Long-range Fluctuations Research Articles

Stronger quantum fluctuation with larger spins: Emergent magnetism in the pressurized high-temperature superconductor FeSe

A counter-intuitive enhancement of quantum fluctuation with larger spins, together with a few novel physical phenomena, is discovered in studying the recently observed emergent magnetism in high-temperature superconductor FeSe under pressure. Starting with experimental crystalline structure from our high-pressure X-ray refinement, we analyze theoretically the stability of the magnetically ordered state with a realistic spin-fermion model. We find surprisingly that in comparison with the magnetically ordered Fe-pnictides, the larger spins in FeSe suffer even stronger long-range quantum fluctuation that diminishes their ordering at ambient pressure. This "fail-to-order" quantum spin liquid state then develops into an ordered state above 1GPa due to weakened fluctuation accompanying the reduction of anion height and carrier density. The ordering further benefits from the ferro-orbital order and shows the observed enhancement around 1GPa. We further clarify the controversial nature of magnetism and its interplay with nematicity in FeSe in the same unified picture for all Fe-based superconductors. In addition, the versatile itinerant carriers produce interesting correlated metal behavior in a large region of phase space. Our study establishes a generic exceptional paradigm of stronger quantum fluctuation with larger spins that complements the standard knowledge of insulating magnetism.

Strongly correlated superconductivity with long-range spatial fluctuations

We review recent studies for superconductivity using diagrammatic extensions of dynamical mean field theory. These approaches take into account simultaneously both, the local correlation effect and spatial long-range fluctuations, which are essential to describe unconventional superconductivity in a quasi-two-dimensional plane. The results reproduce and predict the experimental phase diagrams of strongly correlated system such as cuprates and nickelates. Further studies reveal that the dynamical screening effect of the pairing interaction vertex has dramatic consequences for the transition temperature and may even support exotic mechanisms like odd-frequency pairing. We also discuss the dimensionality of layered materials and how to interpret the numerical results in two dimensions.

Beyond the Average: Spatial and Temporal Fluctuations in Oxide Glass-Forming Systems.

Atomic structure dictates the performance of all materials systems; the characteristic of disordered materials is the significance of spatial and temporal fluctuations on composition-structure-property-performance relationships. Glass has a disordered atomic arrangement, which induces localized distributions in physical properties that are conventionally defined by average values. Quantifying these statistical distributions (including variances, fluctuations, and heterogeneities) is necessary to describe the complexity of glass-forming systems. Only recently have rigorous theories been developed to predict heterogeneities to manipulate and optimize glass properties. This article provides a comprehensive review of experimental, computational, and theoretical approaches to characterize and demonstrate the effects of short-, medium-, and long-range statistical fluctuations on physical properties (e.g., thermodynamic, kinetic, mechanical, and optical) and processes (e.g., relaxation, crystallization, and phase separation), focusing primarily on commercially relevant oxide glasses. Rigorous investigations of fluctuations enable researchers to improve the fundamental understanding of the chemistry and physics governing glass-forming systems and optimize structure-property-performance relationships for next-generation technological applications of glass, including damage-resistant electronic displays, safer pharmaceutical vials to store and transport vaccines, and lower-attenuation fiber optics. We invite the reader to join us in exploring what can be discovered by going beyond the average.

Short-Range Backbone Dihedral Rotations Modulate Internal Friction in Intrinsically Disordered Proteins.

