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At least 451 records · Page 25

Estimates of tropical analysis differences in daily values produced by two operational centers

To assess the uncertainty of daily synoptic analyses for the atmospheric state, the intercomparison of three First GARP Global Experiment level IIIb datasets is performed. Daily values of divergence, vorticity, temperature, static stability, vertical motion, mixing ratio, and diagnosed diabatic heating rate are compared for the period of 26 January-11 February 1979. The spatial variance and mean, temporal mean and variance, 2D wavenumber power spectrum, anomaly correlation, and normalized square difference are employed for comparison.

Kasahara, Akira↗

Long-Lag, Wide-pulse Gamma-Ray Bursts

Currently, the best available probe of the early phase of gamma-ray burst (GRB) jet attributes is the prompt gamma-ray emission, in which several intrinsic and extrinsic variables determine GRB pulse evolution. Bright, usually complex bursts have many narrow pulses that are difficult to model due to overlap. However, the relatively simple, long spectral lag, wide-pulse bursts may have simpler physics and are easier to model. In this work we analyze the temporal and spectral behavior of wide pulses in 24 long-lag bursts, using a pulse model with two shape parameters - width and asymmetry - and the Band spectral model with three shape parameters. We find that pulses in long-lag bursts are distinguished both temporally and spectrally from those in bright bursts: the pulses in long spectral lag bursts are few in number, and approximately 100 times wider (10s of seconds), have systematically lower peaks in vF(v), harder low-energy spectra and softer high-energy spectra. We find that these five pulse descriptors are essentially uncorrelated for our long-lag sample, suggesting that at least approximately 5 parameters are needed to model burst temporal and spectral behavior. However, pulse width is strongly correlated with spectral lag; hence these two parameters may be viewed as mutual surrogates. We infer that accurate formulations for estimating GRB luminosity and total energy will depend on several gamma-ray attributes, at least for long-lag bursts. The prevalence of long-lag bursts near the BATSE trigger threshold, their predominantly low vF(v) spectral peaks, and relatively steep upper power-law spectral indices indicate that Swift will detect many such bursts.

Norris, J. P.↗

Glyoxal Yield from Isoprene Oxidation and Relation to Formaldehyde: Chemical Mechanism, Constraints from SENEX Aircraft Observations, and Interpretation of OMI Satellite Data

Glyoxal (CHOCHO) is produced in the atmosphere by the oxidation of volatile organic compounds(VOCs). Like formaldehyde (HCHO), another VOC oxidation product, it is measurable from space by solar backscatter. Isoprene emitted by vegetation is the dominant source of CHOCHO and HCHO in most of the world. We use aircraft observations of CHOCHO and HCHO from the Southeast Nexus (SENEX) campaign over the southeast US in summer 2013 to better understand the CHOCHO time-dependent yield from isoprene oxidation, its dependence on nitrogen oxides (NO (sub x) triple bonded to NO plus NO2), the behavior of the CHOCHO-HCHO relationship, the quality of Ozone Monitoring Instrument (OMI) CHOCHO satellite observations, and the implications for using CHOCHO observations from space as constraints on isoprene emissions. We simulate the SENEX and OMI observations with the Goddard Earth Observing System chemical transport model (GEOSChem) featuring a new chemical mechanism for CHOCHO formation from isoprene. The mechanism includes prompt CHOCHO formation under low-NO (sub x) conditions following the isomerization of the isoprene peroxy radical (ISOPO2).The SENEX observations provide support for this prompt CHOCHO formation pathway, and are generally consistent with the GEOS-Chem mechanism. Boundary layer CHOCHO and HCHO are strongly correlated in the observations and the model, with some departure under low-NO (sub x) conditions due to prompt CHOCHO formation. SENEX vertical profiles indicate a free-tropospheric CHOCHO background that is absent from the model. The OMI CHOCHO data provide some support for this free-tropospheric background and show southeast US enhancements consistent with the isoprene source but a factor of 2 too low. Part of this OMI bias is due to excessive surface reflectivities assumed in the retrieval. The OMI CHOCHO and HCHO seasonal data over the southeast US are tightly correlated and provide redundant proxies of isoprene emissions. Higher temporal resolution in future geostationary satellite observations may enable detection of the prompt CHOCHO production under low-NO (sub x) conditions apparent in the SENEX data.

