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In an effort to elucidate the origin of the Curie-like paramagnetism that isgeneric for heavily-overdoped cuprates, we have performed high transverse-fieldmuon spin rotation (TF-muSR) measurements of La2-xSrxCuO4 single crystals overthe Sr content range 0.145 < x < 0.33. We show that the x-dependence of thepreviously observed field-induced broadening of the internal magnetic fielddistribution above the superconducting transition temperature Tc reflects thepresence of two distinct contributions. One of these becomes less pronouncedwith increasing x and is attributed to diminishing antiferromagneticcorrelations. 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 theTF-muSR line width extends back into the underdoped regime. Our findings implya coexistence of antiferromagnetically correlated and paramagnetic moments,with the latter becoming dominant beyond x ~ 0.185. This suggests that thedoped holes do not neutralize all Cu spins via the formation of Zhang-Ricesinglets. Moreover, the paramagnetic component of the TF-muSR line width isexplained by holes progressively entering the Cu 3d_{x^2-y^2} orbital withdoping.

Curie-like paramagnetism due to incomplete Zhang-Rice singlet formation in La2-xSrxCuO4