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At least 685 records · Page 38

Structural magnetic glassiness in the spin ice Dy 2 Ti 2 O 7

The origin and nature of glassy dynamics presents one of the central enigmas of condensed-matter physics across a broad range of systems ranging from window glass to spin glasses. The spin-ice compound Dy 2 Ti 2 O 7 , which is perhaps best known as hosting a three-dimensional Coulomb spin liquid with magnetically charged monopole excitations, also falls out of equilibrium at low temperature. How and why it does so remains an open question. Based on an analysis of low-temperature diffuse neutron-scattering experiments employing different cooling protocols alongside recent magnetic noise studies, combined with extensive numerical modeling, we argue that upon cooling, the spins freeze into what may be termed a “structural magnetic glass,” without an a priori need for chemical or structural disorder. Specifically, our model indicates the presence of frustration on two levels, first producing a near-degenerate constrained manifold inside which phase ordering kinetics is in turn frustrated. A remarkable feature is that monopoles act as sole annealers of the spin network and their pathways and history encode the development of glass dynamics, allowing the glass formation to be visualized. Our results suggest that spin ice Dy 2 Ti 2 O 7 provides one prototype of magnetic glass formation specifically and a setting for the study of kinetically constrained systems more generally.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Quasiclassical Theory of C4-Symmetric Magnetic Order in Disordered Multiband Metals

Recent experimental studies performed in the normal state of iron-based superconductors have discovered the existence of the C 4 -symmetric (tetragonal) itinerant magnetic state. This state can be described as a spin density wave with two distinct magnetic vectors Q → 1 and Q → 2 . Given an itinerant nature of magnetism in iron-pnictides, we develop a quasiclassical theory of tetragonal magnetic order in disordered three-band metal with anisotropic band structure. Within our model we find that the C 4 -symmetric magnetism competes with the C 2 -symmetric state with a single Q → magnetic structure vector. Our main results is that disorder promotes tetragonal magnetic state which is in agreement with earlier theoretical studies.

74.45.c, 74.50. r, 74.20.R↗

Structures of full-length VanR from Streptomyces coelicolor in both the inactive and activated states

Vancomycin has historically been used as a last-resort treatment for serious bacterial infections. However, vancomycin resistance has become widespread in certain pathogens, presenting a serious threat to public health. Resistance to vancomycin is conferred by a suite of resistance genes, the expression of which is controlled by the VanR–VanS two-component system. VanR is the response regulator in this system; in the presence of vancomycin, VanR accepts a phosphoryl group from VanS, thereby activating VanR as a transcription factor and inducing expression of the resistance genes. This paper presents the X-ray crystal structures of full-length VanR from Streptomyces coelicolor in both the inactive and activated states at resolutions of 2.3 and 2.0 Å, respectively. Comparison of the two structures illustrates that phosphorylation of VanR is accompanied by a disorder-to-order transition of helix 4, which lies within the receiver domain of the protein. This transition generates an interface that promotes dimerization of the receiver domain; dimerization in solution was verified using analytical ultracentrifugation. The inactive conformation of the protein does not appear intrinsically unable to bind DNA; rather, it is proposed that in the activated form DNA binding is enhanced by an avidity effect contributed by the receiver-domain dimerization.

59 BASIC BIOLOGICAL SCIENCES↗

From Three-Dimensional Clathrates to Two-Dimensional Zintl Phases AMSb 2 (A = Rb, Cs; M = Ga, In) Composed of Pentagonal M–Sb Rings

