@article{12520, author = {Daniel Slaughter and F. Sturm and Roger Bello and K.A. Larsen and N. Shivaram and C. McCurdy and Robert Lucchese and L. Martin and C.W. Hogle and Margaret Murnane and Henry Kapteyn and Predrag Ranitovic and Thorsten Weber}, title = {Nonequilibrium dissociative dynamics of D2 in two-color, few-photon excitation and ionization}, abstract = {D2 molecules, excited by linearly cross-polarized femtosecond extreme ultraviolet (XUV) and near-infrared (NIR) light pulses, reveal highly structured D+ ion fragment momenta and angular distributions that originate from two different 4-step dissociative ionization pathways after four photon absorption (1 XUV + 3 NIR). We show that, even for very low dissociation kinetic energy release ≤~240~meV, specific electronic excitation pathways can be identified and isolated in the final ion momentum distributions. With the aid of {\it ab initio} electronic structure and time-dependent Schrödinger equation calculations, angular momentum, energy, and parity conservation are used to identify the excited neutral molecular states and molecular orientations relative to the polarization vectors in these different photoexcitation and dissociation sequences of the neutral D2 molecule and its D+2 cation. In one sequential photodissociation pathway, molecules aligned along either of the two light polarization vectors are excluded, while another pathway selects molecules aligned parallel to the light propagation direction. The evolution of the nuclear wave packet on the intermediate \Bstate electronic state of the neutral D2 molecule is also probed in real time.}, year = {2021}, journal = {Physical Review Research}, volume = {3}, pages = {033191}, month = {2021-08}, url = {https://journals.aps.org/prresearch/abstract/10.1103/PhysRevResearch.3.033191}, doi = {10.1103/PhysRevResearch.3.033191}, }