The nuclear magnetic resonance of both the lanthanum and hydrogen nuclei in the lanthanum-hydrogen system has been studied as a function of hydrogen concentration and temperature. The concentrations ranged from 0.4 H/La to 2.85 H/ La and temperatures -197 deg C to 400 deg C. The existence of two phases, part La metal and part LaH/sub 2.0/ for concentrations with less than 2 H/La, is confirmed. Measurements of the proton linewidth and thermal relaxation time T/ sub 1/ unambiguously demonstrate that proton self-diffusion takes piace at moderate temperatures. Activation energies and attempt frequencies for the proton self-diffusion, which are determined as a function of hydrogen concentration, decrease abruptly at approximately 2 H/La from 23 kcal/mole and 10/sup 14/ sec/sup -1/, respectiveiy, to 3 kcal/mole and 10/sup 11/ sec/sup -1/at 2.85 H/La. The proton static linewidths vary continuousiy from 7.8 g at 2 H/La to 12.4 g at 2.85 H/La and the proton T/sub 1/ has a characteristic self- diffusion induced minimum of approximately 5 to 8 msec and a maximum of approximately 100 msec where spin diffusion to paramagnetic impurities dominates. The self-diffusing protons have a pronounced effect, via a quadrupole interaction, on the La resonances. For hydrogen concentrations slightlymore » greater than 2 H/La, a broadening and then narrowing again of the La linewidth, and a decrease with a subsequent recovery of the La Knight shift is observed as the proton self-diffusion rate increases with temperature. For concentrations greater than 2.4 H/ La, no La resonance is observed until a sufficiently high proton self-diffusion rate is attained to average out the quadrupolar effects. A detailed semiquantitative analysis incorporating the proton resonance data is made of these quadrupolar effects. At 400 deg C the La Knight shift is found to decrease from 0.23% for 2 H/La to 0.10% for 2.85 H/La while no Knight shift is observed for the proton resonance at any concentration or temperature. The thermal relaxation time of the La resonance in LaH/sub 2.0/ is found to be the result of a conduction electron hyperfine interaction with T/sub 1/T = 11.3 sec deg K when the protons are static. With proton motion the La T/sub 1/ decreases exponentially to a value somewhat greater than the La T/sub 2/ or about 100 mu sec at 400 deg C. A schematic picture of the band structure of the hydride consistent with the available data is suggested, based on an ionized hydrogen atom or proton, whose electron goes into a conduction band localized on the La ion. (auth)« less