The defect structure of Lithium niobate, a phase of variable compositi
on, was studied by differential thermal analysis, second harmonic gene
ration measurements, Raman spectroscopy, and x-ray diffraction. The ni
obium ions occupying lithium sites along the polar axis are expected t
o produce the highest degree of disorder in the structure of lithium n
iobate. Structural perfection of lithium niobate can be improved by ra
ising Lithium content or by doping with cations which occupy Lithium s
ites.