch equations are shown to account for our results.
Summary form only given. We study the interaction between intense (50 MW peak power), shaped ultrafast laser pulses and optically dense samples of Rb vapor. In particular, we concentrate our attention on laser pulses with a the complex hyperbolic secant envelope, or equivalently, a sech electric field envelope with a tanh frequency sweep. In order to produce and characterize the shaped laser pulses used in our experiments, we exploited several new technologies: amplified, shaped laser pulses were generated using an acousto-optic modulator-based system combined with a chirped-pulse regenerative amplifier. The amplitude and phase of these pulses were then characterized by the STRUT (spectrally and temporally resolved upconversion technique). The STRUT was used to measure the laser pulses both before and after propagating through Rb vapor. Examples of such experimental STRUT images are presented. The complex sech pulse was selected because, in optically thin media, only it and rectangular pulses give complete analytical solutions to the Bloch equations. This shape has been found to generate complete population inversion over a well-defined and amplitude-insensitive bandwidth. In optically dense samples the excited state dynamics are not so straightforward. We have found, both in experiments and theoretically, that the extent and character of the population inversion is related to the frequency sweep of the laser pulses as does the amount of residual excited population after the pulse and any subsequent stimulated emission.
We present a numerical study of the properties of optical forces on moving atoms derived from purely stimulated processes produced by multiple adiabatic rapid-passage sequences. The optical Bloch equations are solved for a carefully timed sequence of frequency-swept pulses that can produce a force much larger than the ordinary radiative force. We describe the effects of the sweep range, peak intensity, sweep direction, number of pulses, atomic velocity, and spontaneous emission. Since the momentum of thermal atoms is much larger than that transferred by a single absorption-stimulated emission cycle, multiple repetitions are needed to make a significant velocity change.
A solution to Maxwell's equations in the three-dimensional frequency domain is used to calculate rephasing two-dimensional Fourier transform (2DFT) spectra of the D2 line of atomic rubidium vapor in argon buffer gas. Experimental distortions from the spatial propagation of pulses through the sample are simulated in 2DFT spectra calculated for the homogeneous Bloch line shape model. Spectral features that appear at optical densities of up to 3 are investigated. As optical density increases, absorptive and dispersive distortions start with peak shape broadening, progress to peak splitting, and ultimately result in a previously unexplored coherent transient twisting of the split peaks. In contrast to the low optical density limit, where the 2D peak shape for the Bloch model depends only on the total dephasing time, these distortions of the 2D peak shape at finite optical density vary with the waiting time and the excited state lifetime through coherent transient effects. Experiment-specific conditions are explored, demonstrating the effects of varying beam overlap within the sample and of pseudo-time domain filtering. For beam overlap starting at the sample entrance, decreasing the length of beam overlap reduces the line width along the ωτ axis but also reduces signal intensity. A pseudo-time domain filter, where signal prior to the center of the last excitation pulse is excluded from the FID-referenced 2D signal, reduces propagation distortions along the ωt axis. It is demonstrated that 2DFT rephasing spectra cannot take advantage of an excitation-detection transformation that can eliminate propagation distortions in 2DFT relaxation spectra. Finally, the high optical density experimental 2DFT spectrum of rubidium vapor in argon buffer gas [J. Phys. Chem. A 2013, 117, 6279-6287] is quantitatively compared, in line width, in depth of peak splitting, and in coherent transient peak twisting, to a simulation with optical density higher than that reported.
We present a detailed study of the interaction of ultrashort laser pulses with a resonant three level system (fine structure levels of rubidium). As expected, for low intensities a linear model and for higher intensities a semiclassical model (Maxwell-Bloch) is fully sufficient to describe the observed results. In both cases, however, it is essential to have an accurate knowledge of the incident electric field, i.e., the amplitude and the phase, in order to simulate the interaction process. It is shown that on small time scales the phase modulation of the incident pulse influences the reshaping process during pulse propagation whereas on longer time scales the reshaping is solely governed by the dynamics of the atomic system.
We study slow-light propagation dynamics in warm Rb vapor. We present data showing significant pulse reshaping when the bandwidth of the pulses is increased and present a model that qualitatively explains the observed behavior. Our data and modeling emphasize how the Doppler broadening in a warm vapor strongly affects the propagation of high-frequency components and leads to unintuitive features on the transmitted pulse shapes. This has important consequences for applications involving the delay of large-bandwidth pulses.