Three new antimonide Zintl phases, RbGaSb 2 , CsGaSb 2 , and CsInSb 2 , were discovered during exploration of corresponding A–M–Sb (A = Rb, Cs; M = Ga, In) ternary systems while searching for new clathrates. The AGaSb 2 phases crystallize in the tetragonal space group P4 2 /nmc (No. 137) in the LiBS 2 structure type, while CsInSb 2 crystallizes in lower symmetry in the orthorhombic space group Cmce (No. 64) in the KGaSb 2 structure type with additional disorder of one of the Cs sites. The crystal structures of all three reported AMSb 2 compounds are composed of two-dimensional [MSb 2 ] – tetrahedral layers separated by Rb + or Cs + cations. [MSb 2 ] – layers are built from fused M–Sb pentagons and hexagons, which are also the main structural units for A 8 M 27 Sb 19 clathrate cages. The semiconductor nature of AMSb 2 was suggested by band structure calculations and confirmed by transport property characterization. CsGaSb 2 is a rare example of an n-type pnictide Zintl phase. Finally, all reported compounds exhibit low thermal conductivity typical for complex antimonides of heavy elements.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Gut microbiome partially mediates and coordinates the effects of genetics on anxiety-like behavior in Collaborative Cross mice

Abstract Growing evidence suggests that the gut microbiome (GM) plays a critical role in health and disease. However, the contribution of GM to psychiatric disorders, especially anxiety, remains unclear. We used the Collaborative Cross (CC) mouse population-based model to identify anxiety associated host genetic and GM factors. Anxiety-like behavior of 445 mice across 30 CC strains was measured using the light/dark box assay and documented by video. A custom tracking system was developed to quantify seven anxiety-related phenotypes based on video. Mice were assigned to a low or high anxiety group by consensus clustering using seven anxiety-related phenotypes. Genome-wide association analysis (GWAS) identified 141 genes (264 SNPs) significantly enriched for anxiety and depression related functions. In the same CC cohort, we measured GM composition and identified five families that differ between high and low anxiety mice. Anxiety level was predicted with 79% accuracy and an AUC of 0.81. Mediation analyses revealed that the genetic contribution to anxiety was partially mediated by the GM. Our findings indicate that GM partially mediates and coordinates the effects of genetics on anxiety.

59 BASIC BIOLOGICAL SCIENCES↗

Tuning perovskite nanocrystal superlattices for superradiance in the presence of disorder

The cooperative emission of interacting nanocrystals is an exciting topic fueled by recent reports of superfluorescence and superradiance in assemblies of perovskite nanocubes. Several studies estimated that coherent coupling is localized to a small fraction of nanocrystals (10 -7 –10 -3 ) within the assembly, raising questions about the origins of localization and ways to overcome it. In this work, we examine single-excitation superradiance by calculating radiative decays and the distribution of superradiant wave function in two-dimensional CsPbBr 3 nanocube superlattices. The calculations reveal that the energy disorder caused by size distribution and large interparticle separations reduces radiative coupling and leads to the excitation localization, with the energy disorder being the dominant factor. The single-excitation model clearly predicts that, in the pursuit of cooperative effects, having identical nanocubes in the superlattice is more important than achieving a perfect spatial order. The monolayers of large CsPbBr 3 nanocubes (L NC = 10–20 nm) are proposed as model systems for experimental tests of superradiance under conditions of non-negligible size dispersion, while small nanocubes (L NC = 5–10 nm) are preferred for realizing the Dicke state under ideal conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The seventh blind test of crystal structure prediction: structure generation methods

A seventh blind test of crystal structure prediction was organized by the Cambridge Crystallographic Data Centre featuring seven target systems of varying complexity: a silicon and iodine-containing molecule, a copper coordination complex, a near-rigid molecule, a cocrystal, a polymorphic small agrochemical, a highly flexible polymorphic drug candidate, and a polymorphic morpholine salt. In this first of two parts focusing on structure generation methods, many crystal structure prediction (CSP) methods performed well for the small but flexible agrochemical compound, successfully reproducing the experimentally observed crystal structures, while few groups were successful for the systems of higher complexity. A powder X-ray diffraction (PXRD) assisted exercise demonstrated the use of CSP in successfully determining a crystal structure from a low-quality PXRD pattern. The use of CSP in the prediction of likely cocrystal stoichiometry was also explored, demonstrating multiple possible approaches. Crystallographic disorder emerged as an important theme throughout the test as both a challenge for analysis and a major achievement where two groups blindly predicted the existence of disorder for the first time. Additionally, large-scale comparisons of the sets of predicted crystal structures also showed that some methods yield sets that largely contain the same crystal structures.

