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Abstract Biomaterials such as spider silk and mussel byssi are fabricated by the dynamic manipulation of intra‐ and intermolecular biopolymer interactions. Organisms modulate solution parameters, such as pH and ion co‐solute concentration, to effect these processes. These biofabrication schemes provide a conceptual framework to develop new dynamic and responsive abiotic soft material systems. Towards these ends, the chemical diversity of readily available ionic compounds offers a broad palette to manipulate the physicochemical properties of polyelectrolytes via ion‐specific interactions. In this study, we show for the first time that the ion‐specific interactions of biomimetic polyelectrolytes engenders a variety of phase separation behaviors, creating dynamic thermal‐ and ion‐responsive soft matter that exhibits a spectrum of physical properties, spanning viscous fluids to viscoelastic and viscoplastic solids. These ion‐dependent characteristics are further rendered general by the merger of lysine and phenylalanine into a single, amphiphilic vinyl monomer. The unprecedented breadth, precision, and dynamicity in the reported ion‐dependent phase behaviors thus introduce a broad array of opportunities for the future development of responsive soft matter; properties that are poised to drive developments in critical areas such as chemical sensing, soft robotics, and additive manufacturing.
We present a systematic investigation of particle-number fluctuations in the crossover region near the critical end point of a first-order phase transition using molecular dynamics simulations of the classical Lennard-Jones fluid. We extend our prior studies to third- and fourth-order cumulants in both coordinate- and momentum-space acceptances and integrated correlation functions (factorial cumulants). We find that, even near the critical point, non-Gaussian cumulants equilibrate on timescales comparable to those of the second-order cumulants, but show stronger finite-size effects. The presence of interactions and of the critical point leads to strong deviations of the cumulants from the ideal-gas baseline in coordinate space; these deviations are expected to persist in momentum space in the presence of collective expansion. In particular, the kurtosis becomes strongly negative, κσ 2 ≪ − 1 , on the crossover side of the critical point. However, this signal is significantly diluted once an efficiency cut used to distinguish protons from baryons is applied, leading to |κσ 2 | ≲ 1 even in the presence of the critical point. We discuss our results in the context of ongoing measurements of proton-number cumulants in heavy-ion collisions in RHIC-BES-II.
Eutectic solidification exemplifies nonequilibrium pattern formation, making it a well-studied moving boundary problem. Yet the mechanisms behind the formation of complex-regular microstructures – particularly in highly anisotropic systems with a significant volume fraction of a faceted phase – remain poorly understood. Our understanding of such systems is made complicated by the nonlinear interface kinetics and unique growth dynamics characteristic of faceted phases. To address these challenges, we investigate a model Al–Ge eutectic system, where the faceted Ge phase constitutes a substantial volume fraction (~0.35) and where the two solid phases arrange into so-called “fishbone” or “feather” complex-regular patterns. Using synchrotron-based x-ray nano-imaging and nanotomography with high spatial resolution (22 nm per pixel), we capture in real-time the evolution of the solid–liquid interfaces and the resulting three-dimensional microstructures in this faceted/non-faceted eutectic system. By integrating these observations with electron backscattered diffraction, we elucidate the crystallographic biases on the solidification process and the mechanisms driving the formation of such complex-regular microstructures. These findings inform a new growth model for irregular eutectics in (near-)symmetrical phase diagrams, offering insight on advanced microstructural design and processing strategies. More broadly, we demonstrate how interfacial curvature is generated in irregular eutectic alloys and how it depends on the volume fraction of the faceted phase.
Quantum phase estimation plays a central role in quantum simulation as it enables the study of spectral properties of many-body quantum systems. Most variants of the phase estimation algorithm require the application of the global unitary evolution conditioned on the state of one or more auxiliary qubits, posing a significant challenge for current quantum devices. In this work, we present an approach to quantum phase estimation that uses only locally controlled operations, resulting in a significantly reduced circuit depth. At the heart of our approach are efficient routines to measure the complex phase of the expectation value of the time-evolution operator, the so-called Loschmidt echo, for both circuit dynamics and Hamiltonian dynamics. By tracking changes in the phase during the dynamics, the routines trade circuit depth for increased sampling cost and classical postprocessing. Our approach does not rely on reference states and is applicable to any efficiently preparable state, regardless of its correlations. We provide a comprehensive analysis of the sample complexity and illustrate the results with numerical simulations. Our methods offer a practical pathway for measuring spectral properties in large many-body quantum systems using current quantum devices.
