Bending and Breaking of Stripes in a Charge-Ordered Manganite

In complex electronic materials, coupling between electrons and the atomic lattice gives rise to remarkable phenomena, including colossal magnetoresistance and metal-insulator transitions. Charge-ordered phases are a prototypical manifestation of charge-lattice coupling, in which the atomic lattice undergoes periodic lattice displacements (PLDs). Here we directly map the picometer scale PLDs at individual atomic columns in the room temperature charge-ordered manganite Bi$_{0.35}$Sr$_{0.18}$Ca$_{0.47}$MnO$_3$ using aberration corrected scanning transmission electron microscopy (STEM). We measure transverse, displacive lattice modulations of the cations, distinct from existing manganite charge-order models. We reveal locally unidirectional striped PLD domains as small as $\sim$5 nm, despite apparent bidirectionality over larger length scales. Further, we observe a direct link between disorder in one lattice modulation, in the form of dislocations and shear deformations, and nascent order in the perpendicular modulation. By examining the defects and symmetries of PLDs near the charge-ordering phase transition, we directly visualize the local competition underpinning spatial heterogeneity in a complex oxide.Comment: Main text: 20 pages, 4 figures. Supplemental Information: 27 pages, 14 figure

Commensurate Stripes and Phase Coherence in Manganites Revealed with Cryogenic Scanning Transmission Electron Microscopy

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 order in a manganite using scanning transmission electron microscopy at room temperature and cryogenic temperature ($\sim$ 93K). In diffraction, the ordering wavevector changes upon cooling, a behavior typically associated with incommensurate order. However, using real space measurements, we discover that the underlying ordered state is lattice-commensurate at both temperatures. The cations undergo picometer-scale ($\sim$6-11 pm) transverse displacements, which suggests that charge-lattice coupling is strong and hence favors lattice-locked modulations. We further unearth phase inhomogeneity in the periodic lattice displacements at room temperature, and emergent phase coherence at 93K. Such local phase variations not only govern the long range correlations of the charge-ordered state, but also results in apparent shifts in the ordering wavevector. These atomically-resolved observations underscore the importance of lattice coupling and provide a microscopic explanation for putative "incommensurate" order in hole-doped oxides

Charge order textures induced by non-linear lattice coupling in a half-doped manganite

The self-organization of strongly interacting electrons into superlattice structures underlies the properties of many quantum materials. How these electrons arrange within the superlattice dictates what symmetries are broken and what ground states are stabilized. Here we show that cryogenic scanning transmission electron microscopy enables direct mapping of local symmetries and order at the intra-unit-cell level in the model charge-ordered system Nd$_{1/2}$Sr$_{1/2}$MnO$_{3}$. In addition to imaging the prototypical site-centered charge order, we discover the nanoscale coexistence of an exotic intermediate state which mixes site and bond order and breaks inversion symmetry. We further show that nonlinear coupling of distinct lattice modes controls the selection between competing ground states. The results demonstrate the importance of lattice coupling for understanding and manipulating the character of electronic self-organization and highlight a novel method for probing local order in a broad range of strongly correlated systems

Endotaxial Stabilization of 2D Charge Density Waves with Long-range Order

Charge density waves are emergent quantum states that spontaneously reduce crystal symmetry, drive metal-insulator transitions, and precede superconductivity. In low-dimensions, distinct quantum states arise, however, thermal fluctuations and external disorder destroy long-range order. Here we stabilize ordered two-dimensional (2D) charge density waves through endotaxial synthesis of confined monolayers of 1T-TaS$_2$. Specifically, an ordered incommensurate charge density wave (oIC-CDW) is realized in 2D with dramatically enhanced amplitude and resistivity. By enhancing CDW order, the hexatic nature of charge density waves becomes observable. Upon heating via in-situ TEM, the CDW continuously melts in a reversible hexatic process wherein topological defects form in the charge density wave. From these results, new regimes of the CDW phase diagram for 1T-TaS$_2$ are derived and consistent with the predicted emergence of vestigial quantum order

Author Correction: Limits to the strain engineering of layered square-planar nickelate thin films

Correction to: Nature Communicationshttps://doi.org/10.1038/s41467-023-37117-4, published online 16 March 2023 In the Acknowledgements section of this article the grant number relating to NSF was incorrectly given as DMR 2045826 and should have been DMR-2045826. The original article has been corrected

Antiferromagnetic metal phase in an electron-doped rare-earth nickelate

Long viewed as passive elements, antiferromagnetic materials have emerged as promising candidates for spintronic devices due to their insensitivity to external fields and potential for high-speed switching. Recent work exploiting spin and orbital effects has identified ways to electrically control and probe the spins in metallic antiferromagnets, especially in noncollinear or noncentrosymmetric spin structures. The rare earth nickelate NdNiO3 is known to be a noncollinear antiferromagnet where the onset of antiferromagnetic ordering is concomitant with a transition to an insulating state. Here, we find that for low electron doping, the magnetic order on the nickel site is preserved while electronically a new metallic phase is induced. We show that this metallic phase has a Fermi surface that is mostly gapped by an electronic reconstruction driven by the bond disproportionation. Furthermore, we demonstrate the ability to write to and read from the spin structure via a large zero-field planar Hall effect. Our results expand the already rich phase diagram of the rare-earth nickelates and may enable spintronics applications in this family of correlated oxides.Comment: 25 pages, 4 figure

The Future of the Correlated Electron Problem

The understanding of material systems with strong electron-electron interactions is the central problem in modern condensed matter physics. Despite this, the essential physics of many of these materials is still not understood and we have no overall perspective on their properties. Moreover, we have very little ability to make predictions in this class of systems. In this manuscript we share our personal views of what the major open problems are in correlated electron systems and we discuss some possible routes to make progress in this rich and fascinating field. This manuscript is the result of the vigorous discussions and deliberations that took place at Johns Hopkins University during a three-day workshop January 27, 28, and 29, 2020 that brought together six senior scientists and 46 more junior scientists. Our hope, is that the topics we have presented will provide inspiration for others working in this field and motivation for the idea that significant progress can be made on very hard problems if we focus our collective energies.Comment: 55 pages, 19 figure