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At least 613 records · Page 34

Temporal entanglement transitions in the periodically driven Ising chain

Periodically driven quantum systems can host non-equilibrium phenomena without static analogs, including in their entanglement dynamics. Here, we discover (TET) in a Floquet spin chain, which correspond to a quantum phase transition in the spectrum of the entanglement Hamiltonian and are signaled by dynamical spontaneous symmetry breaking. We identify the symmetry principles underlying these transitions: they appear when the driven Hamiltonian preserves global symmetry (here, ℤ2), the initial state respects this symmetry, and the reduced density matrix carries weight in both subsystem-parity sectors, with TET occurring precisely when the sector weights become equal (given the previous two conditions are also satisfied). Intriguingly, we find these transitions across a broad range of driving frequencies (from adiabatic to high-frequency regime) and independently of drive details, where they manifest as periodic, sharp entanglement spectrum reorganizations marked by the Schmidt-gap closure, a vanishing entanglement echo, and symmetry-quantum-number flips, while remaining invisible to conventional local observables. At high frequencies, the entanglement Hamiltonian acquires an intrinsic timescale decoupled from the drive period, rendering the transitions genuine steady-state features. Finite-size scaling reveals universal critical behavior with correlation-length exponent 𝜈 = 1, matching equilibrium Ising universality despite its emergence from purely dynamical mechanisms decoupled from static criticality. Furthermore, our work establishes TET as novel features in Floquet quantum matter.

36 MATERIALS SCIENCE↗

Molecular Dynamics Investigation of the Structural and Mechanical Properties of Off-Stoichiometric Epoxy Resins

Molecular dynamic (MD) simulations were performed to compute the mechanical properties of off-stoichiometric epoxy resins as a function of hardener/epoxy mixture ratio (r). Properties were characterized in relation to their microscopic structures. Such resins have been used recently for adhesive-free bonding of large-scale composite structures using the co-curing-ply method. In this process, two partially precured composite panels with hardener-poor (HP) off-stoichiometric resins are coupled with ply(ies) of complementary hardener-rich (HR) formulations and then cured simultaneously. This bonding process has the potential to produce reliable and certifiable composite joints without the need for additional fasteners, which are often required for many conventional bonding methods because even small amounts of contamination can cause a weak bond. The reflow and mixing of the HP/HR resin in this bonding process result in a joint with no discernable interface that should not be susceptible to surface contamination. However, incomplete mixing of the two offset resins may result in chemical heterogeneity of the cured polymeric joint. Thus, different r values may be obtained across the joint. Classical MD simulations were performed to compute the Young’s modulus of polymers with different r values and correlate their properties to network structures. High stiffness was associated with molecular packing due to chemical crosslinking, leading to a single network structure. Moreover, the networks became denser as the ratio approached the stoichiometric value r = 1. Thus, the r = 1 systems were single clusters, with high stiffness, high molecular weight, and a high degree of crosslinking. Structural properties such as radius of gyration and mean square displacement were determined to investigate the variation in the stiffness with respect to r. This MD simulation study was validated with experimental measurements.

Chang Woon Jang↗

A general relaxation theory of simple liquids

A relatively simple relaxation theory to account for the behavior of liquids under dynamic conditions was proposed. The general dynamical equations are similar in form to the phenomenological relaxation equations used in theories of viscoelasticity, however, they differ in that all the coefficients of the present equations are expressed in terms of thermodynamic and molecular quantities. The theory is based on the concept that flow in a liquid distorts both the radial and the velocity distribution functions, and that relaxation equations describing the return of these functions to their isotropic distributions, characterizing a stationary liquid, can be written. The theory was applied to the problems of steady and oscillatory shear flows and to the propagation of longitudinal waves. In all cases classical results are predicted for strain rates, and an expression for the viscosity of a liquid, simular to the Macedo-Litovitz equation, is obtained.

