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1. Stress accumulation versus shape flattening in frustrated, warped-jigsaw particle assemblies

   https://doi.org/10.1088/1367-2630/ac753e  

   Spivack, Isaac R ; Hall, Douglas M ; Grason, Gregory M ( June 2022 , New Journal of Physics)

   Abstract Geometrically frustrated assembly has emerged as an attractive paradigm for understanding and engineering assemblies with self-limiting, finite equilibrium dimensions. We propose and study a novel 2D particle based on a so-called ‘warped jigsaw’ (WJ) shape design: directional bonds in a tapered particle favor curvature along multi-particle rows that frustrate 2D lattice order. We investigate how large-scale intra-assembly stress gradients emerge from the microscopic properties of the particles using a combination of numerical simulation and continuum elasticity. WJ particles can favor anisotropic ribbon assemblies, whose lateral width may be self-limiting depending on the relative strength of cohesive to elastic forces in the assembly, which we show to be controlled by the range of interactions and degree of shape misfit. The upper limits of self-limited size are controlled by the crossover between two elastic modes in assembly: the accumulation of shear with increasing width at small widths giving way to unbending of preferred row curvature, permitting assembly to grow to unlimited sizes. We show that the stiffness controlling distinct elastic modes is governed by combination and placement of repulsive and attractive binding regions, providing a means to extend the range of accumulating stress to sizes that are far in excess ofmore »the single particle size, which we corroborate via numerical studies of discrete particles of variable interactions. Lastly, we relate the ground-state energetics of the model to lower and upper limits on equilibrium assembly size control set by the fluctuations of width along the ribbon boundary.« less
2. Shaping nanoparticle fingerprints at the interface of cholesteric droplets

   https://doi.org/10.1126/sciadv.aat8597  

   Tran, Lisa ; Kim, Hye-Na ; Li, Ningwei ; Yang, Shu ; Stebe, Kathleen J. ; Kamien, Randall D. ; Haase, Martin F. ( October 2018 , Science Advances)

   The ordering of nanoparticles into predetermined configurations is of importance to the design of advanced technologies. Here, we balance the interfacial energy of nanoparticles against the elastic energy of cholesteric liquid crystals to dynamically shape nanoparticle assemblies at a fluid interface. By adjusting the concentration of surfactant that plays the dual role of tuning the degree of nanoparticle hydrophobicity and altering the molecular anchoring of liquid crystals, we pattern nanoparticles at the interface of cholesteric liquid crystal emulsions. In this system, interfacial assembly is tempered by elastic patterns that arise from the geometric frustration of confined cholesterics. Patterns are tunable by varying both surfactant and chiral dopant concentrations. Adjusting the particle hydrophobicity more finely by regulating the surfactant concentration and solution pH further modifies the rigidity of assemblies, giving rise to surprising assembly dynamics dictated by the underlying elasticity of the cholesteric. Because particle assembly occurs at the interface with the desired structures exposed to the surrounding water solution, we demonstrate that particles can be readily cross-linked and manipulated, forming structures that retain their shape under external perturbations. This study serves as a foundation for better understanding inter-nanoparticle interactions at interfaces by tempering their assembly with elasticity and for creatingmore »materials with chemical heterogeneity and linear, periodic structures, essential for optical and energy applications.« less
3. Compositional Influence of Local and Long-Range Polarity in the Frustrated Pyrochlore System Bi _2−x RE xTi ₂ O ₇ ( RE = Y ³⁺ , Ho ³⁺ )

   https://doi.org/10.1039/D2TC01328B  

   Bailey, Owen ; Husremovic, Samra ; Murphy, Madison ; Ross, Jason ; Gong, Joyce ; Olds, Daniel ; Laurita, Geneva ( July 2022 , Journal of Materials Chemistry C)

   Structural distortions such as cation off-centering are frustrated in the pyrochlore structure due to the triangular arrangement of cations on the pyrochlore lattice. This geometric constraint inhibits a transition from a paraelectric to ferroelectric phase in majority of pyrochlore oxide materials. Few pyrochlore materials can overcome this frustration and exhibit polar crystal structures, and unraveling the origin of such leads to the understanding of polarity in complex materials. Herein we hypothesize that frustration on the pyrochlore lattice can be relieved through A -site doping with rare earth cations that do not possess stereochemically active lone pairs. To assess if frustration is relieved, we have analyzed cation off-centering in various Bi 2−x RE xTi 2 O 7 ( RE = Y 3+ , Ho 3+ ) pyrochlores through neutron and X-ray total scattering. Motivated by known distortions from the pyrochlore literature, we present our findings that most samples show local distortions similar to the β-cristobalite structure. We additionally comment on the complexity of factors that play a role in the structural behavior, including cation size, bond valence, electronic structure, and magnetoelectronic interactions. We posit that the addition of magnetic cations on the pyrochlore lattice may play a role in an extensionmore »of the real-space correlation length of electric dipoles in the Bi-Ho series, and offer considerations for driving long-range polarity on the pyrochlore lattice.« less
4. Rheological implications of embedded active matter in colloidal gels

   https://doi.org/10.1039/c9sm01496a  

   Szakasits, Megan E. ; Saud, Keara T. ; Mao, Xiaoming ; Solomon, Michael J. ( October 2019 , Soft Matter)

