We show how to emulate a conventional pump-probe scheme using a single frequency-chirped ultrashort UV pulse to obtain a time-resolved image of molecular ultrafast dynamics. The chirp introduces a spectral phase in time that encodes the delay between the pump and the probe frequencies contained in the pulse. By comparing the results of full dimensional ab initio calculations for the ${\mathrm{H}}_2{}^{+}$ molecule with those of a simple sequential model, we demonstrate that, by tuning the chirp parameter, two-photon energy-differential ionization probabilities directly map the wave-packet dynamics generated in the molecule. As a result, one can also achieve a significant amount of control of the total ionization yields, with a possible enhancement by more than an order of magnitude.

• Received 6 February 2017

DOI:https://doi.org/10.1103/PhysRevA.95.043424