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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Localization of Nonblinking Point Sources Using Higher-Order-Mode Detection and Optical Heterodyning: Developing a Strategy for Extending the Scope of Molecular, Super-resolution Imaging

While the stochastic, “blinking” nature of fluorescent systems has enabled the super-resolution of their localization by the fitting of their point-spread functions (PSFs), this strategy cannot be exploited for similar resolution of “nonblinking” systems, such as those that might be encountered in a coherent Raman experiment. An alternative method for subdiffraction-limited imaging lies in the exploitation of optical heterodyning. For example, if a Gaussian PSF (a TEM00 mode) of a point emitter is displaced with respect to the origin of the optical system, photons in the higher-order TEM modes carry information about that displacement. Information concerning the displacement can be extracted from photons in these higher-order modes. These photons can be collected by optical heterodyning, which exploits the large gain in a detector’s response to an optical signal from an emitter coupled to a local oscillator, which is prepared in the TEM of interest, e.g., TEM10. We have generalized and developed the heterodyning technique to localize point emitters via the detection of higher-order spatial modes. We have developed a theoretical approach to find a practical estimation limit of the localization parameters using a realistic model that accounts for shot noise, background noise, and Gaussian noise. To demonstrate the applicability of the method, we designed experiments in which a laser is a surrogate for one and two point emitters. Using the Fisher information and its accompanying Cramér-Rao lower bound, we demonstrate super-resolution localization in these cases: we show that objects can be localized to roughly 2–3 orders of magnitude of their point-spread function’s size for a given optical system. Finally and most importantly, it is suggested that the results will ultimately be generalizable to multiple emitters and, most importantly, to “nonblinking” molecular systems, which will be essential for broadening the scope of super-resolution measurements beyond the limits of fluorescence-based techniques.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Charge Dependence of Local Hydration Dynamics in Poly(Acrylic Acid) Solutions

Localized measurements of hydration dynamics surrounding poly(acrylic acid) (pAA) chains are executed using Overhauser dynamic nuclear polarization relaxometry to determine the role of polymer protonation state on the polymer solvation environment. Alterations in polymer concentration and solution pH uncovered three different regimes of local water dynamics ranging from bulk-water-like to subdued water diffusivity. These experiments, combined with molecular dynamics simulations, reveal that the presence of deprotonated carboxylic acid groups promotes a hydrophilic local environment and extended polymer chain configurations that together incentivize the incorporation of bulk-like water near the polymer. This results in a stretched polymer conformation that leads to faster observed hydration dynamics in the local hydration environment. Meanwhile, protonated carboxylic acid groups are expected to engage in intrapolymer hydrogen bonding between monomer groups, resulting in a more collapsed conformation and slower observed hydration dynamics. The importance of the carboxylic acid groups on mediating hydration behavior is further illustrated by their role in dictating the solvation environment around poly(acrylic acid-stat-(poly(ethylene glycol) methyl ether acrylate) (p(AA-stat-PEGMEA)) copolymers with varying monomer ratios. Furthermore, these local hydration measurements establish a connection between local water dynamics and polymer chain conformation and may provide additional molecular perspective into poly(acrylic acid)’s classification as a superabsorbent polymer.

Conformation↗
DOE OSTI2016

Hybrid Optical–Thermal Antennas for Enhanced Light Focusing and Local Temperature Control

Metal nanoantennas supporting localized surface plasmon resonances have become an indispensable tool in bio(chemical) sensing and nanoscale imaging applications. The high plasmon-enhanced electric field intensity in the visible or near-IR range that enables the above applications may also cause local heating of nanoantennas. We present a design of hybrid optical–thermal antennas that simultaneously enable intensity enhancement at the operating wavelength in the visible and nanoscale local temperature control. We demonstrate a possibility to reduce the hybrid antenna operating temperature via enhanced infrared thermal emission. We predict via rigorous numerical modeling that hybrid optical–thermal antennas that support high-quality-factor photonic-plasmonic modes enable up to 2 orders of magnitude enhancement of localized electric fields and of the optical power absorbed in the nanoscale metal volume. At the same time, the hybrid antenna temperature can be lowered by several hundred degrees with respect to its all-metal counterpart under continuous irradiance of 104–105 W/m2. The temperature reduction effect is attributed to the enhanced radiative cooling, which is mediated by the thermally excited localized surface phonon polariton modes. We further show that temperature reduction under even higher irradiances can be achieved by a combination of enhanced radiative and convective cooling in hybrid antennas. To conclude, we demonstrate how hybrid optical–thermal antennas can be used to achieve strong localized heating of nanoparticles while keeping the rest of the optical chip at low temperature.

