Attosecond science promises to allow new forms of quantum control in which a broadband isolated attosecond pulse excites a molecular wave packet consisting of a coherent superposition of multiple excited electronic states. This electronic excitation triggers nuclear motion on the molecular manifold of potential energy surfaces and can result in permanent rearrangement of the constituent atoms. Here, we demonstrate attosecond transient absorption spectroscopy (ATAS) as a viable probe of the electronic and nuclear dynamics initiated in excited states of a neutral molecule by a broadband vacuum ultraviolet pulse. Owing to the high spectral and temporal resolution of ATAS, we are able to reconstruct the time evolution of a vibrational wave packet within the excited $B^{\prime }{}^1\mathrm{\Sigma }_u{}^{+}$ electronic state of ${\mathrm{H}}_2$ via the laser-perturbed transient absorption spectrum.

• Received 11 May 2016

DOI:https://doi.org/10.1103/PhysRevA.94.023403