Raman spectroscopic investigations are carried out on LiNaSO4 up to a press
ure of 140 kbar. The behavior of the internal modes as a function of pressu
re suggests a structural transition at 22 +/- 2 kbar. Further, the evolutio
n of the Raman spectra suggests that the sulphate ions in the high pressure
phase are orientationally disordered in the beginning. Upon subsequent inc
rease of pressure, the misoriented sulphate ions are found to gradually ord
er, and at pressures above 90 kbar, the system gets completely ordered. Com
parison of the present results with the high pressure behavior of other bin
ary and disulphates reveal that the increase in cationic size ratio beyond
a critical value leads to orientational disordering in the high pressure ph
ases. (C) 1999 Elsevier Science Ltd. All rights reserved.