Chemistry↗

Tuning Catalytic Reactivity via Wetting Control through Oxygen Vacancies: Ru Clusters on Anatase TiO 2 and CeO 2 Supports

The shape of supported metal particles regulates their catalytic reactivity and is determined by the degree of wetting between the metal particle and the support surface. Flattened particles that wet support surfaces were reported in various catalytic systems, particularly in the subnanometer size regime. Such consequential metal–support wetting phenomena are poorly understood, and methods to study them on powder catalysts under realistic conditions are lacking. Here, we investigate the size-dependent wetting behaviors of Ru particles on two reducible-oxide supports, anatase TiO 2 (TiO 2 -A) and CeO 2 , under reducing catalytic conditions. X-ray absorption spectroscopy (XAS), low-energy ion scattering (LEIS), and density functional theory (DFT) are combined to determine the shape of Ru particles. Ru particles remain three-dimensional without wetting the TiO 2 -A support within the coverage range studied (0.06–0.98 Ru nm –2 ). In contrast, at low coverages (<0.25 Ru nm –2 ), Ru wets the CeO 2 support to form flat, disordered structures. The higher wettability of CeO 2 than TiO 2 -A is attributed to oxygen vacancies in the near-surface region. The shape difference between small Ru particles or clusters on the two supports leads to drastically contrasting catalytic reactivities in polyolefin hydrogenolysis, despite similar diameters. As a result, this work highlights the implications of metal–support wetting, or cluster shape, on catalytic behaviors of small metal clusters, while establishing the foundation for future systematic studies of such a phenomenon in realistic systems, by delivering a multitechnique methodology and revealing governing fundamental principles.

42 ENGINEERING↗

Quantum system dynamics with a weakly nonlinear Josephson junction bath

Here, we investigate the influence of a weakly nonlinear Josephson bath consisting of a chain of Josephson junctions on the dynamics of a small quantum system (LC oscillator). Focusing on the regime where the charging energy is the largest energy scale, we perturbatively calculate the correlation function of the Josephson bath to the leading order in the Josephson energy divided by the charging energy while keeping the cosine potential exactly. When the variation of the charging energy along the chain ensures fast decay of the bath correlation function, the dynamics of the LC oscillator that is weakly and capacitively coupled to the Josephson bath can be solved through the Markovian master equation. We establish a duality relation for the Josephson bath between the regimes of large charging and Josephson energies, respectively. The results can be applied to cases where the charging energy either is nonuniformly engineered or disordered in the chain. Furthermore, we find that the Josephson bath may become non-Markovian when the temperature is increased beyond the zero-temperature limit in that the bath correlation function gets shifted by a constant and does not decay with time.

1-dimensional systems↗

Trisodium Phosphate Phases and Solubility in Alkaline Solutions Relevant to Radioactive Waste Processing

The U.S. Department of Energy’s Hanford Site faces significant challenges in managing millions of gallons of legacy radioactive waste, where phosphate precipitation can obstruct pipelines during retrieval and processing. To resolve long-standing inconsistencies in reported solubility and clarify factors governing trisodium phosphate hydrates, we examined the Na3PO4:NaOH:H2O system. Powder and single-crystal X-ray diffraction revealed that commercial precursors undergo transformations that produce multiple hydrates, including three previously unreported phases comprising an ordered polymorph of Na3(PO4)·12H2O·1/6NaOH, Na3PO4·5H2O, and Na3PO4·9H2O. Computational modeling indicated that the ordered dodecahydrate is more stable than its disordered counterpart, suggesting kinetic persistence of structural disorder. Solubility measurements were conducted with solutions prepared either from anhydrous Na3PO4 or from Na3(PO4)·12H2O·1/6NaOH and revealed that release of interstitial NaOH from the hydrate precursor elevated solution alkalinity, thereby significantly reducing phosphate solubility relative to solutions prepared with anhydrous Na3PO4 across 20–44 °C. These results begin to reconcile inconsistencies in prior solubility data and clarify how phase composition dictates phosphate precipitation under alkaline conditions.

