Far-infrared absorption by phonons and librons in solid H2 and D2 in the ordered state

We present an experimental study of the infrared absorption spectra of solid, enriched ortho-hydrogen and para-deuterium in the ordered state for concentrations x of J = 1 molecules between 0.65 and 0.98 and temperatures from 0.9 to 11K. Comparison is made to theoretical expressions and numerical results for the absorption due to various microscopic processes, involving phonons and combinations oflibrons and phonons, which couple to the dipole moment induced by the electric quadrupole (EQ) fields of J = 1 molecules. The concentration dependence of the sharp, low-frequency optical phonon has also been studied. The integrated intensity of this feature is found to be quadratic in x and the frequency is well described by ω(x) = a + bx2,which is the expected behavior for shifts arising from pairwise EQQ interactions. For constant x, the temperature dependence of the intensity of this phonon scales with the square of the long-range orientational order parameter. Our measurements of this quantity are compared to NMR determinations of the temperature dependence of the Pake splitting in the ordered state.