Merilo, M.↗

Long-range exciton diffusion in molecular non-fullerene acceptors

Abstract The short exciton diffusion length associated with most classical organic semiconductors used in organic photovoltaics (5-20 nm) imposes severe limits on the maximum size of the donor and acceptor domains within the photoactive layer of the cell. Identifying materials that are able to transport excitons over longer distances can help advancing our understanding and lead to solar cells with higher efficiency. Here, we measure the exciton diffusion length in a wide range of nonfullerene acceptor molecules using two different experimental techniques based on photocurrent and ultrafast spectroscopy measurements. The acceptors exhibit balanced ambipolar charge transport and surprisingly long exciton diffusion lengths in the range of 20 to 47 nm. With the aid of quantum-chemical calculations, we are able to rationalize the exciton dynamics and draw basic chemical design rules, particularly on the importance of the end-group substituent on the crystal packing of nonfullerene acceptors.

14 SOLAR ENERGY↗

Characterizing the Mechanisms of Ca and Mg Carbonate Ion-Pair Formation with Multi-Level Molecular Dynamics/Quantum Mechanics Simulations

The carbonate minerals of Ca and Mg are abundant throughout the lithosphere and have recently garnered significant research interest as possible long-term carbon sinks in the sequestration of atmospheric carbon dioxide. Nonetheless, an understanding of the atomic-level processes comprising their mineralization remains limited. Furthermore, we characterize and contrast the mechanisms of contact ion-pair formation in aqueous Ca and Mg carbonate systems, which represents the most fundamental step leading to the formation of their mineral solids. Utilizing multilevel embedded correlated wavefunction-based ab initio molecular dynamics/quantum mechanics simulations, we characterize not only the dynamics of these processes but also factors arising from the electronic structure of the involved species, revealing further details of the fundamentally different mechanisms for the interconversion between the contact ion-pairs and solvent-shared ion-pairs of Ca versus Mg carbonate.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Symmetry Breaking and Error Correction in Open Quantum Systems

Symmetry-breaking transitions are a well-understood phenomenon of closed quantum systems in quantum optics, condensed matter, and high energy physics. However, symmetry breaking in open systems is less thoroughly understood, in part due to the richer steady-state and symmetry structure that such systems possess. For the prototypical open system—a Lindbladian—a unitary symmetry can be imposed in a “weak” or a “strong” way. We characterize the possible $\mathbb{Z}_n$ symmetry-breaking transitions for both cases. In the case of $\mathbb{Z}_2$, a weak-symmetry-broken phase guarantees at most a classical bit steady-state structure, while a strong-symmetry-broken phase admits a partially protected steady-state qubit. Viewing photonic cat qubits through the lens of strong-symmetry breaking, we show how to dynamically recover the logical information after any gap-preserving strong-symmetric error; such recovery becomes perfect exponentially quickly in the number of photons. Further, our study forges a connection between driven-dissipative phase transitions and error correction.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Recent Developments in DFTB+, a Software Package for Efficient Atomistic Quantum Mechanical Simulations

DFTB+ is a flexible, open-source software package developed by its community, designed for fast and efficient atomistic quantum mechanical simulations. It employs various methods that approximate density functional theory (DFT), such as density functional-based tight binding (DFTB) and the extended tight binding (xTB) approach allowing simulations of large systems over extended time scales with reasonable accuracy, while being significantly faster than traditional ab initio methods. In recent years, several new extensions of the DFTB method have been developed and implemented in the DFTB+ program package in order to improve the accuracy and generality of the available simulation results. In this paper, we review those enhancements, show several use case examples and discuss the strengths and limitations of its features.