42 ENGINEERING↗
DOE OSTI2024

Tailoring Local Chemical Ordering via Elemental Tuning in High-Entropy Alloys

Due to the large multi-elemental space desired for property screening and optimization, high-entropy alloys (HEAs) hold greater potential over conventional alloys for a range of applications, such as structural materials, energy conversion, and catalysis. However, the relationship between the HEA composition and its local structural/elemental configuration is not well understood, particularly in noble-metal-based HEA nanomaterials, hindering the design and development of nano-HEAs in energy conversion and catalysis applications. In this work, we determined precise atomic-level structural and elemental arrangements in model HEAs composed of RhPtPdFeCo and RuPtPdFeCo to unveil their local characteristics. Notably, by changing just one constituent element in the HEA (Rh to Ru), we found dramatic changes in the elemental arrangement from complete random mixing to a local single elemental ordering feature. Additionally, we demonstrate that the local ordering in RuPtPdFeCo can be further controlled by varying the Ru concentration, allowing us to toggle between local Ru clustering and distinct heterostructures in multicomponent systems. Overall, our study presents a practical approach for manipulating local atomic structures and elemental arrangements in noble-metal-based HEA systems, which could provide in-depth knowledge to mechanistically understand the functionality of noble-metal-based HEA nanomaterials in practical applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Local Structure of Ba 1-x Sr x TiO 3 and BaTi 1-y Zr y O 3 Nanocrystals Probed by X-ray Absorption and X-ray Total Scattering

The effect of isovalent chemical substitution on the magnitude and coherence length of local ferroelectric distortions present in sub-20 nm Ba 1–x Sr x TiO 3 (x = 0.0, 0.30, 0.50, 1.0) and BaTi 1–y Zr y O 3 (y = 0.0, 0.15, 0.50, 1.0) nanocrystals synthesized at room temperature is investigated using X-ray absorption near edge structure (XANES) and pair distribution function analysis of X-ray total scattering data (PDF). Although the average crystal structure of the nanocrystals is adequately described by a centrosymmetric, cubic Pm3¯m space group, local ferroelectric distortions due to the displacement of the titanium atom from the center of the perovskite lattice are observed for all compositions, except BaZrO 3 . The symmetry of the ferroelectric distortions is adequately described by a tetragonal P4mm space group. The magnitude of the local displacements of the titanium atom in BaTiO 3 nanocrystals is comparable to that observed in single crystals and bulk ceramics, but the coherence length of their ferroelectric coupling is much shorter (≤20 Å). Substitution of Sr 2+ for Ba 2+ and of Zr 4+ for Ti 4+ induces a tetragonal-to-cubic transition of the room temperature local crystal structure, analogous to that observed for single crystals and bulk ceramics at similar compositions. This transition is driven by a reduction of the magnitude of the local displacements of the titanium atom and/or of the coherence length of their ferroelectric coupling. Replacing 50% of Ba 2+ with Sr 2+ slightly reduces the magnitude of the titanium displacement, but the coherence length is not affected. In contrast, replacing 15% of the ferroelectrically active Ti 4+ with Zr 4+ leads to a significant reduction of the coherence length. Deviations from the ideal solid solution behavior are observed in BaTi 1–y Zr y O 3 nanocrystals and are attributed to an inhomogeneous distribution of the barium atoms in the nanocrystal. Composition–structure relationships derived for Ba 1–x Sr x TiO 3 and BaTi 1–y Zr y O 3 nanocrystals demonstrate that the evolution of the room temperature local crystal structure with chemical composition parallels that of single crystals and bulk ceramics, and that chemical control over ferroelectric distortions is possible in the sub-20 nm size range. In addition, the potential of PDF analysis of total scattering data to probe compositional fluctuations in nanocrystals is demonstrated.