Protein folding and dynamics are governed by an intricate interplay of thermal and viscosity-mediated effects. The solvent viscosity contributes to the frictional drag in protein dynamics. In addition to this viscosity-dependent effect, there is also an intriguing viscosity-independent component that represents the intrinsic resistance of the polypeptide chain to changing its conformation. This solvent-independent component is termed internal friction. A longstanding question is what is the fundamental molecular origin of internal friction in highly solvated and rapidly fluctuating intrinsically disordered proteins (IDPs) devoid of any persistent intrachain interactions? Here, we present a unique case to directly demonstrate that sequence-specific backbone dihedral barriers control local internal friction in an archetypal IDP, namely, α-synuclein. We performed site-directed fluorescence depolarization kinetics using picosecond time-resolved fluorescence anisotropy measurements to directly observe the directional decorrelation arising due to short-range backbone torsional fluctuations in the dihedral space. A linear viscosity-dependent model of the dihedral relaxation time yielded a finite zero-viscosity intercept that corresponds to internal friction. Our site-specific dynamic readouts were able to detect localized sequence-specific frictional components that are otherwise skewed in viscosity-dependent long-range chain fluctuations. Our results revealed the presence of low internal friction in nonproline sequence segments. In contrast, a proline introduces torsional stiffness in the segment exhibiting high internal friction that can be compensated by a conformationally flexible glycine. Such an intriguing interplay of local dihedral dynamics can modulate sequence-dependent internal friction in a wide range of IDPs involved in a myriad of important events including folding, binding, assembly, and phase transitions.

Finite-size scaling and thermodynamics of model supercooled liquids: long-range concentration fluctuations and the role of attractive interactions.

We compute partial structure factors, Kirkwood-Buff integrals (KBIs) and chemical potentials of model supercooled liquids with and without attractive interactions. We aim at investigating whether relatively small differences in the tail of the radial distribution functions result in contrasting thermodynamic properties. Our results suggest that the attractive potential favours the nucleation of long-range structures. Indeed, upon decreasing temperature, Bathia-Thornton structure factors display anomalous behaviour in the k→0 limit. KBIs extrapolated to the thermodynamic limit confirm this picture, and excess coordination numbers identify the anomaly with long-range concentration fluctuations. By contrast, the purely repulsive system remains perfectly miscible for the same temperature interval and only reveals qualitatively similar concentration fluctuations in the crystalline state. Furthermore, differences in both isothermal compressibilities and chemical potentials show that thermodynamics is not entirely governed by the short-range repulsive part of the interaction potential, emphasising the nonperturbative role of attractive interactions. Finally, at higher density, where both systems display nearly identical dynamical properties and repulsive interactions become dominant, the anomaly disappears, and both systems also exhibit similar thermodynamic properties.

Volume viscosity and ultrasonic relaxation of ethanol-water mixtures studied by molecular dynamics simulations.

The volume viscosity of ethanol-water mixtures at various compositions was calculated by means of equilibrium molecular dynamics simulations, and the results were compared with acoustic experiments. The volume viscosity exhibited a strong maximum around the ethanol mole fraction of 0.27, which is in agreement with experiments. The relaxation in the 100 ps regime, which had been revealed by ultrasonic spectroscopy, was also reproduced. Analysis of the two-body density and the adiabatic pressure fluctuation demonstrated that the large volume viscosity of the mixture originates from the long-range concentration fluctuation.

Salt effects on knot dynamics in polyelectrolyte solutions

ABSTRACT We study the dynamics of linear polyelectrolyte (PE) knot in solution with doping salt by molecular dynamics simulations. The molecular mechanisms of PE knot dynamics are explained. The knot dynamics are the coupling results by the moving effect of chain entanglement and by the breathing effect of knot fluctuations. The moving effect is important as the whole chain is in the random coil state and becomes weak as shrinking to the close-to-globule (CTG) state. Interestingly, as the chain in the CTG state, the knot swells with occupying more segments. The breathing effect dominates the knot dynamics in the CTG state. This nontrivial behaviour (in comparison to neutral polymer knot) is prominent for the cases of doping salt with high concentration or of doping high-valent salt, which attributes to the enhanced electrostatic interactions and long-range fluctuation effects.

Multipoint correlation functions at phase separation. Exact results from field theory

We consider near-critical two-dimensional statistical systems with boundary conditions inducing phase separation on the strip. By exploiting low-energy properties of two-dimensional field theories, we compute arbitrary n-point correlation of the order parameter field. Finite-size corrections and mixed correlations involving the stress tensor trace are also discussed. As an explicit illustration of the technique, we provide a closed-form expression for a three-point correlation function and illustrate the explicit form of the long-ranged interfacial fluctuations as well as their confinement within the interfacial region.

