Large Phase Space Research Articles

A Jacobian-free pseudo-arclength continuation method for phase transitions in inhomogeneous thermodynamic systems.

Developing phase diagrams for inhomogeneous systems in thermodynamics is difficult, in part, due to the large phase space and the possibility of unstable and metastable solutions arising from first-order phase transitions. Pseudo-arclength continuation (PAC) is a method that allows one to trace out stable and unstable solutions of nonlinear systems. Typically, PAC utilizes the Jacobian in order to implement Newton (or quasi-Newton) steps. In this work, we present a Jacobian-free PAC method that is amenable to the usual workflows in inhomogeneous thermodynamics. We demonstrate our method in systems that have first-order phase transitions, including a novel example of polyelectrolyte complex coacervation in confinement, where multiple surface phase transitions occur and can overlap with one another.

Magnon-mediated topological superconductivity in a quantum wire

Many emergent phases of matter stem from the intertwined dynamics of quasiparticles. Here we show that a topological superconducting phase emerges as the result of interactions between electrons and magnons in a quantum wire and a helical magnet. The magnon-mediated interaction favors triplet superconductivity over a large magnetic phase space region, and stabilizes topological superconductivity over an extended region of chemical potentials. The superconducting gap depends exponentially on the spin-electron coupling, allowing it to be enhanced through material engineering techniques. Published by the American Physical Society 2024

Impact of Planetary Parameters on Water Clouds Microphysics

Potentially habitable exoplanets are targets of great interest for the James Webb Space Telescope and upcoming mission concepts such as the Habitable Worlds Observatory. Clouds strongly affect climate and habitability, but predicting their properties is difficult. In Global Climate Models (GCMs), especially those aiming at simulating Earth, cloud microphysics is often crudely approximated by assuming that all cloud particles have a single, constant size or a prescribed size distribution and that all clouds in a grid cell are identical. For exoplanets that range over a large phase space of planetary properties, this method could result in large errors. In this work, our goal is to determine how cloud microphysics on terrestrial exoplanets, whose condensable is mainly water vapor, depend on aerosol properties and planetary parameters such as surface pressure, surface gravity, and incident stellar radiation. We use the Community Aerosol and Radiation Model for Atmospheres as a 1D microphysical model to simulate the formation and evolution of clouds including the processes of nucleation, condensation, evaporation, coagulation, and vertical transfer. In these 1D idealized experiments, we find that the parameters that determine the macrophysical thermal structure of the atmospheres, including surface pressure and stellar flux, impact cloud radiative effect (CRE) most significantly. Parameters such as gravity and number density of aerosols working as cloud condensation nuclei affect the microphysical processes of cloud formation, including activation and vertical transfer. They also have a significant, though weaker effect on CRE. This work motivates the development of more accurate GCM cloud schemes and should aid in the interpretation of future observations.

Strongly Interacting Photons in 2D Waveguide QED.

One-dimensional confinement in waveguide quantum electrodynamics (QED) plays a crucial role to enhance light-matter interactions and to induce a strong quantum nonlinear optical response. In two or higher-dimensional settings, this response is reduced since photons can be emitted within a larger phase space, opening the question whether strong photon-photon interaction can be still achieved. In this study, we positively answer this question for the case of a 2D square array of atoms coupled to the light confined into a two-dimensional waveguide. More specifically, we demonstrate the occurrence of long-lived two-photon repulsive and bound states with genuine 2D features. Furthermore, we observe signatures of these effects also in free-space atomic arrays in the form of weakly subradiant in-band scattering resonances. Our findings provide a paradigmatic signature of the presence of strong photon-photon interactions in 2D waveguide QED.

High-Performance Iridium-Molybdenum Oxide Electrocatalysts for Water Oxidation in Acid: Bayesian Optimization Discovery and Experimental Testing.

Ir oxides are costly and scarce catalysts for oxygen evolution reaction (OER) in acid. There has been extensive interest in developing alternatives that are either Ir-free or require smaller amounts of Ir to drive the reactions at acceptable rates. One design strategy is to identify Ir-based mixed oxides that achieve similar performance while requiring smaller amounts of Ir. The obstacle to this strategy has been a very large phase space of the Ir-based mixed metal oxides, in terms of the metals combined with Ir and the different crystallographic structures of the mixed oxides, which prevents a thorough exploration of possible materials. In this work, we developed a workflow that uses machine-learning-aided Bayesian optimization in combination with density functional theory to make the exploration of this phase space plausible. This screening identified Mo as a promising dopant for forming acid-tolerant Ir-based oxides for the OER. We synthesized and characterized the Ir-Mo mixed oxides in the form of thin-film electrocatalysts with a known surface area. We show that these mixed oxides exhibited overpotentials ∼30 mV lower than a pure Ir control while maintaining 24% lower Ir dissolution rates than the Ir control. These findings suggest that Mo is a promising dopant and highlight the promise of machine learning to guide the experimental exploration and optimization of catalytic materials.