36 MATERIALS SCIENCE↗

A quantum processor based on coherent transport of entangled atom arrays

The ability to engineer parallel, programmable operations between desired qubits within a quantum processor is key for building scalable quantum information systems. In most state-of-the-art approaches, qubits interact locally, constrained by the connectivity associated with their fixed spatial layout. Here we demonstrate a quantum processor with dynamic, non-local connectivity, in which entangled qubits are coherently transported in a highly parallel manner across two spatial dimensions, between layers of single- and two-qubit operations. Our approach makes use of neutral atom arrays trapped and transported by optical tweezers; hyperfine states are used for robust quantum information storage, and excitation into Rydberg states is used for entanglement generation. We use this architecture to realize programmable generation of entangled graph states, such as cluster states and a seven-qubit Steane code state. Furthermore, we shuttle entangled ancilla arrays to realize a surface code state with thirteen data and six ancillary qubits and a toric code state on a torus with sixteen data and eight ancillary qubits. Finally, we use this architecture to realize a hybrid analogue–digital evolution and use it for measuring entanglement entropy in quantum simulations, experimentally observing non-monotonic entanglement dynamics associated with quantum many-body scars. Realizing a long-standing goal, these results provide a route towards scalable quantum processing and enable applications ranging from simulation to metrology.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Scalable simulation of coupled adsorption and transport of methane in confined complex porous media with density preconditioning

The growing significance of shales and tight formations in the transition to less carbon-intensive and clean energy drives the research endeavor to understand the physics of gas flow within these systems. However, shales are composed of massively heterogeneous physical and chemical features. Most nano-sized pores connect to millimeter-scale fractures, leading to multiscale transport. These nano-scale pore throats demonstrate non-classical flow behavior, such as non-negligible slip velocities and adsorbed gas layers at the boundary. As a result, classical computational fluid dynamics models do not capture the physics. In this work, we develop a coupling scheme for the multiple-relaxation-time (MRT) lattice Boltzmann (LB) method that integrates the Peng-Robinson equation of state into a pseudo-potential interaction model to capture the physics of methane flow in irregular networks of channels that represent nano-scale porous media. We use atomistic simulations to calibrate and validate our model in slit nano-channels. We propose a preconditioning scheme to initialize the coupled transport and adsorption simulation of methane in complex porous media. The results of this implementation of LB agree with Direct Simulation Monte Carlo (DSMC) and Molecular Dynamics (MD) simulations. We then scale up the LB implementation through vectorization and indirect addressing. We parallelize it using Message Passing Interface (MPI) and OpenMP frameworks to simulate transport and adsorption in complex media with a million lattices. Additionally, we analyze the differences between coupled and transport-only simulations in two case studies and show that considering phase behavior, i.e., adsorption, can significantly change the flow behavior. This work constitutes an important step towards bridging the gap between molecular flow and system-scale behavior of complex disordered porous media.

42 ENGINEERING↗

Refined Classical Force Field for Choline Chloride and Ethylene Glycol Mixtures over Wide Composition Range

In this work, a classical force field based on the General Amber Force Field (GAFF) was refined for the simulation of choline chloride (ChCl) and ethylene glycol (EG) mixtures over a wide composition range by scaling the partial charges and van der Waals parameters. The scaling factors were derived by fitting the simulation results to only eight experimental density and viscosity data points of pure EG, and ChCl/EG mixtures at 1:2, 1:4, and 1:6 molar ratios. Using the refined force field, properties essential for electrochemical applications such as density, viscosity, self-diffusion coefficient, and ionic conductivity were calculated, and excellent agreement to experimental results was found even for compositions and temperatures not used in the fitting procedure. In addition, new experimental data for density, viscosity, and ionic conductivity are reported as a function of temperature and composition for this mixture. To the best of our knowledge, this is the first classical force field developed for the study of ChCl/EG mixtures over a composition range that includes the eutectic point. Using the new model, the liquid dynamics was studied in terms of ionic conductivity. It was found that the dynamics in ChCl/EG mixtures with ChCl mole fraction higher than 20% is similar to that of ionic liquids, high temperature molten salts, and highly concentrated water-in-salt electrolytes.