Rabuffetti, Federico A.↗
DOE OSTI2019

Impacts of Local Convective Processes on Rain on the Caribbean Island of Puerto Rico

Abstract This study aims to determine the impacts of tropical island processes on local convective storms. An analysis of rain events on the island of Puerto Rico between 1 June 2015 and 31 July 2016 showed that local island‐enhanced western storms accounted for 89 of 322 storms. This period is of particular importance for the Caribbean as 2015 was one of the driest years on record. While large‐scale influences such as the El Niño–Southern Oscillation, the North Atlantic Oscillation, African easterly waves, and Saharan dust transport modulate moisture conditions in the region, correlations between precipitation and El Niño–Southern Oscillation (−0.14), North Atlantic Oscillation (−0.42), and Saharan dust (0.1) for 1980–2016 ranged from weak to moderate. Local data for the island of Puerto Rico from weather stations, the Convection, Aerosol, and Synoptic‐Effects in the Tropics field campaign, and the North American Mesoscale model support the initiation or enhancement of convective rain events due to local island processes. In particular, analysis of surface wind speed/direction, convective available potential energy, lifted index, and the bulk Richardson number substantiate local instability due to surface heating, orographic uplift, and sea breeze trade‐wind convergence. These convective forcings along with available precipitable water in excess of 50 mm ultimately led to intense storms despite severe rainfall‐mitigating dust episodes for which aerosol optical thickness exceeded 0.4. These results may have major implications for considering the impacts of local air‐sea‐land interactions on rainfall over other tropical islands.

Hosannah, N.↗
DOE OSTI2020

Response of Landfalling Atmospheric Rivers on the U.S. West Coast to Local Sea Surface Temperature Perturbations

Atmospheric rivers (ARs) play a crucial role in the hydroclimate of the U.S. west coast. While the impact of large-scale sea surface temperature (SST) patterns on ARs is well recognized, the specific roles of local SST on ARs have not been systematically investigated. Here, we analyzed the landfalling ARs from two regional climate simulations that differ only in the local SST. With local SST warming, AR frequency increases across the U.S. west coast, with comparable contributions from the spatial expansion of ARs and emergence of new ARs. AR landfalling area, inland intrusion distance, and intensity also increase, with landfalling area showing the largest sensitivity. Although local SST warming only increases the AR moisture by ~0.4%/K, AR-related precipitation increases by 3%/K, demonstrating the important impact of local SST warming on intensifying storms. Hence, local SST is important for accurate depiction of ARs and their precipitation in the western United States.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Altering the localization and toxicity of arsenic in rice grain

Previous work has shown that inorganic As localizes in rice bran whereas DMA localizes in the endosperm, but less is known about co-localization of As and S species and how they are affected by growing conditions. We used high-resolution synchrotron X-ray fluorescence imaging to image As and S species in rice grain from plants grown to maturity in soil (field and pot) and hydroponically (DMA or arsenite dosed) at field-relevant As concentrations. In hydroponics, arsenite was localized in the ovular vascular trace (OVT) and the bran while DMA permeated the endosperm and was absent from the OVT in all grains analyzed, and As species had no affect on S species. In pot studies, soil amended with Si-rich rice husk with higher DMA shifted grain As into the endosperm for both japonica and indica ecotypes. In field-grown rice from low-As soil, As localized in the OVT as arsenite glutathione, arsenite, and DMA. Results support a circumferential model of grain filling for arsenite and DMA and show Si-rich soil amendments alter grain As localization, potentially lessening risk to rice consumers.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2026

An AI-driven framework for evaluating local and state authorities’ permitting processes

The demand for new energy infrastructure is increasing across the United States, but heterogenous permitting processes and embedded requirements across different local jurisdictions can cause project delays, increase “soft costs,” and hinder developer expansion. This study analyzes the variability in local permitting requirements across the U.S. and develops a quantitative approach to describe their clarity and effectiveness in enabling infrastructure project development. By using an Energy Language Model (ELM), a large language model (LLM) for energy technologies, we systematically gathered permitting information from nearly 300 state-, county-, and city-level documents, creating a structured dataset of requirements and procedures on an unprecedented scale and speed. Our analysis revealed that local (city and county) permitting requirement documents are underrepresented compared to state-level guidance documents, which can impede timely and cost-effective installation of new electric infrastructure. Our validation process showed that the final database has an accuracy of approximately 95%. We, further, created a new quantitative method to score permitting requirements for clarity and efficiency, with electric vehicle supply equipment as an initial use case. The average local permitting document scored a 1.8 out of 5, which we interpret as meaning that half of the requirements developers face when installing electric infrastructure are ambiguous, increasing both cost and time. We also created a “Generalized Permit Process”, highlighting common procedural steps and identifying specific opportunities for municipalities to improve their documentation. This research establishes a systematic and scalable framework for evaluating the complexities of local infrastructure permitting processes by combining LLM-powered data collection and quantitative scoring. The framework enables policymakers and developers to identify and mitigate procedural bottlenecks, with the expectation that these improvements can accelerate application review and approval, reduce project costs, and expedite connection to utility distribution grids. As a foundational approach for streamlining local project development processes, this study’s methods are intended to be extended to a wide range of energy applications.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗
DOE OSTI2019

