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Physical Review A

Chirping the probe pulse in a coherent transients experiment

S. J. Weber, B. Girard, B. Chatel

Published Feb 18, 2010• 1 citation
Publisher

Abstract

Coherent transients occur when a chirped pump pulse excites a two-level transition. They have been observed with an ultrashort probe pulse. Several studies have been dedicated to using various pump shapes. In this study, the roles of the pump and the probe pulses are reversed. With a Fourier-transform-limited pump pulse followed by a chirped-probe pulse, similar effects can be observed. Finally, the case of two pulses with opposite chirps is considered.

DOI
10.1103/physreva.81.023415

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Coherent transients occur when a chirped pump pulse excites a two-level transition. They have been observed with an ultrashort probe pulse. Several studies have been dedicated to using various pump shapes. In this study, the roles of the pump and the probe pulses are reversed. With a Fourier-transform-limited pump pulse followed by a chirped-probe pulse, similar effects can be observed. Finally, the case of two pulses with opposite chirps is considered.
The effects of coherent excitation of a two-level system with a linearly chirped pulse are studied theoretically and experimentally [in Rb (5s-5p)] in the low field regime. The coherent transients are measured directly on the excited state population on an ultrashort time scale. A sharp step corresponds to the passage through resonance. It is followed by oscillations resulting from interferences between off-resonant and resonant contributions. We finally show the equivalence between this experiment and Fresnel diffraction by a sharp edge.
It is nowadays possible to generate, in different spectral ranges, ultrabroadband light pulses with transform-limited (TL) duration corresponding to a few optical cycles. Whenever broadband pulses are employed, the dispersion experienced by the pulses causes a frequency chirp which may severely lengthen their duration and influence time-resolved measurements. While it is well known that the relative weight of ground-state versus excited-state oscillations can be controlled by the chirp in the pump pulse, the effects of probe pulse chirp have not been fully investigated. In this paper we show, both theoretically and experimentally, that a pump-probe experiment using strongly-chirped probe pulses can preserve the temporal resolution of the TL pulses.
We present a time-domain treatment of pump–probe experiments with chirped pulses derived from the same laser source. In this theory we treat the nonlinearities as decaying either instantaneously or exponentially. Therefore the results from it cover different mechanisms originating from electronic orbitals, molecular vibrations, molecular orientations, excited-state populations, etc., as long as their decay falls into one of the two classes. We derive expressions for the transmission of the probe in each case. We divide the transmission expression from nonlinearities with exponential decay into a number of terms, each of which describes a unique situation. These include two-beam coupling in the coherent region that is not present with chirp-free pulses, two-photon absorption, and excited-state absorption. We give analytical expressions for the transmission where possible, and we give the first-order approximation and the estimated error when expression in closed form is unattainable. We discuss various aspects of these terms.
We demonstrate that frequency-chirped laser excitation pulses may be employed to generate coherent transient signals possessing the same temporal profile as a particular excitation pulse. In comparison with the short, fixedfrequency pulses used in previous studies of this effect, chirped pulses can be temporally longer, of lower intensity, and hence easier to generate. The experiment was performed on the 555.6-nm transition of vapor-phase atomic ytterbium, and pulse-shape information was stored in a coherence between excited-state Zeeman levels. A simple theoretical analysis of our results is presented.