The Statistical Mechanics of Ideal Magnetohydrodynamic Turbulence and a Solution of the Dynamo Problem

We review and extend the theory of ideal, homogeneous, incompressible, magnetohydrodynamic (MHD) turbulence. The theory contains a solution to the ‘dynamo problem’, i.e., the problem of determining how a planetary or stellar body produces a global dipole magnetic field. We extend the theory to the case of ideal MHD turbulence with a mean magnetic field that is aligned with a rotation axis. The existing theory is also extended by developing the thermodynamics of ideal MHD turbulence based on entropy. A mathematical model is created by Fourier transforming the MHD equations and dynamical variables, resulting in a dynamical system consisting of the independent Fourier coefficients of the velocity and magnetic fields. This dynamical system has a large but finite-dimensional phase space in which the phase flow is divergenceless in the ideal case. There may be several constants of the motion, in addition to energy, which depend on the presence, or lack thereof, of a mean magnetic field or system rotation or both imposed on the magnetofluid; this leads to five different cases of MHD turbulence that must be considered. The constants of the motion (ideal invariants)—the most important being energy and magnetic helicity—are used to construct canonical probability densities and partition functions that enable ensemble predictions to be made. These predictions are compared with time averages from numerical simulations to test whether or not the system is ergodic. In the cases most pertinent to planets and stars, nonergodicity is observed at the largest length-scales and occurs when the components of the dipole field become quasi-stationary and dipole energy is directly proportional to magnetic helicity. This nonergodicity is evident in the thermodynamics, while dipole alignment with a rotation axis may be seen as the result of dynamical symmetry breaking, i.e., ‘broken ergodicity’. The relevance of ideal theoretical results to real (forced, dissipative) MHD turbulence is shown through numerical simulation. Again, an important result is a statistical solution of the ‘dynamo problem’.

A prototype electromagnetic calorimeter for the MUonE experiment: status and first performance results

The MUonE experiment proposes a novel approach to determine the leading hadronic contribution to the muon g-2, from a precise measurement of the differential cross section of the μ-e elastic scattering, achievable by using the CERN SPS muon beam onto atomic electrons of a light target. The detector layout is modular, consisting of an array of identical tracking stations, each one made of a light target and silicon strip planes, followed by an electromagnetic calorimeter made of PbWO4 crystals with APD readout, placed after the last station, and a muon filter. The scattering particles are tracked without any magnetic field, and the event kinematics can be defined in a large phase space region from the expected correlation of the outgoing particle angles. The ambiguity affecting a specific region, with electron and muon outgoing with similar deflection angles, can be solved by identifying the electron track as the one with extrapolation matching the calorimeter cluster or the muon track by associating it to hits in the muon filter. The role of the calorimeter will be important for background estimate and reduction, and to assess systematic errors, providing some useful redundancy and allowing for alternative selections.Beam tests are carried out at CERN with a prototype calorimeter to determine its calibration with both high energy (20–150 GeV) and low energy electrons (1–10 GeV). In late summer a pilot run is scheduled with up to three tracking stations and the calorimeter integrated within a common triggerless readout system. The main motivations for the MUonE calorimeter are discussed, and the status and first performance results will be presented.

Spectroscopic Imaging of the Sun with MeerKAT: Opening a New Frontier in Solar Physics

Solar radio emissions provide several unique diagnostics to estimate different physical parameters of the solar corona, which are otherwise simply inaccessible. However, imaging the highly dynamic solar coronal emissions spanning a large range of angular scales at radio wavelengths is extremely challenging. At gigahertz frequencies, MeerKAT radio telescope is possibly globally the best-suited instrument at present for providing high-fidelity spectroscopic snapshot solar images. Here, we present the first published spectroscopic images of the Sun made using the observations with MeerKAT in the 880–1670 MHz band. This work demonstrates the high fidelity of spectroscopic snapshot MeerKAT solar images through a comparison with simulated radio images at MeerKAT frequencies. The observed images show extremely good morphological similarities with the simulated images. Our analysis shows that below ∼900 MHz MeerKAT images can recover essentially the entire flux density from the large angular-scale solar disk. Not surprisingly, at higher frequencies, the missing flux density can be as large as ∼50%. However, it can potentially be estimated and corrected for. We believe once solar observation with MeerKAT is commissioned, it will enable a host of novel studies, open the door to a large unexplored phase space with significant discovery potential, and also pave the way for solar science with the upcoming Square Kilometre Array-Mid telescope, of which MeerKAT is a precursor.