25 ENERGY STORAGE↗

Estimating Eigenenergies from Quantum Dynamics: A Unified Noise-Resilient Measurement-Driven Approach

Ground state energy estimation in physical, chemical, and materials sciences is one of the most promising applications of quantum computing. In this work, we introduce a new hybrid approach that finds the eigenenergies by collecting real-time measurements and post-processing them using the machinery of dynamic mode decomposition (DMD). From the perspective of quantum dynamics, we establish that our approach can be formally understood as a stable variational method on the function space of observables available from a quantum many-body system. We also provide strong theoretical and numerical evidence that our method converges rapidly even in the presence of a large degree of perturbative noise, and show that the method bears an isomorphism to robust matrix factorization methods developed independently across various scientific communities. Our numerical benchmarks on spin and molecular systems demonstrate an accelerated convergence and a favorable resource reduction over state-of-the-art algorithms. The DMD-centric strategy can systematically mitigate noise and stands out as a leading hybrid quantum-classical eigensolver.

Shen, Yizhi↗

Interstitial proton transport through defective MXenes

Proton transport across nanometer-thick membranes in an aqueous medium is important for applications in energy and molecular sieving. Recently, Hu et al. [Nature 516(7530), 227–230 (2014)] experimentally demonstrated proton tunneling through 2D materials like graphene and hexagonal boron nitride, opening up a wide range of applications in hydrogen-based technologies such as fuel cells. Here, we demonstrate proton transport in an aqueous medium across a 2D cubic Ti 2 C membrane, a representative defective MXene, from ab initio molecular dynamics simulations. We observe bidirectional translocation of protons, which occurs through the interstitial vacancies in the surface. We show from our simulations that water dissociates on the membrane and the dissociated proton moves into the interstitial sites in the membrane. The proton hops from interstitial-to-interstitial and transports across the membrane. Here, we also show that this interstitial proton transport is associated with an induced electric field that is modulated with bidirectional transport of protons across the membrane.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Potentials of mean force fail to describe chemical bond-breaking in solution

Many liquid phase studies assume that the potential energy surfaces of reacting molecules are the same as in the gas phase, neglecting complex solvent dynamics that can completely alter the nature of chemical reactivity. Even studies that include solvent effects typically only consider them in an average, equilibrium way as part of a potential of mean force (PMF). In this work, we use mixed quantum/classical simulations to compare how equilibrium and non-equilibrium solvent motions affect the photodissociation of a simple diatomic molecule, NaK + , in liquid tetrahydrofuran. A PMF analysis shows that as the excited-state molecule dissociates with the solvent at equilibrium, the bonding electron remains associated with K + at short bond distances but eventually localizes on Na + at the end of dissociation. When we examine non-equilibrium dynamical photodissociation trajectories, however, we find that they fall into three distinct categories: about a quarter of them have the bonding electron mainly associated with Na + , another quarter stay mainly associated with K + , and about half have the bonding electron shared roughly equally between the two ions. The results show that equilibrium PMFs cannot accurately describe the dynamics of bond-breaking chemical reactions in solution because there is insufficient time for the solvent to reach equilibrium on the time scale over which bond dissociation occurs. Furthermore, our analysis shows that the solvent coupling between the electronic energy surfaces is similar at and away from equilibrium, suggesting that other factors, such as solute velocity-driven solvent memory effects, play a more important role in explaining the failure of the equilibrium PMF to predict the non-equilibrium dynamics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Lubrication of Machine Elements

The understanding of hydrodynamic lubrication began with the classical experiments of Tower and Petrov. Reynolds used a reduced form of the Navier-Stokes equations and the continuity equation to generate a second order differential equation for the pressure in the narrow, converging gap of a bearing contact. Such a pressure enables a load to be transmitted between the surfaces with very low friction since the surfaces are completely separated by a film of fluid. In such a situation it is the physical properties of the lubricant, notably the dynamic viscosity, that dictate the behavior of the contact. The understanding of boundary lubrication is normally attributed to Hardy and Doubleday. In boundary lubrication it is the physical and chemical properties of thin films of molecular proportions and the surfaces to which they are attached that determine contact behavior. The lubricant viscosity is not an influential parameter. Research is devoted to a better understanding and more precise definition of other lubrication regimes between these extremes. One such regime, elastohydrodynamic lubrication, occurs in nonconformal contacts, where the pressures are high and the bearing surfaces deform elastically. In this situation the viscosity of the lubricant may raise considerably, and this further assists the formation of an effective fluid film. The science of these three lubrication regimes (hydrodynamic, elastohydrodynamic, and boundary) are described and the manner in which this science is used in the design of machine elements is examined.