Reciprocity between local moments and collective magnetic excitations in the phase diagram of BaFe 2 (As 1-x P x ) 2

Unconventional superconductivity arises at the border between the strong coupling regime with local magnetic moments and the weak coupling regime with itinerant electrons, and stems from the physics of criticality that dissects the two. Unveiling the nature of the quasiparticles close to quantum criticality is fundamental to understand the phase diagram of quantum materials. Here, using resonant inelastic x-ray scattering (RIXS) and Fe-K β emission spectroscopy (XES), we visualize the coexistence and evolution of local magnetic moments and collective spin excitations across the superconducting dome in isovalently-doped BaFe 2 (As 1-x P x ) 2 (0.00 ≤ x ≤0.52). Collective magnetic excitations resolved by RIXS are gradually hardened, whereas XES reveals a strong suppression of the local magnetic moment upon doping. This relationship is captured by an intermediate coupling theory, explicitly accounting for the partially localized and itinerant nature of the electrons in Fe pnictides. Finally, our work identifies a local-itinerant spin fluctuations channel through which the local moments transfer spin excitations to the particle-hole (paramagnons) continuum across the superconducting dome.

36 MATERIALS SCIENCE↗
DOE OSTI2011

Comment on 'Mapping of localized spin-wave excitations by near-field Brillouin light scattering' [Appl. Phys. Lett. 97, 152502 (2010)].

The authors reported in their letter some outstanding experimental results of spin excitations in nano-particles investigated by near-field Brillouin scattering. They conclude from their observations that existing theories -- in particular micromagnetic simulations -- do not correctly describe the behavior of the spin modes. Since excellent agreement has been reported between spin-wave mode frequencies obtained from Brillouin scattering experiments and those obtained from micromagnetic-based simulations, it is somewhat surprising that the simulations should fail for the particles investigated in Ref. 1. In the literature, there is also evidence of various kinds and degrees of mode localization when exchange competes with dipolar interactions. When dipolar long-range interactions are taken into account, the eigenmodes can be seen as the superposition of plane waves, leading to different localizations and in particular to the appearence of bulk-dead modes. We have simulated the normal modes of the particles used in Ref. 1, with the dynamical matrix method; the results are shown in Fig. 1 for different values of the applied field. In addition to the lowest frequency non-localized mode (1-BA), several localized modes are present. Large particles exhibit modes with oscillations along the field direction;8 for such modes, we use the label n-BA-loc, with n the number of nodes. While the profile of the pure end-mode, i.e., 0-BA-loc, has its maximum at the edge with the amplitude monotonously decreasing toward the interior of the ellipse, as correctly described by the authors, the localized modes with n > 0, not considered by them, do not have this characteristic: see inset of Fig. 1. Based on Fig. 1, we believe that the assumption that the mode they observe is 'the' localized spin mode is not correct. Instead, we believe that the mode detected in the experiment at H > 700 Oe is a combinations (due to non-linear excitation conditions of the experiment) of several n-BA-loc modes, with n?>?0. In this picture, the sharp peaks of the n-BA-loc modes are smoothed in the experimental measurements, thanks to the superposition of modes with different nodal lines. Finally, at 350 Oe, the measured profile and frequency suggest that the mode seen in the experiment may be well due to the 1-BA mode. The observed change in mode profile at 350 Oe is substantiated by the frequency behavior shown in Fig. 3(b) of Ref. 1, where it can be observed that the frequency of the low-field point does not lie on the same curve as the high-field points. In summary, before concluding that micromagnetic-based simulations of spin wave modes in nano-particles are unreliable, we believe that it is necessary to await either the simulation of large particles using small cell sizes or for more exhaustive experiments reaching lower frequencies on particles of varying size. The comparison of calculations with experiment would greatly benefit if the authors were to provide the field dependence of all the modes detected in their experiment (in order to achieve a proper assignment).