Machine Learning Accelerated Exploration of Ternary Organic Heterojunction Photocatalysts for Sacrificial Hydrogen Evolution.

Donor-acceptor heterojunctions in organic photocatalysts can provide enhanced exciton dissociation and charge separation, thereby improving the photocatalytic activity. However, the wide choice of possible donors and acceptors poses a challenge for the rational design of organic heterojunction photocatalysts, particularly for large ternary phase spaces. We accelerated the exploration of ternary organic heterojunction photocatalysts (TOHP) by using a combination of machine learning and high-throughput experimental screening. This involved 736 experiments in all, out of possible 4320 ternary combinations. The top ten most active TOHPs discovered using this strategy showed outstanding sacrificial hydrogen production rates of more than 500 mmol g-1 h-1, with the most active ternary material reaching a rate of 749.8 mmol g-1 h-1 under 1 sun illumination. These rates of photocatalytic hydrogen generation are among the highest reported for organic photocatalysts in the literature.

High-throughput ab initio design of atomic interfaces using InterMatch

Forming a hetero-interface is a materials-design strategy that can access an astronomically large phase space. However, the immense phase space necessitates a high-throughput approach for an optimal interface design. Here we introduce a high-throughput computational framework, InterMatch, for efficiently predicting charge transfer, strain, and superlattice structure of an interface by leveraging the databases of individual bulk materials. Specifically, the algorithm reads in the lattice vectors, density of states, and the stiffness tensors for each material in their isolated form from the Materials Project. From these bulk properties, InterMatch estimates the interfacial properties. We benchmark InterMatch predictions for the charge transfer against experimental measurements and supercell density-functional theory calculations. We then use InterMatch to predict promising interface candidates for doping transition metal dichalcogenide MoSe2. Finally, we explain experimental observation of factor of 10 variation in the supercell periodicity within a few microns in graphene/α-RuCl3 by exploring low energy superlattice structures as a function of twist angle using InterMatch. We anticipate our open-source InterMatch algorithm accelerating and guiding ever-growing interfacial design efforts. Moreover, the interface database resulting from the InterMatch searches presented in this paper can be readily accessed online.

Exploring mixed lepton-quark interactions in non-resonant leptoquark production at the LHC

Searches for new physics (NP) at particle colliders typically involve multivariate analysis of kinematic distributions of final state particles produced in a decay of a hypothetical NP resonance. Since the pair-production cross-sections mediated by such resonances are strongly suppressed by the NP scale, this analysis becomes less relevant for NP searches for masses of the BSM resonance above 1 TeV. On the other hand, t-channel processes are less sensitive to the mass of the virtual mediator and therefore larger phase-space can be potentially probed as well as the couplings between the NP particles and the Standard Model fields. The fact that transitions between different generations of quarks and leptons may exist, the potential of the search presented in this article can be used, as a reference guide, to enlarge significantly the scope of searches performed at the LHC to flavour off-diagonal channels, in a theoretically consistent approach. In this work, we study non-resonant production of scalar leptoquarks which have been proposed in the literature to provide a potential avenue for radiative generation of neutrino masses, accommodating as well the existing flavour physics data. Final states involving just two muons at the LHC (μ+μ−), are used as a well-motivated case study.

Pipelines for automating compliance-based elimination and extension (PACE2): a systematic framework for high-throughput biomolecular materials simulation workflows

The formation of biomolecular materials via dynamical interfacial processes, such as self-assembly and fusion, for diverse compositions and external conditions can be efficiently probed using ensemble Molecular Dynamics (MD). However, this approach requires many simulations when investigating a large composition phase space. In addition, there is difficulty in predicting whether each simulation will yield biomolecular materials with the desired properties or outcomes and how long each simulation will run. These difficulties can be overcome by rules-based management systems, including intermittent inspection, variable sampling, and premature termination or extension of the individual MD simulations. Automating such a management system can significantly improve runtime efficiency and reduce the burden of organizing large ensembles of MD simulations. To this end, a computational framework, the Pipelines for Automating Compliance-based Elimination and Extension (PACE2), is proposed for high-throughput ensemble biomolecular materials simulations. The PACE2 framework encompasses Candidate pipelines, where each pipeline includes temporally separated simulation and analysis tasks. When a MD simulation is completed, an analysis task is triggered, which evaluates the MD trajectory for compliance. Compliant simulations are extended to the next MD phase with a suitable sample rate to allow additional, detailed analysis. Non-compliant simulations are eliminated, and their computational resources are reallocated or released. The framework is designed to run on local desktop computers and high-performance computing resources. Preliminary scientific results enabled by the use of PACE2 framework are presented, which demonstrate its potential and validates its function. In the future, the framework will be extended to address generalized workflows and investigate composition-structure-property relations for other classes of materials.