Graham, Trenton R. (ORCID:0000000189078004)↗

Spin frustration and an exotic critical point in ferromagnets from nonuniform opposite g factors

Here, it is demonstrated that novel spin frustration can be induced in ferromagnets with nonuniform opposite Landé g-factors. The frustrated state is characterized by a mutual interplay of typical ferromagnetic (FM) and antiferromagnetic (AF) features, such as the zero-field susceptibility being FM-like at low temperatures but AF-like at high temperatures. It is also found to contain an exotic zero-temperature 'half fire, half ice' critical point at which the spins on one sublattice are fully disordered and on the other one are fully ordered. We suggest that such frustration may occur in a number of copper-iridium oxides such as Sr 3 CuIrO 6 . We also anticipate a realization of the frustration and 'partial fire, partial ice' states in certain antiferromagnets, lattice gas, and neuron systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Martensitic Transformation in Fe x Mn 80-x Co 10 Cr 10 High-Entropy Alloy

High-entropy alloys and even medium-entropy alloys are an intriguing class of materials in that structure and property relations can be controlled via alloying and chemical disorder over wide ranges in the composition space. Employing density-functional theory combined with the coherent-potential approximation to average over all chemical configurations, we tune free energies between face-centered-cubic and hexagonal-close-packed phases in Fe x Mn 80 - x Co 10 Cr 10 systems. Within Fe-Mn-based alloys, we show that the martensitic transformation and chemical short-range order directly correlate with the face-centered-cubic and hexagonal-close-packed energy difference and stacking-fault energies, which are in quantitative agreement with recent observation of two phase region (face-centered cubic and hexagonal closed pack) in a polycrystalline high-entropy alloy sample at x = 40 at.%. Our predictions are further confirmed by single-crystal measurements on a x = 40 at.% using transmission-electron microscopy, selective-area diffraction, and electron-backscattered-diffraction mapping. The results herein offer an understanding of transformation-induced or twinning-induced plasticity in this class of high-entropy alloys and a design guide for controlling the physics at the electronic level.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Evolution of magnetic surfboards and spin glass behavior in (Fe 1- p Ga p ) 2 TiO 5

The unusual anisotropy of the spin glass (SG) transition in the pseudobrookite system Fe 2 TiO 5 has been interpreted as arising from an induced, van der Waals-like, interaction among magnetic clusters. Here we present susceptibility ($\chi$) and specific heat data ($C$) for Fe 2 TiO 5 diluted with non-magnetic Ga, (Fe 1- p Ga p ) 2 TiO 5 , for disorder parameter $p$ = 0, 0.11, and 0.42, and elastic neutron scattering data for $p$ = 0.20. A uniform suppression of ${T_g}$ is observed upon increasing $p$, along with a value of $\chi \left( {{T_g}} \right)$ that increases as $T_g$ decreases, i.e. $d\chi ({T_g})/d{T_g} < 0$ We also observe $C\left( T \right) \propto {T^2}$ in the low temperature limit. In conclusion, the observed behavior places (Fe 1- p Ga p ) 2 TiO 5 in the category of a strongly geometrically frustrated SG.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Quantum-enhanced photoprotection in neuroprotein architectures emerges from collective light-matter interactions

