Neutron scattering has been used to investigate the evolution of the long- and short-range charge-ordered (CO), ferromagnetic (FM), and antiferromagnetic (AF) correlations in single crystals of Pr1-xCaxMnO3. The existence and population of spin clusters as refected by short-range correlations are found to drastically depend on the doping (x) and temperature (T). Concentrated spin clusters coexist with long-range canted AF order in a wide temperature range in x = 0.3 while clusters do not appear in x = 0.4 crystal. In contrast, both CO and AF order parameters in the x = 0.35 crystal show a precipitous decrease below ~ 35 K where spin clusters form. These results provide direct evidence of magnetic phase separation and indicate that there is a critical doping x_c (close to x = 0.35) that divides the phase-separated site-centered from the homogeneous bond-centered or charge-disproportionated CO ground state.
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