   Colloidal gels represent an important class of soft matter, in which networks formed due to strong, short-range interactions display solid-like mechanical properties, such as a finite low-frequency elastic modulus. Here we examine the effect of embedded active colloids on the linear viscoelastic moduli of fractal cluster colloidal gels. We find that the autonomous, out-of-equilibrium dynamics of active colloids incorporated into the colloidal network decreases gel elasticity, in contrast to observed stiffening effects of myosin motors in actin networks. Fractal cluster gels are formed by the well-known mechanism of aggregating polystyrene colloids through addition of divalent electrolyte. Active Janus particles with a platinum hemisphere are created from the same polystyrene colloids and homogeneously embedded in the gels at dilute concentration at the time of aggregation. Upon addition of hydrogen peroxide – a fuel that drives the diffusiophoretic motion of the embedded Janus particles – the microdynamics and mechanical rheology change in proportion to the concentration of hydrogen peroxide and the number of active colloids. We propose a theoretical explanation of this effect in which the decrease in modulus is mediated by active motion-induced softening of the inter-particle attraction. Furthermore, we characterize the failure of the fluctuation–dissipation theorem in the active gelsmore »by identifying a discrepancy between the frequency-dependent macroscopic viscoelastic moduli and the values predicted by microrheology from measurement of the gel microdynamics. These findings support efforts to engineer gels for autonomous function by tuning the microscopic dynamics of embedded active particles. Such reconfigurable gels, with multi-state mechanical properties, could find application in materials such as paints and coatings, pharmaceuticals, self-healing materials, and soft robotics.« less
5. Stranger than metals

   https://doi.org/10.1126/science.abh4273  

   Phillips, Philip W. ; Hussey, Nigel E. ; Abbamonte, Peter ( July 2022 , Science)

   BACKGROUND Landau’s Fermi liquid theory provides the bedrock on which our understanding of metals has developed over the past 65 years. Its basic premise is that the electrons transporting a current can be treated as “quasiparticles”—electron-like particles whose effective mass has been modified, typically through interactions with the atomic lattice and/or other electrons. For a long time, it seemed as though Landau’s theory could account for all the many-body interactions that exist inside a metal, even in the so-called heavy fermion systems whose quasiparticle mass can be up to three orders of magnitude heavier than the electron’s mass. Fermi liquid theory also lay the foundation for the first successful microscopic theory of superconductivity. In the past few decades, a number of new metallic systems have been discovered that violate this paradigm. The violation is most evident in the way that the electrical resistivity changes with temperature or magnetic field. In normal metals in which electrons are the charge carriers, the resistivity increases with increasing temperature but saturates, both at low temperatures (because the quantized lattice vibrations are frozen out) and at high temperatures (because the electron mean free path dips below the smallest scattering pathway defined by the lattice spacing).more »In “strange metals,” by contrast, no saturation occurs, implying that the quasiparticle description breaks down and electrons are no longer the primary charge carriers. When the particle picture breaks down, no local entity carries the current. ADVANCES A new classification of metallicity is not a purely academic exercise, however, as strange metals tend to be the high-temperature phase of some of the best superconductors available. Understanding high-temperature superconductivity stands as a grand challenge because its resolution is fundamentally rooted in the physics of strong interactions, a regime where electrons no longer move independently. Precisely what new emergent phenomena one obtains from the interactions that drive the electron dynamics above the temperature where they superconduct is one of the most urgent problems in physics, attracting the attention of condensed matter physicists as well as string theorists. One thing is clear in this regime: The particle picture breaks down. As particles and locality are typically related, the strange metal raises the distinct possibility that its resolution must abandon the basic building blocks of quantum theory. We review the experimental and theoretical studies that have shaped our current understanding of the emergent strongly interacting physics realized in a host of strange metals, with a special focus on their poster-child: the copper oxide high-temperature superconductors. Experiments are highlighted that attempt to link the phenomenon of nonsaturating resistivity to parameter-free universal physics. A key experimental observation in such materials is that removing a single electron affects the spectrum at all energy scales, not just the low-energy sector as in a Fermi liquid. It is observations of this sort that reinforce the breakdown of the single-particle concept. On the theoretical side, the modern accounts that borrow from the conjecture that strongly interacting physics is really about gravity are discussed extensively, as they have been the most successful thus far in describing the range of physics displayed by strange metals. The foray into gravity models is not just a pipe dream because in such constructions, no particle interpretation is given to the charge density. As the breakdown of the independent-particle picture is central to the strange metal, the gravity constructions are a natural tool to make progress on this problem. Possible experimental tests of this conjecture are also outlined. OUTLOOK As more strange metals emerge and their physical properties come under the scrutiny of the vast array of experimental probes now at our disposal, their mysteries will be revealed and their commonalities and differences cataloged. In so doing, we should be able to understand the universality of strange metal physics. At the same time, the anomalous nature of their superconducting state will become apparent, offering us hope that a new paradigm of pairing of non-quasiparticles will also be formalized. The correlation between the strength of the linear-in-temperature resistivity in cuprate strange metals and their corresponding superfluid density, as revealed here, certainly hints at a fundamental link between the nature of strange metallicity and superconductivity in the cuprates. And as the gravity-inspired theories mature and overcome the challenge of projecting their powerful mathematical machinery onto the appropriate crystallographic lattice, so too will we hope to build with confidence a complete theory of strange metals as they emerge from the horizon of a black hole. Curved spacetime with a black hole in its interior and the strange metal arising on the boundary. This picture is based on the string theory gauge-gravity duality conjecture by J. Maldacena, which states that some strongly interacting quantum mechanical systems can be studied by replacing them with classical gravity in a spacetime in one higher dimension. The conjecture was made possible by thinking about some of the fundamental components of string theory, namely D-branes (the horseshoe-shaped object terminating on a flat surface in the interior of the spacetime). A key surprise of this conjecture is that aspects of condensed matter systems in which the electrons interact strongly—such as strange metals—can be studied using gravity.« less