Long-Range Photon Fluctuations Enhance Photon-Mediated Electron Pairing and Superconductivity.

Recently, the possibility of inducing superconductivity for electrons in two-dimensional materials has been proposed via cavity-mediated pairing. The cavity-mediated electron-electron interactions are long range, which has two main effects: firstly, within the standard BCS-type pairing mediated by adiabatic photons, the superconducting critical temperature depends polynomially on the coupling strength, instead of the exponential dependence characterizing the phonon-mediated pairing; secondly, as we show here, the effect of photon fluctuations is significantly enhanced. These mediate novel non-BCS-type pairing processes, via nonadiabatic photons, which are not sensitive to the electron occupation but rather to the electron dispersion and lifetime at the Fermi surface. Therefore, while the leading temperature dependence of BCS pairing comes from the smoothening of the Fermi-Dirac distribution, the temperature dependence of the fluctuation-induced pairing comes from the electron lifetime. For realistic parameters, also including cavity loss, this results in a critical temperature which can be more than 1 order of magnitude larger than the BCS prediction. Moreover, a finite average number of photons (as can be achieved by incoherently pumping the cavity) adds to the fluctuations and leads to a further enhancement of the critical temperature.

Wave transport in 1D stealthy hyperuniform phononic materials made of non-resonant and resonant scatterers

Stealthy hyperuniform point patterns are characterized by a vanishing spatial Fourier transform around the origin of the reciprocal vector space. The long-range point density fluctuations are suppressed as well in materials consisting of such distribution of scatterers, opening up opportunities to control waves. Beside wave transport in such structured materials are driven by several elements, such as the acoustic properties of the host material, the scatterer characteristics, i.e., dimensions or resonant features, and the scatterer distribution patterns. The effects of these three basic elements on the wave transport properties are usually hard to discriminate. In this work, we analyze the transport properties of acoustic waves in one-dimensional phononic materials constituted of either non-resonant or resonant scatterers distributed along stealthy hyperuniform patterns in air. The pattern is controlled by the stealthiness, allowing us to continuously vary from random phononic materials to phononic crystals. The properties of the scatterers are controlled by their size and/or the resonant frequencies. The properties of the host material are controlled by the viscothermal losses. Transport properties of stealthy hyperuniform materials are found to be robust to both the scatterer dimensions and inherent viscothermal losses, while strongly affected by the scatterer resonances, which introduce sharp dips in the transmission coefficient.

Modeling the interstitial fluid effect in turbulent disperse slurry flow in a vertical pipe

A numerical study was conducted to assess the performance of a Two-Fluid Model (TFM) developed for gas-solid flow in predicting liquid-solid flow, as well as a TFM specifically modified for liquid-solid flow, which considers the effect of the interstitial fluid. Both cases use the Kinetic Theory of Granular Flow (KTGF) for prediction of the solid phase flow features. Some of the physics involved in gas-solid and liquid-solid flows is intuitively different, and some model terms that can be neglected in a gas-solid formulation turn out to be important for liquid-solid flow. For instance, the much larger density and viscosity of the liquid compared to a gas suggest that the solid particle fluctuations and collisions are reduced. Three intermediate model formulations were developed to assess the relevance of the interstitial terms. The intermediate model formulations, together with the two base case models, were assessed based on their predictions for the case of fully developed, turbulent, steady flow of a liquid solid mixture in a vertical pipe. The main differences in the model formulations pertain to the transport equations for the streamwise liquid momentum, granular temperature and turbulence kinetic energy. The predictions considered such flow features as: the velocity profiles of both the liquid and solid phases, the solids volume fraction profile and budgets of the transport equations for the granular temperature and turbulence kinetic energy. The results obtained were used to identify the most significant model terms. These include modified formulations for the solids viscosity and granular temperature conductive coefficient to include the effects of the interstitial fluid. The single most important term was the model for the long-range particle fluctuations through the fluid, which played a dominant role in the balance of the turbulence kinetic energy and granular temperature transport equations. The present analysis demonstrates that this term should be reconfigured as a sink term in the granular temperature equation and a source term in the turbulence kinetic energy equation. With this modification, the numerical predictions were much closer to the experimental data, especially in terms of the solids volume fraction profile.

