In an effort to elucidate the origin of the Curie-like paramagnetism that is
generic for heavily-overdoped cuprates, we have performed high transverse-field
muon spin rotation (TF-muSR) measurements of La2-xSrxCuO4 single crystals over
the Sr content range 0.145 < x < 0.33. We show that the x-dependence of the
previously observed field-induced broadening of the internal magnetic field
distribution above the superconducting transition temperature Tc reflects the
presence of two distinct contributions. One of these becomes less pronounced
with increasing x and is attributed to diminishing antiferromagnetic
correlations. The other grows with increasing x, but decreases above x ~ 0.30,
and is associated with the Curie-like term in the bulk magnetic susceptibility.
In contrast to the Curie-like term, however, this second contribution to the
TF-muSR line width extends back into the underdoped regime. Our findings imply
a coexistence of antiferromagnetically correlated and paramagnetic moments,
with the latter becoming dominant beyond x ~ 0.185. This suggests that the
doped holes do not neutralize all Cu spins via the formation of Zhang-Rice
singlets. Moreover, the paramagnetic component of the TF-muSR line width is
explained by holes progressively entering the Cu 3d_{x^2-y^2} orbital with
doping.Comment: 8 pages, 7 figure
