Percolative phase separation induced by nonuniformly distributed excess oxygen in low-doped La1-xCaxMnO3+delta (x <= 0.2)

The zero-field $^{139}$La and $^{55}$Mn nuclear magnetic resonances were studied in $\rm La_{0.8}Ca_{0.2}MnO_{3+\delta}$ with different oxygen stoichiometry $\delta$. The signal intensity, peak frequency and line broadening of the $^{139}$La NMR spectrum show that excess oxygens have a tendency to concentrate and establish local ferromagnetic ordering around themselves. These connect the previously existed ferromagnetic clusters embedded in the antiferromagnetic host, resulting in percolative conduction paths. This phase separation is not a charge segregation type, but a electroneutral type. The magnetoresistance peak at the temperature where percolative paths start to form provides a direct evidence that phase separation is one source of colossal magnetoresistance effect.