Streaked photoelectron emission spectra access the correlated dynamics of photoelectrons and residual target electrons with attosecond temporal resolution. Here, we calculated ab initio single-ionization spectra for photoemission from helium atoms by colinearly polarized ultrashort XUV and assisting few-femtosecond IR pulses. Distinguishing direct and shake-up ionization resulting in ground-state and excited (𝑛 = 2, 3) He + residual ions, respectively, we examined the effects of the correlated photoemission dynamics on the photoelectron phase accumulation as a function of the observable photoelectron detection direction and kinetic energy and XUV–IR pulse delay. We tracked the dynamical evolution of the residual ion in relative streaked photo- emission delays and found dominant contributions for shake-up emission from the residual-ion–photoelectron interaction. These are in very good and fair agreement, respectively, for 𝑛 = 2 and 𝑛 = 3 shake-up photoemission along the pulse-polarization directions, with previous experimental and theoretical investigations [Ossiander et al ., Nat. Phys. 13, 280 (2017)] and reveal a strong photoemission-direction dependence for shake-up ionization due to the coupling between the photoelectron and evolving residual-ion charge distribution in the IR-laser field.
Interactions between shock waves and gas bubbles in a liquid can lead to bubble collapse and high-speed liquid jet formation, relevant to biomedical applications such as shock wave lithotripsy and targeted drug delivery. This study reveals a complex interplay between acceleration-induced instabilities that drive jet formation and radial accelerations causing overall bubble collapse under shock wave pressure. Using high-speed synchrotron X-ray phase contrast imaging, the dynamics of micrometre-sized air bubbles interacting with laser-induced underwater shock waves are visualised. These images offer full optical access to phase discontinuities along the X-ray path, including jet formation, its propagation inside the bubble, and penetration through the distal side. Jet formation from laser-induced shock waves is suggested to be an acceleration-driven process. A model predicting jet speed based on the perturbation growth rate of a single-mode Richtmyer–Meshkov instability shows good agreement with experimental data, despite uncertainties in the jet-driving mechanisms. The jet initially follows a linear growth phase, transitioning into a nonlinear regime as it evolves. To capture this transition, a heuristic model bridging the linear and nonlinear growth phases is introduced, also approximating jet shape as a single-mode instability, again matching experimental observations. Upon piercing the distal bubble surface, jets can entrain gas and form a toroidal secondary bubble. Linear scaling laws are identified for the pinch-off time and volume of the ejected bubble relative to the jet’s Weber number, characterising the balance of inertia and surface tension. At low speeds, jets destabilise due to capillary effects, resulting in ligament pinch-off.
The formation and preservation of the active phase of the catalysts at the triple-phase interface during CO 2 capture and reduction is essential for improving the conversion efficiency of CO 2 electroreduction toward value-added chemicals and fuels under operational conditions. Designing such ideal catalysts that can mitigate parasitic hydrogen generation and prevent active phase degradation during the CO 2 reduction reaction (CO 2 RR), however, remains a significant challenge. Herein, we developed an interfacial engineering strategy to build a new SnO x catalyst by invoking multiscale approaches. This catalyst features a hierarchically nanoporous structure coated with an organic F-monolayer that modifies the triple-phase interface in aqueous electrolytes, substantially reducing competing hydrogen generation (less than 5%) and enhancing CO 2 RR selectivity (~90%). This rationally designed triple-phase interface overcomes the issue of limited CO 2 solubility in aqueous electrolytes via proactive CO 2 capture and reduction. Concurrently, we utilized pulsed square-wave potentials to dynamically recover the active phase for the CO 2 RR to regulate the production of C1 products such as formate and carbon monoxide (CO). This protocol ensures profoundly enhanced CO 2 RR selectivity (~90%) compared with constant potential (~70%) applied at -0.8 V (V vs RHE). We further achieved a mechanistic understanding of the CO 2 capture and reduction processes under pulsed square-wave potentials via in situ Raman spectroscopy, thereby observing the potential-dependent intensity of Raman vibrational modes of the active phase and CO 2 RR intermediates. Finally, this work will inspire material design strategies by leveraging triple-phase interface engineering for emerging electrochemical processes, as technology moves toward electrification and decarbonization.
We report a molecular dynamics study of ab initio quality of the ferroelectric phase transition in crystalline PbTiO3. We model anharmonicity accurately in terms of potential energy and polarization surfaces trained on density functional theory data with modern machine learning techniques. Our simulations demonstrate that the transition has a strong order-disorder character, in agreement with diffraction experiments, and provide fresh insight into the approach to equilibrium across the phase transition. We find that the emergence and disappearance of the macroscopic polarization is driven by dipolar switching at the nanometer scale. We also computed the infrared optical absorption spectra in both the ferroelectric and the paraelectric phases, finding good agreement with the experimental Raman frequencies. Often, the almost ideal displacive character of the soft mode detected by Raman scattering in the paraelectric phase has been contrasted with the order-disorder character of the transition suggested by diffraction experiments. We settle this issue by showing that the soft mode coexists with a strong Debye relaxation associated with thermal disordering of the dipoles. The Debye relaxation feature is centered at zero frequency and appears near the transition temperature in both the ferroelectric and the paraelectric phases.
