The rotationally resolved infrared (IR) spectrum of D-2-OH in its ground electronic state has been obtained in the OH overtone region at 1.4 mu m via IR-ultraviolet (UV) action spectroscopy. The pure OH overtone and combination bands involving intermolecular bending excitation were observed. The experimental spectrum was compared with IR transition frequencies computed from ab initio theory for o-D-2-OH and p-D-2-OH. The state-selective IR excitation of D2-OH also serves to initiate inelastic and/or reactive scattering dynamics between the D-2 and OH partners under restricted initial orientation conditions. Time- and frequency-resolved measurements of the OH (v = 1) fragments from vibrational predissociation showed that vibrationally activated D2-OH is short-lived and that the D-2 fragment is vibrationally excited as a result of an efficient near-resonant vibration-to-vibration energy transfer process. The remaining 350 cm(-1) of available energy is disposed primarily as rotational excitation of OH. The OH fragments also exhibit a striking lambda-doublet preference, revealing alignment of the unpaired p pi orbital with respect to the OH rotation plane that changes with the intermolecular state selected. The results are consistent with half-collisions that sample different restricted angular regions of the OH + D-2 potential energy surface for each of the initially prepared states.