Competing spin-glass and spin-fluctuation states in NdxPr4-xNi3O8

Neodymium nickelates have attracted research interest due to their strongly correlated behaviour and remarkable magnetic properties. More importantly, superconductivity has recently been confirmed in thin-film samples of Sr-doped NdNiO2, bringing the layered rare earth nickel oxides into the research spotlight. In this report, we present results on a series of NdNiO2 analogues, NdxPr4-xNi3O8 (x = 0.1, 0.25, 1, 2, and 4) obtained by topotactic reduction, in which we observe systematic changes in the magnetic behaviour. As the Nd3+ content increases, the initially large spin-freezing region with magnetic frustration becomes smaller and gradually shifts to low temperatures, while the magnetic response gradually increases. The muon-spin spectroscopy measurements on Nd4Ni3O8 show that this phenomenon is likely due to the enhancement of spin fluctuations in NdxPr4-xNi3O8, which weakens the spin frustration behaviour for high Nd3+ contents and at low temperatures. These spin fluctuations can be caused by both Nd and Ni ions and could be one of the factors determining the occurrence of possible superconductivity.