Disorder effects in topological insulator nanowires

Three-dimensional topological insulator (TI) nanowires with quantized surface subband spectra are studied as a main component of Majorana bound states (MBS) devices. However, such wires are known to have large concentration $N\ensuremath{\sim}{10}^{19}\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{\ensuremath{-}3}$ of Coulomb impurities. It is believed that a MBS device can function only if the amplitude of long-range fluctuations of the random Coulomb potential $\mathrm{\ensuremath{\Gamma}}$ is smaller than the subband gap $\mathrm{\ensuremath{\Delta}}$. Here we calculate $\mathrm{\ensuremath{\Gamma}}$ for recently experimentally studied large-dielectric-constant ${({\mathrm{Bi}}_{1\ensuremath{-}x}{\mathrm{Sb}}_{x})}_{2}{\mathrm{Te}}_{3}$ wires in a small-dielectric-constant environment (no superconductor). We show that provided by such a dielectric-constant contrast, the confinement of electric field of impurities within the wire allows more distant impurities to contribute into $\mathrm{\ensuremath{\Gamma}}$, leading to $\mathrm{\ensuremath{\Gamma}}\ensuremath{\sim}3\mathrm{\ensuremath{\Delta}}$. We also calculate a TI wire resistance as a function of the Fermi level and carrier concentration due to scattering on Coulomb and neutral impurities and do not find observable discrete subband-spectrum-related oscillations at $N\ensuremath{\gtrsim}{10}^{18}\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{\ensuremath{-}3}$.

Manifestations of metastable criticality in the long-range structure of model water glasses

Much attention has been devoted to water’s metastable phase behavior, including polyamorphism (multiple amorphous solid phases), and the hypothesized liquid-liquid transition and associated critical point. However, the possible relationship between these phenomena remains incompletely understood. Using molecular dynamics simulations of the realistic TIP4P/2005 model, we found a striking signature of the liquid-liquid critical point in the structure of water glasses, manifested as a pronounced increase in long-range density fluctuations at pressures proximate to the critical pressure. By contrast, these signatures were absent in glasses of two model systems that lack a critical point. We also characterized the departure from equilibrium upon vitrification via the non-equilibrium index; water-like systems exhibited a strong pressure dependence in this metric, whereas simple liquids did not. These results reflect a surprising relationship between the metastable equilibrium phenomenon of liquid-liquid criticality and the non-equilibrium structure of glassy water, with implications for our understanding of water phase behavior and glass physics. Our calculations suggest a possible experimental route to probing the existence of the liquid-liquid transition in water and other fluids.

Equilibrium Mean-Field-Like Statistical Models with KPZ Scaling

We have considered three different “one-body” statistical systems involving Brownian excursions, which possess for fluctuations Kardar–Parisi–Zhang scaling with the critical exponent $$\nu = \tfrac{1}{3}$$ . In all models imposed external constraints push the underlying stochastic process to a large deviation regime. Specifically, we have considered fluctuations for: (i) Brownian excursions on non-uniform finite trees with linearly growing branching originating from the mean-field approximation of the Dumitriu–Edelman representation of matrix models, (ii) (1+1)D “magnetic” Dyck paths within the strip of finite width, (iii) inflated ideal polymer ring with fixed gyration radius. In the latter problem cutting off the long-ranged spatial fluctuations and leaving only the “typical” modes for stretched paths, we ensure the KPZ-like scaling for bond fluctuations. To the contrary, summing up all normal modes, we get the Gaussian behavior. In all considered models, KPZ fluctuations emerge in presence of two complementary conditions: (i) the trajectories are pushed to a large deviation region of a phase space, and (ii) the trajectories are leaning on an impenetrable boundary.

