Abstract We present a theoretical study on the quantum control of ultrafast Rabi dynamics in atoms driven by chirped extreme ultraviolet (XUV) pulses. Motivated by recent experimental advances using free-electron lasers, we derive an analytical solution of the Rabi oscillation under the rotating wave approximation, incorporating the spectral chirp of the XUV field. Within the essential-states model, we demonstrate how the chirp modulates the phase of the excited-state amplitude, inducing an observable asymmetry in the Autler–Townes (AT) doublets of the photoelectrons. Our theoretical predictions, benchmarked against time-dependent Schrödinger equation simulations, reveal that chirp-dependent phase modulation governs the spectral asymmetry, offering a time-domain perspective for interpreting strong-field photoionization at short wavelengths. This work provides a compact analytical framework for chirp-mediated coherent control in the XUV regime and sheds light on recent experimental observations of asymmetric AT structures in helium.
Traditional schemes for coherent population transfer or generation of coherent superposition states in multilevel atoms or molecules usually utilize two or more laser beams with radiation bandwidth smaller than the frequency interval between the working levels. We show the possibility of creation of the coherent superposition of three metastable states of a four-level atom with tripodlike level structure using a single short frequency-chirped laser pulse. The bandwidth of the pulse envelope (without chirp) must be comparable to or exceed the frequency distance between the two metastable levels. No appreciable excitation of the atom takes place during the creation of the coherent superposition state, thus diminishing significantly the effect of decoherence due to the spontaneous decay of the excited state. The proposed method of creation of superposition states is robust against variations in the laser pulse parameters. Since this method does not require maintaining steady resonance with the atomic transitions (owing to the frequency chirp of the laser pulse), it is effective both in homogeneously and inhomogeneously broadened media.
We investigate the behavior of
85Rb atoms in the field of a sequence of frequency-chirped short laser pulses. The analysis is based on a numerical solution of equations for the probability amplitudes of the hyperfine levels of the ${5S}_{1/2}{\ensuremath{-}5P}_{3/2}$ transition in the
85Rb atom and the dressed-states analysis. We analyze different regimes of interaction, including relatively short laser pulses (when the width of the pulse envelope spectrum is of the order of or exceeds the frequency interval between the hyperfine levels resulting in effective mixing of them) and relatively long ones (when the ground hyperfine levels are resolved but the excited ones are not resolved). In the latter case dependence of the population transfer efficiency on the initial coherence of the ground states is analyzed. The case of long laser pulses when all working hyperfine levels are resolved is also discussed using numerical simulations and a dressed-states analysis. We show that in all regimes considered, the interaction of a frequency-chirped laser pulse with the multilevel
85Rb system is similar to the interaction with an effective two-level atom at sufficiently large peak intensities of the pulses. It allows us to perform efficient excitation of the multilevel atom by transferring populations of two hyperfine ground states to the excited ones and back to the ground states using a pair of frequency-chirped laser pulses. We propose to utilize this scheme of population transfer for the coherent manipulation of a beam of
85Rb atoms using sequences of counterpropagating frequency-chirped short laser pulses.