C. Turc et al., EFFECT OF ORIENTATIONAL AND SUBSTITUTIONAL DISORDERS ON THE N2 VIBRATIONAL EXCITON IN N2 CO MIXED-CRYSTALS/, Chemical physics, 161(1-2), 1992, pp. 39-50
High resolution Raman spectroscopy was performed on the N2 vibron band
s over a large concentration range at various temperatures in N2/CO mi
xed crystals. The Davydov splitting appears for N2 concentration above
0.2 and linearly increases up to the pure crystal limit. The Raman li
newidth exhibits a maximum for a N2 concentration of 0.15 and decrease
s towards a residual value in the low concentration limit. Two types o
f disorder for the asymmetric CO molecules. A Hamiltonian including co
rrelated diagonal and off-diagonal disorder terms was suggested to des
cribe the vibron band. The first moments of the Raman intensity were c
alculated as a function of the concentration. The first moment account
s for the linear dependence of the Davydov splitting in terms of the c
oncentration. The second moment predicts the residual bandwidth in the
low N2 concentration limit which is proved to result from the orienta
tional disorder of the CO molecules.