The neurocognitive correlates of brain entropy estimated by resting state fMRI

Resting state brain activity consumes most of brain energy, likely creating and maintaining a reserve of general brain functionality. The latent reserve if it exists may be reflected by the profound long-range fluctuations of resting brain activity. The long-range temporal coherence (LRTC) can be characterized by resting state fMRI (rsfMRI)-based brain entropy (BEN) mapping. While BEN mapping results have shown sensitivity to neuromodulations or disease conditions, the underlying neuromechanisms especially the associations of BEN or LRTC to neurocognition still remain unclear. To address this standing question and to test a novel hypothesis that resting BEN reflects a latent functional reserve through the link to general functionality, we mapped resting BEN of 862 young adults and comprehensively examined its associations to neurocognitions using data from the Human Connectome Project (HCP). Our results unanimously highlighted two brain circuits: the default mode network (DMN) and executive control network (ECN) through their negative associations of BEN to general functionality, which is independent of age and sex. While BEN in DMN/ECN increases with age, it decreases with education years. These results demonstrated the neurocognitive correlates of resting BEN in DMN/ECN and suggest resting BEN in DMN/ECN as a potential proxy of the latent functional reserve that facilitates general brain functionality and may be enhanced by education.

NEUTRON NOISE PATTERNS FROM COUPLED FUEL-ASSEMBLY VIBRATIONS

The neutron flux fluctuation magnitude of KWU-built PWRs shows a hitherto unexplained correlation with the types of loaded fuel assemblies. Also, certain measured long-range neutron flux fluctuation patterns in neighboring core quadrants still lack a closed understanding of their origin. The explanation of these phenomena has recently revived a new interest in neutron noise research. The contribution at hand investigates the idea that a synchronized coolant-driven vibration of major parts of the fuel-assembly ensemble leads to these phenomena. Starting with an assumed mode of such collective vibration, the resulting effects on the time-dependent neutron-flux distribution are analyzed via a DYN3D simulation. A three-dimensional representation of the time-dependent bow of all fuel assemblies is taken into account as a nodal DYN3D feedback parameter by time-dependent variations of the fuel-assembly pitch. The impact of its variation on the cross sections is quantified using a cross-section library that is generated from the output of corresponding CASMO5 calculations. The DYN3D simulation qualitatively reproduces the measured neutron-flux fluctuation patterns. The magnitude of the fluctuations and its radial dependence are comparable to the measured details. The results imply that collective fuel-assembly vibrations are a promising candidate for being the key to understand long-known fluctuation patterns in KWU built PWRs. Further research should elaborate on possible excitation mechanisms of the assumed vibration modes.

Spatially correlated incommensurate lattice modulations in an atomically thin high-temperature Bi2.1Sr1.9CaCu2.0O8+y superconductor

Strong variations in superconducting critical temperatures in different families of the cuprate perovskites, even with similar hole doping in their copper-oxygen planes, suggest the importance of lattice modulation effects. The one-dimensional incommensurate lattice modulation (ILM) of Bi_2Sr_2CaCu_2O_{8+y}, with the average atomic positions perturbed beyond the unit cell, offers an ideal test ground for studying the interplay between superconductivity and the long-range incommensurate lattice fluctuations. Here we report Scanning nano X-ray Diffraction (SnXRD) imaging of incommensurate lattice modulations in Bi_{2.1}Sr_{1.9}CaCu_{2.0}O_{8+{\delta}} Van der Waals heterostructures of thicknesses down to two-unit cells. Using SnXRD, we probe that the long-range and short-range incommensurate lattice modulations in bulk sample surface with spatial resolution below 100 nm. We find that puddle-like domains of ILM of size uniformly evolving with dimensionality. In the 2-unit cell thin sample, it is observed that the wavevectors of the long- and short-range orders become anti-correlated with emerging spatial patterns having a directional gradient. The emerging patterns, originated by tiny tuning of lattice strain, induce static mesoscopic charge density waves. Our findings thus demonstrate that the strain can be used to tune and control the electromagnetic properties of two-dimensional high-temperature superconductors.

