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  1. Abstract

    Checkerboard lattices—where the resulting structure is open, porous, and highly symmetric—are difficult to create by self-assembly. Synthetic systems that adopt such structures typically rely on shape complementarity and site-specific chemical interactions that are only available to biomolecular systems (e.g., protein, DNA). Here we show the assembly of checkerboard lattices from colloidal nanocrystals that harness the effects of multiple, coupled physical forces at disparate length scales (interfacial, interparticle, and intermolecular) and that do not rely on chemical binding. Colloidal Ag nanocubes were bi-functionalized with mixtures of hydrophilic and hydrophobic surface ligands and subsequently assembled at an air–water interface. Using feedback between molecular dynamics simulations and interfacial assembly experiments, we achieve a periodic checkerboard mesostructure that represents a tiny fraction of the phase space associated with the polymer-grafted nanocrystals used in these experiments. In a broader context, this work expands our knowledge of non-specific nanocrystal interactions and presents a computation-guided strategy for designing self-assembling materials.

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  2. We present a novel heterostructured approach to disentangle the mechanism of electrical transport of the strongly correlated PrNiO3, by placing the nickelate under the photoconductor CdS. This enables the injection of carriers into PrNiO3 in a controlled way, which can be used to interrogate its intrinsic transport mechanism. We find a nonvolatile resistance decrease when illuminating the system at temperatures below the PrNiO3 metal-insulator transition. The photoinduced change becomes more volatile as the temperature increases. These data help understand the intrinsic transport properties of the nickelate-CdS bilayer. Together with data from a bare PrNiO3 film, we find that the transport mechanism includes a combination of mechanisms, including both thermal activation and variable range hopping. At low temperatures without photoinduced carriers, the transport is governed by hopping, while at higher temperatures and intense illumination the activation mechanism becomes relevant. This work shows a new way to control optically control the low-temperature resistance of PrNiO3. 
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    Free, publicly-accessible full text available December 1, 2024
  3. The Fe intercalated transition metal dichalcogenide (TMD), Fe 1 / 3 NbS 2 , exhibits remarkable resistance switching properties and highly tunable spin ordering phases due to magnetic defects. We conduct synchrotron x-ray scattering measurements on both underintercalated ( x = 0.32 ) and overintercalated ( x = 0.35 ) samples. We discover a new charge order phase in the overintercalated sample, where the excess Fe atoms lead to a zigzag antiferromagnetic order. The agreement between the charge and magnetic ordering temperatures, as well as their intensity relationship, suggests a strong magnetoelastic coupling as the mechanism for the charge ordering. Our results reveal the first example of a charge order phase among the intercalated TMD family and demonstrate the ability to stabilize charge modulation by introducing electronic correlations, where the charge order is absent in bulk 2 H − NbS 2 compared to other pristine TMDs. 
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    Free, publicly-accessible full text available October 1, 2024
  4. Most resonant inelastic x-ray scattering (RIXS) studies of dynamic charge order correlations in the cuprates have focused on the high-symmetry directions of the copper oxide plane. However, scattering along other in-plane directions should not be ignored as it may help understand, for example, the origin of charge order correlations or the isotropic scattering resulting in strange metal behavior. Our RIXS experiments reveal dynamic charge correlations over theqx-qyscattering plane in underdoped Bi2Sr2CaCu2O8+δ. Tracking the softening of the RIXS-measured bond-stretching phonon, we show that these dynamic correlations exist at energies below approximately 70 meV and are centered around a quasi-circular manifold in theqx-qyscattering plane with radius equal to the magnitude of the charge order wave vector,qCO. This phonon-tracking procedure also allows us to rule out fluctuations of short-range directional charge order (i.e., centered around [qx= ±qCO,qy= 0] and [qx= 0,qy= ±qCO]) as the origin of the observed correlations.

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    Free, publicly-accessible full text available July 21, 2024
  5. Mesoscopic antiferromagnetic domains are imaged using resonant coherent x-ray diffraction without phase reconstruction algorithm. 
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  6. Abstract

    The shape of 3d-orbitals often governs the electronic and magnetic properties of correlated transition metal oxides. In the superconducting cuprates, the planar confinement of the$${d}_{{x}^{2}-{y}^{2}}$$dx2y2orbital dictates the two-dimensional nature of the unconventional superconductivity and a competing charge order. Achieving orbital-specific control of the electronic structure to allow coupling pathways across adjacent planes would enable direct assessment of the role of dimensionality in the intertwined orders. Using CuL3and PrM5resonant x-ray scattering and first-principles calculations, we report a highly correlated three-dimensional charge order in Pr-substituted YBa2Cu3O7, where the Prf-electrons create a direct orbital bridge between CuO2planes. With this we demonstrate that interplanar orbital engineering can be used to surgically control electronic phases in correlated oxides and other layered materials.

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