36 MATERIALS SCIENCE↗
DOE OSTI2014

Quantum transport through disordered 1D wires: Conductance via localized and delocalized electrons

Coherent electronic transport through disordered systems, like quantum wires, is a topic of fundamental and practical interest. In particular, the exponential localization of electron wave functions-Anderson localization-due to the presence of disorder has been widely studied. In fact, Anderson localization, is not an phenomenon exclusive to electrons but it has been observed in microwave and acoustic experiments, photonic materials, cold atoms, etc. Nowadays, many properties of electronic transport of quantum wires have been successfully described within a scaling approach to Anderson localization. On the other hand, anomalous localization or delocalization is, in relation to the Anderson problem, a less studied phenomenon. Although one can find signatures of anomalous localization in very different systems in nature. In the problem of electronic transport, a source of delocalization may come from symmetries present in the system and particular disorder configurations, like the so-called Lévy-type disorder. We have developed a theoretical model to describe the statistical properties of transport when electron wave functions are delocalized. In particular, we show that only two physical parameters determine the complete conductance distribution.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Local structure and polarization resistance of Ce doped SrMnO{sub 3} using extended x-ray fine structure analysis

Changes to the local structure of Sr and Mn atoms in Sr{sub 1−x}Ce{sub x}MnO{sub 3} (SCM) according to increasing Ce content and the effect of the structural change on the polarization resistance of SCM were investigated. The reduction of manganese was confirmed by the absorption edge shift of the Mn K-edge toward lower energies. The noise of oscillation in extended X-ray absorption fine structure k{sup 3}χ data at Mn K-edge reveals the distortion of the local structure of Mn atoms, and the peak that indicates the bonding length of Mn-O, Sr/Ce, and -Mn decreased with the addition of Ce content in Fourier transformations of the Mn K-edge. The distortion of the local structure at Mn atoms was affected by the reduced manganese ions having larger ionic radii than Mn{sup 4+}. Meanwhile, few distortions of local atomic structures of Sr atoms occurred, and the average nearest neighboring distances of Sr-O and Sr-Mn are ∼2.13 Å and ∼2.95 Å, respectively. The average bonding lengths of the Ce-O and Ce-Mn increased because the ionic radius of substituted Ce ion with 12 coordination number is smaller than that of Sr ion, which leads the reduction of Mn ions and the distortion of local structure at the substituted A-site. Therefore, we reasoned that the distortion of the local atomic structure at Mn atoms in MnO{sub 6} and Ce atoms in A-site is one of the causes for interrupting oxygen ion transfers as a geometric factor, which results in an increase in the polarization resistance of SCM within the Ce composition range from 10 mol. % to 30 mol. %.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Quantization of systems with temporally varying discretization. II. Local evolution moves

Several quantum gravity approaches and field theory on an evolving lattice involve a discretization changing dynamics generated by evolution moves. Local evolution moves in variational discrete systems (1) are a generalization of the Pachner evolution moves of simplicial gravity models, (2) update only a small subset of the dynamical data, (3) change the number of kinematical and physical degrees of freedom, and (4) generate a dynamical (or canonical) coarse graining or refining of the underlying discretization. To systematically explore such local moves and their implications in the quantum theory, this article suitably expands the quantum formalism for global evolution moves, constructed in Paper I [P. A. Höhn, “Quantization of systems with temporally varying discretization. I. Evolving Hilbert spaces,” J. Math. Phys. 55, 083508 (2014); e-print http://arxiv.org/abs/arXiv:1401.6062 [gr-qc]], by employing that global moves can be decomposed into sequences of local moves. This formalism is spelled out for systems with Euclidean configuration spaces. Various types of local moves, the different kinds of constraints generated by them, the constraint preservation, and possible divergences in resulting state sums are discussed. It is shown that non-trivial local coarse graining moves entail a non-unitary projection of (physical) Hilbert spaces and “fine grained” Dirac observables defined on them. Identities for undoing a local evolution move with its (time reversed) inverse are derived. Finally, the implications of these results for a Pachner move generated dynamics in simplicial quantum gravity models are commented on.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2014

Quantitative prediction of radio frequency induced local heating derived from measured magnetic field maps in magnetic resonance imaging: A phantom validation at 7 T