The vacua of dipolar cavity quantum electrodynamics

The structure of solids and their phases is mainly determined by static Coulomb forces while the coupling of charges to the dynamical, i.e., quantized degrees of freedom of the electromagnetic field plays only a secondary role. Recently, it has been speculated that this general rule can be overcome in the context of cavity quantum electrodynamics (QED), where the coupling of dipoles to a single field mode can be dramatically enhanced. Here we present a first exact analysis of the ground states of a dipolar cavity QED system in the non-perturbative coupling regime, where electrostatic and dynamical interactions play an equally important role. Specifically, we show how strong and long-range vacuum fluctuations modify the states of dipolar matter and induce novel phases with unusual properties. Beyond a purely fundamental interest, these general mechanisms can be important for potential applications, ranging from cavity-assisted chemistry to quantum technologies based on ultrastrongly coupled circuit QED systems.

Comprehensive in silico mutational-sensitivity analysis of PTEN establishes signature regions implicated in pathogenesis of Autism Spectrum Disorders

An extensively studied cancer and Autism Spectrum Disorders (ASD) gene like PTEN provided an exclusive opportunity to map its mutational-landscape, compare and establish plausible genotypic predictors of ASD-associated phenotypic outcomes. Our exhaustive in silico analysis on 4252 SNPs using >30 tools identified increased mutational-density in exon7. Phosphatase domain, although evolutionarily conserved, had the most nsSNPs localised within signature regions. The evolutionarily variable C-terminal side contained the highest truncating-SNPs outside signature regions of C2 domain and most PTMs within C-tail site which displayed maximum intolerance to polymorphisms, and permitted benign but destabilising nsSNPs that enhanced its intrinsically-disordered nature. ASD-associated SNPs localised within ATP-binding motifs and Nuclear-Localising-Sequences were the most potent triggers of ASD manifestation. These, along with variations within P, WPD and TI loops, M1 within phosphatase domain, M2 and MoRFs of C2 domain, caused severe long-range conformational fluctuations altering PTEN's dynamic stability- not observed in variations outside signature regions. 3’UTR-SNPs affected 44 strong miRNA brain-specific targets; several 5’ UTR-SNPs targeted transcription-factor POLR2A and 10 pathogenic Splice-Affecting-Variants were identified.

Do Deep Eutectic Solvents Form Uniform Mixtures Beyond Molecular Microheterogeneities?

We have performed small-angle neutron scattering in a momentum transfer range (0.05 < Q < 0.5 Å-1) to study long-range order and concentration fluctuations in deep eutectic solvents (DESs) and their aqueous solutions. Ethaline (choline chloride/ethylene glycol), glycerol/lactic acid, and menthol/decanoic acid mixtures were selected to illustrate individually the case of ionic, nonionic, and hydrophobic mixtures. Carefully designed isotopic labeling was used to emphasize selectively the spatial correlations between the different solvent components. For ethaline DESs and their aqueous solutions, a weak low-Q peak observed only for certain compositions and some partial structure factors revealed the mesoscopic segregation of ethylene glycol molecules that do not participate in the solvation of ionic units, either because they are in excess with respect to the eutectic stoichiometry (1:4 neat ethaline) or substituted by water (4w-ethaline and higher aqueous dilutions). For the nonionic hydrophilic solutions, such a mesoscopic segregation was not observed. This indicates that the better balanced interactions between the three nonionic H-bonded components (water, lactic acid, and glycerol) favor homogeneous mixing. For the hydrophobic DESs, we observed an excess of coherent scattering intensity centered at Q = 0, which could be reproduced by a model of noninteracting spherical domains. Local concentration fluctuations are not excluded either. However, unlike liquid mixtures with a tendency to demix, we have found no evidence of expansion of domains with different compositions to a large scale.