Quantitative prediction of surface energy of high-entropy-alloys based on intrinsic descriptors

A wide range of surface properties of interest are closely correlated to the surface energy of metallic materials. High-entropy-alloys (HEAs) are known for their novel mechanical and physical properties, while their inherent surface complexity hinders the quantitative description of the structure-property relationship. In this work, we utilize the surface electronic descriptor Жsurface, which is based on the period number, group number, valence-electron number and electronegativity of surface atoms, to point-to-point describe the non-local surface environment of complex HEA surfaces with different geometries. We find that surface energy is strongly correlated with the atoms in the HEA single surface layer, while the bulk phase atoms of HEAs slightly affect the linear relationship only when the bulk phase is in the low entropy state, and different geometries mainly lead to the overall shift of surface energy distribution. This model quantitatively correlates surface energy with the intrinsic properties of IrRuRhPdPt, NbMoTaTi and NbMoTaTiV HEAs, and could be helpful to fine-tune the surface energy in materials design. Moreover, our model allows rapid screening of potentially interesting materials through a large phase space of HEA surfaces, owing to that all the parameters are easily accessible from the periodic table of elements.

Observation of skyrmion bubbles in multilayer [Pt/Co/Cu]n using spin-polarized STM

Magnetic multilayers are a promising platform for storage and logic devices based on skyrmion spin textures, due to the large materials phase space for tuning properties. Epitaxial superlattice structures of [Pt/Co/Cu]n thin films were grown by molecular beam epitaxy at room temperature. Spin-polarized scanning tunneling microscopy (SP-STM) of these samples was used to probe the connection between surface structure and skyrmion morphology with nanoscale spatial resolution. Irregular-shaped skyrmion bubbles were observed, with effective diameters from 20 to 200 nm that are much larger than the nanoscale grain structure of the surface topography. Nucleation, annihilation, and motion of skyrmion bubbles could be driven using the stray field of the ferromagnetic tip in repeated imaging, and spin-polarized current/voltage pulses. Our detailed comparison of STM topography and differential conductance images shows that there are no surface defects or inhomogeneities at length scales that could account for the range in skyrmion bubble size or shape observed in the measurements.

Anomalous high [formula omitted] above 2.2 in light element dominated compound Li[formula omitted]OTe due to low thermal conductivity

Thermoelectric materials usually contain heavy metal elements to ensure low lattice thermal conductivity κl. However, such elements like Pb, Bi and Sb have the expenses of high prices and potential risks of pollution. Herein, we propose a novel design strategy for thermoelectrics by constructing new light element dominated materials, such as quasi-antifluorite Li4OTe, with a high figure of merit surpassing 2.2. The introduction of O atom in Li4OTe crystal causes optical phonon softening and large phase space for three-phonon scattering processes, leading to much lower κl (<1 W m−1 K−1) than antifluorite Li2X (X=O, Te). This picture can be extended to other quasi-antifluorites, which will stimulate intense interests in the exploration of the light element dominated compounds, as new environmentally friendly and low-cost thermoelectric materials.

Twisted bilayer graphene as topological heavy fermion: II. Analytical approximations of the model parameters

The recently-introduced topological heavy fermion (THF) model [1] of twisted bilayer graphene (TBG) aims to reconcile the quantum-dot-like electronic structure of the latter observed by scanning tunneling microscopy, with its electron delocalization seen in transport measurements. The THF model achieves this by coupling localized (heavy) fermions with anomalous conduction electrons. Originally, the parameters of the THF model were obtained numerically from the Bistritzer–Macdonald (BM) model of TBG [1]. In this work, we derive analytical expressions for the THF model parameters as a function of the twist angle, the ratio between the tunneling amplitudes at the AA and AB regions (w0/w1), and the screening length of the interaction potential. By numerically computing the THF model parameters across an extensive experimentally-relevant parameter space, we show that the resulting approximations are remarkably good, i.e., within the 30% relative error for almost the entire parameter space. At the single-particle level, the THF model accurately captures the energy spectrum of the BM model over a large phase space of angles and tunneling amplitude ratios. When interactions are included, we also show that the THF description of TBG is good around the magic angle for realistic values of the tunneling amplitude ratios (0.6 ≤ w0/w1 ≤ 1.0), for which the hybridization between the localized and conduction fermions γ is smaller than the onsite repulsion of the heavy fermions U1 (i.e., |γ| &amp;lt; U1).