Sr-secondary phase formation is a potentially significant degradation mode threatening solid-oxide cell (SOC) commercial viability. A first-principles thermodynamic study was performed for rhombohedral perovskite (La1-xSrx) MnO3±δ (LSM) to assess its stability against Sr secondary phase formation in SOC applications. In this work, the Sr secondary phase formation reaction free energies were determined by combining ab initio lattice dynamics calculations for the solid phases and an ab initio thermodynamics approach for the gas phases. Furthermore, this approach goes beyond previous thermodynamic modeling studies by integrating first-principles based point-defect equilibria into the analyses. The modeling results indicate an increased tendency to form SrO oxide from LSM upon decreasing the oxygen partial pressure. Additionally, enhancing factors to form the Sr-related secondary phase from the associated SrO activity in LSM are further quantified by considering the equilibrium of SrO reacting with contaminant gas species as a function of temperature and gas pressure.
Understanding irradiation damage and tritium transport in LiAlO2 ceramics is essential for their deployment in tritium-producing burnable absorber rods (TPBARs). Grain boundaries (GBs) play an important role in governing radiation response and tritium transport in LiAlO2 and its secondary phase LiAl5O8. Using molecular dynamics simulations, we investigated defect evolution and tritium diffusion during displacement cascades in single-crystal and bicrystal LiAlO2 and LiAl5O8 at 600 K. The results reveal that GBs suppress the damage in the LiAlO2 bicrystals as compared to single crystals, via interstitial emission. The effect is more pronounced for Li defects, than for Al and O. In LiAl5O8 the damage reduction due to introduction of GB is less pronounced overall. Tritium diffusion coefficients at GBs are higher by factors of 2–10 relative to diffusion inside grain bulk. The effect is particularly pronounced in LiAlO2, where S5, S17, and S25 GBs promote rapid tritium transport, whereas LiAl5O8 exhibits slower diffusion due to reduced free volume at its GBs. These findings evince a trade-off that while GBs mitigate radiation damage by absorbing interstitials, they simultaneously provide fast pathways for tritium migration which is not desirable for TPBAR application. The mechanistic insights gained here establish a foundation for microstructural design strategies to balance radiation tolerance and tritium retention in ceramic breeder materials.
We present a detailed numerical and analytical study of the out-of-equilibrium dynamics of Model G, the dynamical universality class relevant to the chiral phase transition. We perform numerical 3D stochastic (Langevin) simulations of the 𝑂(4) critical point for large lattices in the chiral limit. We quench the system from the high-temperature unbroken phase to the broken phase and study the nonequilibrium dynamics of pion fields. Strikingly, the nonequilibrium evolution of the two-point functions exhibits a regime of growth, a parametrically large enhancement, and a subsequent slow relaxation to equilibrium. We analyze our numerical results using dynamic critical scaling and mean-field theory. The growth of the two-point functions is determined by the nonlinear dynamics of an ideal non-Abelian superfluid, which is a limit of Model G that reflects the broken chiral symmetry. We also relate the nonequilibrium two-point functions to a long-lived parametric enhancement of soft pion yields relative to thermal equilibrium following a quench.
Here we examine run-and-tumble disks in two-dimensional systems where the particles also have a Magnus component to their dynamics. For increased activity, we find that the system forms a motility-induced phase-separated (MIPS) state with chiral edge flow around the clusters, where the direction of the current is correlated with the sign of the Magnus term. The stability of the MIPS state is non-monotonic as a function of increasing Magnus term amplitude, with the MIPS region first extending down to lower activities followed by a break up of MIPS at large Magnus amplitudes into a gel-like state. We examine the dynamics in the presence of quenched disorder and a uniform drive and find that the bulk flow exhibits a drive-dependent Hall angle. This is a result of the side jump effect produced by scattering from the pinning sites and is similar to the behavior found for skyrmions in chiral magnets with quenched disorder.
Beam loss monitors (BLMs) and beam current monitors (BCMs) are ubiquitous at particle accelerators around the world. These simple devices provide noninvasive high-level beam measurements but give no insight into the detailed 6D (𝑥,𝑦,𝑧,𝑝 𝑥 ,𝑝 𝑦 ,𝑝 𝑧 ) beam phase-space distributions or dynamics. We show that generative conditional latent diffusion models can learn intricate patterns to solve the extreme inverse problem of mapping waveforms of tens of BLMs or BCMs along an accelerator to detailed 2D projections of a charged particle beam’s 6D phase-space density. This transformational method can be used at any particle accelerator to transform simple noninvasive devices into detailed beam phase-space diagnostics. We demonstrate this concept via multiparticle simulations of the high-intensity beam in the kilometer-long Los Alamos Neutron Science Center linear proton accelerator.
