The mechanism of high-transition-temperature (high-Tc) superconductivity in doped copper oxides is an enduring problem. Antiferromagnetism is established as the competing order1,2, but the relationship between the two states in the intervening ‘pseudogap’ regime has become a central puzzle3. The role of the crystal lattice, which is important in conventional superconductors, also remains unclear. Here we report an anomalous increase of the distance between copper oxide planes on cooling, which results in negative thermal volume expansion, for layered ruthenium copper oxides4,5 that have been doped to the boundary of antiferromagnetism and superconductivity. We propose that a crossover between these states is driven by spin ordering in the ruthenium oxide layers, revealing a novel mechanism for negative lattice expansion in solids. The differences in volume and lattice strain between the distinct superconducting and antiferromagnetic states can account for the phase segregation phenomena found extensively in low-doped copper oxides, and show that Cooper pair formation is coupled to the lattice. Unusually large variations of resistivity with magnetic field are found in these ruthenium copper oxides at low temperatures through coupling between the ordered Ru and Cu spins.
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We thank P. Littlewood, P. Monthoux and N. Mathur for discussions, and P. Henry and E. Suard for assistance with the neutron experiments. We also acknowledge the Royal Society of Edinburgh for a SEELLD research fellowship (A.C.M.), the Ministry of Science and Technology, Government of Pakistan for a studentship (F.S.), and the UK EPSRC for beam time provision and financial support.
Reprints and permissions information is available at npg.nature.com/reprintsandpermissions. The authors declare no competing financial interests.
Two tables containing refinement parameters and derived quantities such as bond distances for RuSr2Nd0.9 Ce0.9Y0.2Cu2O10, from slow warming neutron diffraction data at temperatures from 4 to 290 K. (DOC 37 kb)
Figures S1-S6, showing profile fits and magnetic peak variations from the neutron diffraction analysis of RuSr2Nd0.9 Ce0.9Y0.2Cu2O10 and other ruthenocuprates; also magnetisation and magneto-transport data for RuSr2Nd0.9 Ce0.9Y0.2Cu2O10. (DOC 968 kb)
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Mclaughlin, A., Sher, F. & Attfield, J. Negative lattice expansion from the superconductivity–antiferromagnetism crossover in ruthenium copper oxides. Nature 436, 829–832 (2005). https://doi.org/10.1038/nature03828
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