Cyclic versus Linear Alkylammonium Cations: Preventing Phase Transitions at Operational Temperatures in 2D Perovskites.

Two-dimensional lead halide perovskites offer numerous attractive features for optoelectronics owing to their soft, deformable lattices and high degree of chemical tunability. While alteration of the metal and halide ions gives rise to significant modification of the bandgap energy, the organic spacer cations offer in-roads to tuning phase behavior and more subtle functionalities in ways that remain to be understood. Here, we study six variations of 2D perovskites changing only the organic spacer cations and demonstrate that these components intrinsically impact material response in important ways such as altering crystallographic structure, temperature-induced phase transitions, and photoluminescence emission. Two-dimensional perovskites containing commonly utilized aliphatic linear spacers, such as butylammonium, undergo phase transitions near room temperature. These transitions and temperature changes induce spacer-dependent variations in the emission spectra. Conversely, 2D perovskites comprising cyclic aliphatic spacers, such as cyclobutylammonium, are found to lack first-order phase transitions. These cyclic molecules are more sterically hindered within the crystal lattice, leading to temperature-induced contraction or expansion along certain crystallographic planes but no other significant thermal effects; additionally, they undergo changes in their emission spectra that cannot be explained by simple thermal expansion. Given the similarities in the dielectric and chemical makeup of this set of six alkylammonium molecules, these results are unexpected and suggest a large structural and thermal phase space via spacer manipulation that could lead to improved 2D perovskite functionalization.

Linearizing Toda and SVD flows on large phase spaces of matrices with real spectrum

We consider different phase spaces for the Toda flows (Flaschka, 1974; Moser, 1975) and the less familiar SVD flows (Chu, 1986; Li, 1997). For the Toda flow, we handle symmetric and non-symmetric matrices with real simple eigenvalues, possibly with a given profile. Profiles encode, for example, band matrices and Hessenberg matrices. For the SVD flow, we assume simplicity of the singular values. In all cases, an open cover is constructed, as are corresponding charts to Euclidean space. The charts linearize the flows, converting it into a linear differential system with constant coefficients and diagonal matrix. A variant construction transforms the flows into uniform straight line motion. Since limit points belong to the phase space, asymptotic behavior becomes a local issue. The constructions rely only on basic facts of linear algebra, making no use of symplectic geometry.

Selective electrochemical reductive amination of benzaldehyde at heterogeneous metal surfaces

Ammonia is one of the largest-volume commodity chemicals, and electrochemical routes to ammonia utilization are appealing due to increasingly available renewable electricity. In this work, we demonstrate an electrochemical analog to reductive amination for the synthesis of benzylamine from benzaldehyde and ammonia. Previous works on electrochemical reductive amination have generally focused on proof-of-concept outer-sphere routes. In our system, imine hydrogenation proceeds via an inner-sphere route on an Ag electrocatalyst at ambient conditions with an initial Faradaic efficiency toward the primary amine product of ∼80% and partial current greater than 4 mA/cm2 at −1.96 V versus Fc/Fc+ (−1.36 V versus the normal hydrogen electrode). Ag was selected after evaluating diverse transition metal electrocatalysts, and the rate-determining step was the initial electron transfer to the imine. Overall, this work represents a step toward inner-sphere electrochemical reductive amination systems, opening a large phase space of heterogeneous electrocatalysts for reactions that currently rely on thermochemical routes.

Nonclassicality of axionlike dark matter through gravitational self-interactions

Axion-like particles (ALPs) are promising dark matter candidates. They are typically described by a classical field, motivated by large phase space occupation numbers. Here we show that such a description is accompanied by a quantum effect: squeezing due to gravitational self-interactions. For a typical QCD axion today, the onset of squeezing is reached on $\mathrm{\mu s}$-scales and grows over millennia. Thus within the usual models based on the classical Schr\"odinger-Poisson equation, a type of Gross-Pitaevskii equation, any viable ALP is nonclassical. We also show that squeezing may be relevant on the scales of other self-gravitating systems such as galactic haloes, or solitonic cores. Conversely, our results highlight the incompleteness and limitations of the classical single field description of ALPs.