Hamrock, Bernard J.↗

A First Principles Approach to Spectral Phonon Transport in Heterostructures

Understanding thermal transport across interfaces which give rise to a thermal resistance (also known as Kapitza resistance) is a critical issue affecting the development of nanotechnologies. Much modern and emergent nanotechnology consist of adjacent materials, and phonon mediated heat transfer governs thermal behavior across internal interfaces in these devices. The physics of thermal transport in solids are governed both by phenomena occurring at the atomic scale and interactions with the material's microstructure. The forecasting of fundamental quantities such as temperature, heat flux and thermal conductivity typically employs the semi-classical Boltzmann transport equation to predict the macroscopic behavior of materials in terms of the microscopic dynamics of its heat carriers. Kapitza resistance was first discovered in liquid helium experiments and has led to a fundamental research thrust in micro and nano-scale heat transport, the behavior of thermal carriers across internal interfaces. Thermal interfacial resistance (TIR) is a widely studied phenomenon, first engaged by Swartz and Pohl through their development of the acoustic and diffuse mismatch methods, then continued through myriad efforts with varying methods and approaches in an attempt to resolve carrier behavior at thermal interfaces. Many of the fundamental approaches to TIR have been at the nanoscale, and research is conducted with molecular dynamics (MD) and density functional theory (DFT) methods. The limitations of these methods is system size; atomistic methods tend to be limited to system sizes of 100,000 atoms or less. Larger length-scale methods have also been pursued, based on the principles of acoustic or diffuse mismatch, but not all include simulation of TIR using a full phonon band spectrum, or temperature dependent methods. Our approach to enabling phonon transport in layered materials draws upon our previous work of demonstrating spectrally coupled phonon transport in homogeneous and heterogeneous materials. We use a semi-analytical approach in which the Bose-Einstein (B-E) statistics set the strength of the phonon radiance in a frequency group, but the B-E statistics are informed with information from the transport system. The B-E statistics in a single frequency group feels the influence of all the groups through the spatial temperature. We also include a new field term which is an indicator of the amount of non-equilibrium behavior of the phonon spectrum---this is added to the phonon source term in all groups to ensure closure and conservation of energy, as the phonon groups in the transport system and the analytical systems are coupled. This work builds upon our previous approach by adding a phonon coupling term at an internal interface, using the principles of the DMM through transmission and reflection coefficients. In this work, the coefficients are determined through computing a common temperature at the interface, influenced by the phonon band structure of both materials, in effect, providing mixing between the two material systems and using the common temperature to set the strength of the phonon radiance at the boundaries on either side of the interface. Our approach uses material properties computed along various crystallographic orientations, and while some isotropy is built into the interface condition, the material properties weight the phonon distributions in the proper crystalline direction. Greater resolution of phonon behavior in proximity to an interface, and more accurate predictions of TIR are obtained. While it is true the assumption of diffuse mismatch can yield inconsistent results compared to experiment especially at low temperatures, this work focuses on room temperature and beyond effects, for future applications in nuclear fuel, or thermoelectric devices; a modified mismatch approach may be feasible if applied properly. Additionally, our methods focus on bridging mesoscale to engineering scale

36 MATERIALS SCIENCE↗

Correlation between time and angular alignment in molecular dynamics simulations of heavy ion collisions

