Abstract
Charge order is a modulation of the electron density and is associated with unconventional phenomena, including colossal magnetoresistance and metal–insulator transitions. Determining how the lattice responds provides insights into the nature and symmetry of the ordered state. Scanning transmission electron microscopy can measure lattice displacements with picometer precision, but its use has been limited to room-temperature phases only. Here, we demonstrate high-resolution imaging at cryogenic temperature and map the nature and evolution of charge order in a manganite. We uncover picometer-scale displacive modulations whose periodicity is strongly locked to the lattice and visualize temperature-dependent phase inhomogeneity in the modulations. These results pave the way to understanding the underlying structure of charge-ordered states and other complex phenomena.
Incommensurate charge order in hole-doped oxides is intertwined with exotic phenomena such as colossal magnetoresistance, high-temperature superconductivity, and electronic nematicity. Here, we map, at atomic resolution, the nature of incommensurate charge–lattice order in a manganite using scanning transmission electron microscopy at room temperature and cryogenic temperature (
∼
93 K). In diffraction, the ordering wave vector changes upon cooling, a behavior typically associated with incommensurate order. However, using real space measurements, we discover that the ordered state forms lattice-locked regions over a few wavelengths interspersed with phase defects and changing periodicity. The cations undergo picometer-scale (
∼
6 pm to 11 pm) transverse displacements, suggesting that charge–lattice coupling is strong. We further unearth phase inhomogeneity in the periodic lattice displacements at room temperature, and emergent phase coherence at 93 K. Such local phase variations govern the long-range correlations of the charge-ordered state and locally change the periodicity of the modulations, resulting in wave vector shifts in reciprocal space. These atomically resolved observations underscore the importance of lattice coupling and phase inhomogeneity, and provide a microscopic explanation for putative “incommensurate” order in hole-doped oxides.