Abstract
Charge carriers in low-doped semiconductors may distort the atomic lattice around them and through this interaction form so-called small polarons1,2. High carrier concentrations on the other hand can lead to short-range ordered polarons (large polarons)3,4 and even to a long-range charge and orbital order5. These ordered systems should be insulating with a large electrical resistivity6. However, recently a polaronic pseudogap was found in a metallic phase of La2−2xSr1+2xMn2O7 (ref. 7). This layered manganite is famous for colossal magnetoresistance associated with a phase transition from this low-temperature metallic phase to a high-temperature insulating phase7,8,9. Broad charge-order peaks due to large polarons in the insulating phase disappear when La2−2xSr1+2xMn2O7 becomes metallic10. Investigating how polaronic features survive in the metallic phase, here we report the results of inelastic neutron scattering measurements showing that inside the metallic phase polarons remain as fluctuations that strongly broaden and soften certain phonons near the wavevectors where the charge-order peaks appeared in the insulating phase. Our findings imply that polaronic signatures in metals may generally come from a competing insulating charge-ordered phase. Our findings are highly relevant to cuprate superconductors with both a pseudogap11,12 and a similar phonon effect associated with a competing stripe order13.
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Acknowledgements
The authors would like to thank M. Braden and L. Pintschovius for helpful discussions and suggestions, and M. Braden and W. Reichardt for allowing us to use shell model parameters for La2−2xSr1+2xMn2O7 that they found in a separate investigation. D.N.A. and D.R. thank Dan Dessau and Jan Zaanen for discussions. Work at Argonne National Laboratory was supported under Contract No. DE-AC02-06CH11357 by UChicago Argonne, LLC, Operator of Argonne National Laboratory, a US Department of Energy Office of Science Laboratory. N.A, was supported in part by the Hytrain Project of the Marie Curie Research Training Network funded under the EC’s 6th Framework Human Resources and Mobility Program.
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D.R. and D.N.A. conceived and oversaw the project. H.Z. and J.F.M. grew the single-crystal sample. The first measurements were carried out by F.W., N.A., D.N.A. and D.R. F.W. and D.R. carried out many further measurements. F.W. carried out the data analysis and lattice dynamics calculations. D.R. and D.N.A. wrote the manuscript with revisions from F.W. F.W. and D.R. prepared figures and Supplementary Information.
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Weber, F., Aliouane, N., Zheng, H. et al. Signature of checkerboard fluctuations in the phonon spectra of a possible polaronic metal La1.2Sr1.8Mn2O7. Nature Mater 8, 798–802 (2009). https://doi.org/10.1038/nmat2513
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DOI: https://doi.org/10.1038/nmat2513
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