Neutron-proton equilibration is a process which has been used to study the density dependence of the symmetry energy term in the nuclear equation-of-state. Here, this study utilizes constrained molecular dynamics (CoMD) simulations of 70 Zn + 70 Zn with collision energies of 35 and 45 MeV/nucleon. An algorithm is used which searches through CoMD events and identifies the PLF* after it separates from the target and determines its lifetime, Δt. It also determines the fragments that the PLF* breaks apart into and determines their angular alignment. This technique gives an opportunity to explore how the average alignment of dynamically produced fragments, $\langle$α $\rangle$ dyn , evolves with PLF* lifetime. An approximately linear relationship was determined with d$\langle$α $\rangle$ dyn /dΔt = 0.98 ± 0.08 rad / zs and 1.06 ± 0.09 rad / zs for the 35 and 45 MeV / nucleon, respectively, indicating a correlation with magnitude consistent with classically determined values which were used for prior experimental studies.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Unraveling the multi-step crystallization mechanism of polytetrafluoroethylene, modified polytetrafluoroethylene, and their nanocomposites with boron nitride nanobarbs: Experimental insights and theoretical analysis

The non-isothermal crystallization behavior and kinetics of polytetrafluoroethylene (PTFE) composites with boron nitride nanobarb (BNNB), a new generation nanostructure with unique surface morphology and mechanical “barbs” have been analyzed, understanding these properties is essential for their high-end applications as thermal interface materials (TIM) for microwave, 5G and microelectronic devices. The analysis of the crystallization parameters includes crystallization onset, peak and end temperatures, crystallization half-life and overall crystallinity of PTFE, modified PTFE and their BNNB composites. The results were further analyzed using theoretical models such as the combined Avrami-Ozawa model. It was found that BNNB supports crystallization in the modified PTFE but shows minimal effect on the crystallization of PTFE. Due to the limitation of the classical theoretical models used above in fully characterizing the multi-step crystallization process of PTFE, an in-depth analysis using the model-free advanced isoconversional computation was used to characterize the PTFE crystallization based on the evolution of activation energy with fractional crystallinity and for the first time with temperature. Three kinetic regions were identified in the crystallization mechanism. Here, this study investigated the molecular organization and microstructural evolution of PTFE, modified PTFE and their composites during non-isothermal crystallization using advanced X-ray scattering measurements. An insight into the changes undergone by the material's microstructural units including crystallite size and morphology, lamellar thickness and lamellar interfacial layer thickness, and crystallographic phase dynamics during non-isothermal cooling from the melt, was provided here in this work. The effect of copolymer modification of PTFE and the inclusion of pristine and functionalized BNNB (a thermally conductive and electrically insulating ceramic) are both new investigations that provide valuable knowledge for the development of materials with strong matrix-nanofiller interaction and guidance for optimizing sintering and cooling cycles, two key steps in PTFE processing that largely affect the material microstructural features. Overall, the result of the three-part investigation demonstrates that BNNB supports crystallization in the modified PTFE up to 20 wt% concentration and at low and high cooling rates typically used in the industrial processing of PTFE.

36 MATERIALS SCIENCE↗

Molecular structure retrieval directly from laboratory-frame photoelectron spectra in laser-induced electron diffraction

Ubiquitous to most molecular scattering methods is the challenge to retrieve bond distance and angle from the scattering signals since this requires convergence of pattern matching algorithms or fitting methods. This problem is typically exacerbated when imaging larger molecules or for dynamic systems with little a priori knowledge. Here, we employ laser-induced electron diffraction (LIED) which is a powerful means to determine the precise atomic configuration of an isolated gas-phase molecule with picometre spatial and attosecond temporal precision. We introduce a simple molecular retrieval method, which is based only on the identification of critical points in the oscillating molecular interference scattering signal that is extracted directly from the laboratory-frame photoelectron spectrum. The method is compared with a Fourier-based retrieval method, and we show that both methods correctly retrieve the asymmetrically stretched and bent field-dressed configuration of the asymmetric top molecule carbonyl sulfide (OCS), which is confirmed by our quantum-classical calculations.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