Background Superradiance is the phenomenon of many identical quantum systems absorbing and/or emitting photons collectively at a higher rate than any one system can individually. This phenomenon has been studied analytically in idealized distributions of electronic two-level systems (TLSs), each with a ground and excited state, as well as numerically in realistic photosynthetic nanotubes and cytoskeletal architectures. Methods Superradiant effects are studied here in idealized toy model systems and realistic biological mega-networks of tryptophan (Trp) molecules, which are strongly fluorescent amino acids found in many proteins. Each Trp molecule acts as a chromophore absorbing in the ultraviolet spectrum and can be treated approximately as a TLS, with its 1 L a excited singlet state; thus, organized Trp networks can exhibit superradiance. Such networks are found, for example, in microtubules, actin filaments, and amyloid fibrils. Microtubules and actin filaments are spiral-cylindrical protein polymers that play significant biological roles as primary constituents of the eukaryotic cytoskeleton, while amyloid fibrils have been targeted in a variety of neurodegenerative diseases. We treat these proteinaceous Trp networks as open quantum systems, using a non-Hermitian Hamiltonian to describe interactions of the chromophore network with the electromagnetic field. We numerically diagonalize the Hamiltonian to obtain its complex eigenvalues, where the real part is the energy and the imaginary part is its associated enhancement rate. We also consider multiple realizations of increasing static disorder in either the site energies or the decay rates. Results We obtained the energies and enhancement rates for realistic microtubules, actin filament bundles, and amyloid fibrils of differing lengths, and we use these values to calculate the quantum yield, which is the ratio of the number of photons emitted to the number of photons absorbed. We find that all three of these structures exhibit highly superradiant states near the low-energy portion of the spectrum, which enhances the magnitude and robustness of the quantum yield to static disorder and thermal noise. Conclusion The high quantum yield and stable superradiant states in these biological architectures may play a photoprotective rolein vivo, downconverting energetic ultraviolet photons—absorbed from those emitted by reactive free radical species—to longer, safer wavelengths and thereby mitigating biochemical stress and photophysical damage. Contrary to conventional assumptions that quantum effects cannot survive in large biosystems at high temperatures, our results suggest that macropolymeric collectives of TLSs in microtubules, actin filaments, and amyloid fibrils exhibit increasingly observable and robust effects with increasing length, up to the micron scale, due to quantum coherent interactions in the single-photon limit. Superradiant enhancement and high quantum yield exhibited in neuroprotein polymers could thus play a crucial role in information processing in the brain, the development of neurodegenerative diseases such as Alzheimer’s and related dementias, and a wide array of other pathologies characterized by anomalous protein aggregates.

Physics↗

Interplay of superconducting, metallic, and crystalline states of composite fermions at 𝜈 = $\frac{1}{6}$ in wide quantum wells

Evidence for developing fractional quantum Hall effect (FQHE) at filling fraction 𝜈 = 1/6 and 1/8 was recently reported in wide GaAs quantum wells [Wang et al., Phys. Rev. Lett. 134, 046502 (2025)]. In this article, we theoretically investigate the nature of the state at 𝜈 = 1/6 as a function of the quantum well width and the density by considering composite-fermion (CF) crystals, CF Fermi sea, and various kinds of paired CF states. The 𝑓-wave paired state has the lowest energy among the paired CF states. However, for parameters of interest, the energies of the CF crystal, the CF Fermi liquid, and the 𝑓-wave paired CF state are too close to distinguish. We, therefore, predict that 𝑖𝑓 the FQHE at 𝜈 = 1/6 is experimentally confirmed, this state would be an 𝑓-wave paired state of CFs, which can be verified by measurement of its thermal Hall conductance. Exact diagonalization studies on clean systems with up to eight electrons show that the ground states at 𝜈 = 𝑛/(6⁢𝑛 ± 1) are incompressible for all widths and densities we have considered, and are well described by the corresponding Laughlin and Jain states. We propose a phase diagram for large quantum well widths and densities in which at zero disorder, incompressible FQHE states are stabilized at 𝜈 = 𝑛/(6⁢𝑛 ± 1) and 𝜈 = 1/6, but in between these fillings the CF crystal is stabilized. We also present a qualitative discussion on the effects of disorder and propose a schematic phase diagram based on it. With disorder, which creates a spatial variation in the filling factor, two regimes are identified: (i) for small disorder, when the incompressible states percolate at the special fillings, FQHE with quantized Hall plateaus and vanishing longitudinal resistance should occur; and (ii) for larger disorder, when the CF crystal percolates, the longitudinal resistance rises with decreasing temperature but the domains of FQHE liquid produce minima at the special filling factors. Here, experiments are consistent with the latter scenario. We also mention a possible connection of the phase diagram presented here to a puzzling behavior observed for the fractional quantum anomalous Hall effect in pentalayer graphene.

