Bilayer manganites reveal polarons in the midst of a metallic breakdown

The origin of colossal magnetoresistance (CMR) in manganese oxides is among the most challenging problems in condensed- matter physics today. The true nature of the low-temperature electronic phase of these materials is heavily debated. By combining photoemission and tunnelling data, we show that in the archetypal bilayer system La_2-2xSr_1+2xMn₂O₇, polaronic degrees of freedom win out across the CMR region of the phase diagram. This means that the generic ground state of bilayer manganites supports a vanishing coherent quasi-particle spectral weight at the Fermi level throughout k-space. The incoherence of the charge carriers, resulting from strong electron–lattice interactions and the accompanying orbital physics, offers a unifying explanation for the anomalous charge-carrier dynamics seen in transport, optics and electron spectroscopies. The stacking number N is the key factor for true metallic behaviour, as an intergrowth-driven breakdown of the polaronic domination to give a metal possessing a traditional Fermi surface is seen in this system.