This letter proposes a novel hybrid method for assessing grid-connected three-phase converter interfaced resources (CIR) dynamics with the IEEE standard 1547-2018 grid support functions (GSFs), which blends physics and data-driven techniques. First, the letter derives an analytical model of a CIR to represent the internal physics and data-driven model (DDM) using a system identification algorithm to represent the rest of the dynamics, including the GSF. The derived hybrid model combines the analytical model of CIR and DDM, which balances accuracy and flexibility and is compared with the detailed switched model. Furthermore, the efficacy of the proposed approach to represent the advanced CIR dynamics is substantiated by power hardware-in-the-loop experiment data where real measurements from a commercial CIR are used to cross-validate the proposed approach. Furthermore, the results indicate that despite simple, the hybrid model accurately reproduces the dynamics of the detailed CIR model with an acceptable accuracy.
Ultrafast stimuli can stabilize metastable states of matter inaccessible by equilibrium means. Establishing the spatiotemporal link between ultrafast excitation and metastability is crucial to understand these phenomena. Here, in this work, we utilize single-shot optical pump–X-ray probe measurements to capture snapshots of the emergence of a persistent polar vortex supercrystal in a heterostructure that hosts a fine balance between built-in electrostatic and elastic frustrations by design. By perturbing this balance with photoinduced charges, an initially heterogeneous mixture of polar phase disorders within a few picoseconds, leading to a state composed of disordered ferroelectric and suppressed vortex orders. On the picosecond–nanosecond timescales, transient labyrinthine fluctuations develop, accompanied by the recovery of the vortex order. On longer timescales, these fluctuations are progressively quenched by dynamical strain modulations, which drive the collective emergence of a single vortex supercrystal phase. Our results, corroborated by dynamical phase-field modelling, reveal non-equilibrium pathways following the ultrafast excitation of designer systems to persistent metastability.
The microwave synchrotron radiation in the sub-cyclotron frequency region has been systematically validated as a diagnostic method for runaway electrons (>1 MeV) with radiation modeling and experiments on the DIII-D tokamak. Experimental observations reveal that sub-cyclotron frequency microwave radiation emerges only after runaway electrons are excited during plasma disruptions. Electron gyro-magnetic radiation modeling confirms that only runaway electrons with energies exceeding 1 MeV can emit radiation in the observed sub-cyclotron frequency band on DIII-D. The synchrotron Razin and Beaming effects are modeled in both the sub-cyclotron and standard Electron Cyclotron Emission (ECE) frequency region. Due to the pronounced beaming effect, the modeling supports that a standard ECE system is insensitive to synchrotron radiation from beamed runaway electrons (p ∥ >> p ⟂ ), but very sensitive to ECE radiation from isotropic suprathermal electrons (100 keV or less). DIII-D experiments further show that combining ECE and sub-cyclotron receivers reveals new insights into transient runaway dynamics during the plateau phase. Certain transient crash events appear only in the sub-cyclotron band or lead to opposite changes on the sub-cyclotron and standard ECE signals, supporting models where transient MHD events can exert a different effect on electrons of different energy levels. This novel diagnostic technique offers a powerful tool for studying and detecting runaway electron dynamics in both present-day and high-field future tokamaks. The diagnostic approach has been extrapolated to the SPARC tokamak, where sub-cyclotron radiation is predicted to respond sensitively and solely to runaway electrons during SPARC’s L-mode startup phase.
The prototypical α → ω phase transition in zirconium is an ideal test bed for our understanding of polymorphism under extreme loading conditions. After half a century of study, a consensus had emerged that the transition is realized via one of two distinct displacive mechanisms, depending on the nature of the compression path. However, recent dynamic-compression experiments equipped with diffraction diagnostics performed in the past few years have revealed new transition mechanisms, demonstrating that our understanding of the underlying atomistic dynamics and transition kinetics is in fact far from complete. We present classical molecular dynamics simulations of the α → ω phase transition in single-crystal zirconium shock compressed along the [0001] axis using a machine-learning-class potential. The transition is predicted to proceed primarily via a modified version of the two-stage Usikov-Zilberstein mechanism, whereby the high-pressure ω phase heterogeneously nucleates at boundaries between grains of an intermediate β phase. We further observe the fomentation of atomistic disorder at the junctions between β grains, leading to the formation of highly defective interstitial material between the ω grains. We directly compare synthetic x-ray diffraction patterns generated from our simulations with those obtained using femtosecond diffraction in recent dynamic-compression experiments, and show that the simulations produce the same unique, anisotropic diffuse scattering signal unlike any previously seen from an elemental metal. Our simulations suggest that the diffuse signal arises from a combination of thermal diffuse scattering, nanoparticlelike scattering from residual kinetically stabilized α and β grains, and scattering from interstitial defective structures. Published by the American Physical Society 2024