Composite fermions↗

A Theoretical Analysis on the Dynamic Behavior and Electromechanical Response of PZT

Piezoelectric materials are used as a power source in stockpile components for safety and reliability assurances. The objective of this project is to gain insights into the fundamental pressure-induced behavior and electromechanical response of lead zirconate titanate (PZT). Specifically, to establish the basis for an accurate, physics-based material model for robust model-based design to rapidly optimize PZT-based materials and components for performance studies. Established ab-initio methods are used to interrogate and understand the dynamic behavior of PZT as a function of composition (50/50, 65/35, 80/20, 95/5) and dopants (La, Nb) to overcome the costly and time-consuming experimental methodologies. New cold curves for pure and doped single-crystal PZT are obtained as the reference equation-of-state (EOS). A negligible change in the pressure responses was observed for the systems and strains studied. Dielectric and piezoelectric responses of pure and doped single-crystal PZT were also calculated as a function of pressure. For undoped PZT, there is a clear and orderly pressure and composition dependence. For doped PZT, there is a significant increase in the responses, but the behavior is very disordered and inconclusive.

36 MATERIALS SCIENCE↗

Effects of Ligand Chemistry on Ion Transport in 2D Hybrid Organic–Inorganic Perovskites

2D hybrid organic–inorganic perovskites are potentially promising materials as passivation layers that can enhance the efficiency and stability of perovskite photovoltaics. The ability to suppress ion transport is proposed as a stabilization mechanism, yet an effective characterization of relevant modes of halide diffusion in 2D perovskites is nascent. In light of this knowledge gap, molecular dynamics simulations with enhanced sampling and experimental validation to systematically characterize how ligand chemistry in seven (R-NH 3 ) 2 PbI 4 systems impacts halide diffusion, particularly in the out-of-plane direction is combined. It is found that increasing stiffness and length of ligands generally inhibits ion transport, while increasing ligand polarization generally enhances it. Structural and energetic analyses of the migration pathways provide quantitative explanations for these trends, which reflect aspects of the disorder of the organic layer. Overall, this mechanistic analysis greatly enhances the current understanding of halide migration in 2D hybrid organic–inorganic perovskites and yields insights that can inform the design of future passivation materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Accelerated annealing of colloidal crystal monolayers by means of cyclically applied electric fields

Abstract External fields are commonly applied to accelerate colloidal crystallization; however, accelerated self-assembly kinetics can negatively impact the quality of crystal structures. We show that cyclically applied electric fields can produce high quality colloidal crystals by annealing local disorder. We find that the optimal off-duration for maximum annealing is approximately one-half of the characteristic melting half lifetime of the crystalline phase. Local six-fold bond orientational order grows more rapidly than global scattering peaks, indicating that local restructuring leads global annealing. Molecular dynamics simulations of cyclically activated systems show that the ratio of optimal off-duration for maximum annealing and crystal melting time is insensitive to particle interaction details. This research provides a quantitative relationship describing how the cyclic application of fields produces high quality colloidal crystals by cycling at the fundamental time scale for local defect rearrangements; such understanding of dynamics and kinetics can be applied for reconfigurable colloidal assembly.

36 MATERIALS SCIENCE↗