Electrical Properties Tomography (EPT) technique utilizes measurable radio frequency (RF) coil induced magnetic fields (B1 fields) in a Magnetic Resonance Imaging (MRI) system to quantitatively reconstruct the local electrical properties (EP) of biological tissues. Information derived from the same data set, e.g., complex numbers of B1 distribution towards electric field calculation, can be used to estimate, on a subject-specific basis, local Specific Absorption Rate (SAR). SAR plays a significant role in RF pulse design for high-field MRI applications, where maximum local tissue heating remains one of the most constraining limits. The purpose of the present work is to investigate the feasibility of such B1-based local SAR estimation, expanding on previously proposed EPT approaches. To this end, B1 calibration was obtained in a gelatin phantom at 7 T with a multi-channel transmit coil, under a particular multi-channel B1-shim setting (B1-shim I). Using this unique set of B1 calibration, local SAR distribution was subsequently predicted for B1-shim I, as well as for another B1-shim setting (B1-shim II), considering a specific set of parameter for a heating MRI protocol consisting of RF pulses plaid at 1% duty cycle. Local SAR results, which could not be directly measured with MRI, were subsequently converted into temperature change which in turn were validated against temperature changes measured by MRI Thermometry based on the proton chemical shift.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2014

Origin of radiative recombination and manifestations of localization effects in GaAs/GaNAs core/shell nanowires

Radiative carrier recombination processes in GaAs/GaNAs core/shell nanowires grown by molecular beam epitaxy on a Si substrate are systematically investigated by employing micro-photoluminescence (μ-PL) and μ-PL excitation (μ-PLE) measurements complemented by time-resolved PL spectroscopy. At low temperatures, alloy disorder is found to cause localization of photo-excited carriers leading to predominance of optical transitions from localized excitons (LE). Some of the local fluctuations in N composition are suggested to lead to strongly localized three-dimensional confining potential equivalent to that for quantum dots, based on the observation of sharp and discrete PL lines within the LE contour. The localization effects are found to have minor influence on PL spectra at room temperature due to thermal activation of the localized excitons to extended states. Under these conditions, photo-excited carrier lifetime is found to be governed by non-radiative recombination via surface states which is somewhat suppressed upon N incorporation.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2017

Segment-scale, force-level theory of mesoscopic dynamic localization and entropic elasticity in entangled chain polymer liquids

In this study, we develop a segment-scale, force-based theory for the breakdown of the unentangled Rouse model and subsequent emergence of isotropic mesoscopic localization and entropic elasticity in chain polymer liquids in the absence of ergodicity-restoring anisotropic reptation or activated hopping motion. The theory is formulated in terms of a conformational N-dynamic-order-parameter generalized Langevin equation approach. It is implemented using a universal field-theoretic Gaussian thread model of polymer structure and closed at the level of the chain dynamic second moment matrix. The physical idea is that the isotropic Rouse model fails due to the dynamical emergence, with increasing chain length, of time-persistent intermolecular contacts determined by the combined influence of local uncrossability, long range polymer connectivity, and a self-consistent treatment of chain motion and the dynamic forces that hinder it. For long chain melts, the mesoscopic localization length (identified as the tube diameter) and emergent entropic elasticity predictions are in near quantitative agreement with experiment. Moreover, the onset chain length scales with the semi-dilute crossover concentration with a realistic numerical prefactor. Distinctive novel predictions are made for various off-diagonal correlation functions that quantify the full spatial structure of the dynamically localized polymer conformation. As the local excluded volume constraint and/or intrachain bonding spring are softened to allow chain crossability, the tube diameter is predicted to swell until it reaches the radius-of-gyration at which point mesoscopic localization vanishes in a discontinuous manner. Finally, a dynamic phase diagram for such a delocalization transition is constructed, which is qualitatively consistent with simulations and the classical concept of a critical entanglement degree of polymerization.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

A density-based continuous local symmetry measure

Although continuous symmetry theory has attracted increasing attention in modern chemistry, local symmetry remains under-investigated. As a consequence, the relationship between symmetry and chemical behavior is often obscured, limiting the practical use of fuzzy symmetry measures. Here, in this study, we introduce a novel framework for evaluating local symmetry based on electron density localization and present continuous symmetry representations for several representative molecules. Our approach not only quantitatively captures global symmetry but also reveals distinctive features of symmetry in a local chemical environment. The related concept, local chirality or chirotopicity, is also discussed. Overall, the proposed local symmetry and chirality measures provide valuable insights into molecular structure and structure–property relationships.

Lai, Duc Anh [Southern Methodist Univ., Dallas, TX↗