OMI↗

BEYONDPLANCK VI. Noise characterization and modeling

We present a Bayesian method for estimating instrumental noise parameters and propagating noise uncertainties within the global BeyondPlanck Gibbs sampling framework, and apply this to Planck Low Frequency Instrument (LFI) time-ordered data. Following previous literature, we initially adopt a 1/ f model for the noise power spectral density (PSD), but find the need for an additional lognormal component in the noise model for the 30 and 44 GHz bands. We implement an optimal Wiener-filter (or constrained realization) gap-filling procedure to account for masked data. We then use this procedure to both estimate the gapless correlated noise in the time-domain, n corr , and to sample the noise PSD parameters, ξ n = {σ 0 , f knee , α, A p }. In contrast to previous Planck analyses, we assume piecewise stationary noise only within each pointing period (PID), not throughout the full mission, but we adopt the LFI Data Processing Center (DPC) results as priors on α and f knee . On average, we find best-fit correlated noise parameters that are mostly consistent with previous results, with a few notable exceptions. However, a detailed inspection of the time-dependent results reveals many important findings. First and foremost, we find strong evidence for statistically significant temporal variations in all noise PSD parameters, many of which are directly correlated with satellite housekeeping data. Second, while the simple 1/ f model appears to be an excellent fit for the LFI 70 GHz channel, there is evidence for additional correlated noise not described by a 1/ f model in the 30 and 44 GHz channels, including within the primary science frequency range of 0.1–1 Hz. In general, most 30 and 44 GHz channels exhibit deviations from 1/ f at the 2–3σ level in each one hour pointing period, motivating the addition of the lognormal noise component for these bands. For some periods of time, we also find evidence of strong common mode noise fluctuations across the entire focal plane. Overall, we conclude that a simple 1/ f profile is not adequate to fully characterize the Planck LFI noise, even when fitted hour-by-hour, and a more general model is required. These findings have important implications for large-scale CMB polarization reconstruction with the Planck LFI data, and the current work is a first attempt at understanding and mitigating these issues.

79 ASTRONOMY AND ASTROPHYSICS↗

Analysis of scintillation light dependence on Liquid Argon purity in the ICARUS detector

Previous studies have investigated the correlation between impurities concentration in Liquid Argon (LAr) and the temporal evolution of either the slow scintillation decay time or the light yield.These impurities typically consist of various molecular species. Electronegative contaminants directly affect electron drift and photon production, while other molecules, such as nitrogen (N$_{2}$), can influence LAr scintillation properties without necessarily affecting electron lifetime.Many current and future neutrino and dark-matter experiments use LAr detectors. This study aims to evaluate the measured electron lifetime in relation to the timing characteristics of the scintillation light signal in the SBN ICARUS detector at Fermi National Accelerator Laboratory. The ICARUS detector consists of two cryostats that have shown different behaviors in the measured electron lifetime over the years. In particular, this study addresses the use of data collected under varying purity conditions in the two cryostats and presents the methodology used to extract scintillation timing characteristics and their correlation with LAr purity.

Saia, C. [Catania Astrophys. Observ.] (ORCID:00090↗

Investigation of oscillations above the acoustic cut-off frequency for a sample of Kepler stars. II. Identifying temporal frequency shifts

ABSTRACT Stellar oscillations with frequencies greater than the acoustic cut-off frequency are not trapped within the star’s interior. Geometric interference between these high-frequency waves produces a peak-like structure in the power spectrum of the star, known as the pseudo-modes. In this study, we aim to analyse 51 stars previously identified (from a sample of 91 Kepler stars) to contain statistically significant evidence for pseudo-modes, to determine if the pseudo-mode frequencies vary in time. We obtained these frequency variations and the uncertainty by the resampled periodogram approach, where periodogram realisations were created from successive, overlapping 90-d time segments, and a cross-correlation function was generated between them. The computed shifts were compared against temporal p-mode frequency shifts and a stellar magnetic activity proxy, $S_{\mathrm{ph}}$. We found that for 16 per cent of the stars pseudo-mode frequency shifts were significantly anticorrelated with p-mode shifts, as is the case for the Sun. However, we also found pseudo-mode and p-mode shifts to be significantly correlated in-phase in 8 per cent of our sample. The remainder showed no significant correlation. We also searched for trends between the maximum variation of pseudo-mode frequency shifts and stellar parameters. Whilst we found no correlation between the maximum variation and stellar photospheric and chromospheric proxies, we found frequency variations to have a greater amplitude for cooler and slower rotating stars, which is in opposition to p-mode frequency shift variation. Temporal changes to pseudo-mode frequencies may be attributable to variations in stellar magnetic activity, and therefore can contribute to our understanding of stellar activity cycles.

Millson, L. J. (ORCID:0009000342542676)↗

Kankakee Water Resources: Monitoring Temperature and Vegetation to Detect River Flow Impediments at Energy Intake Structures

In recent years, unpredictable grassing events have occurred at the Dresden Generating Station, located on the Kankakee River in northern Illinois. Grassing events are characterized by large mats of aquatic vegetation that accumulate downstream, resulting in the clogging of water intake structures and leading to major disruptions in power generation. Currently, employees at the Dresden Generating Station are responsible for reactively responding to each grassing event individually. This project, in partnership with Constellation Nuclear and the United States Geological Survey (USGS), assessed the feasibility of using Earth observations (Landsat 9 OLI-2, Landsat 8 OLI, Sentinel-2 MSI, DOVE PlanetScope, WorldView-3, and GPM IMERG) to detect floating aquatic vegetation within the Kankakee River and identify predictive factors that trigger grassing events, as doing so will provide the Dresden Generating Station the ability to anticipate future grassing events and enhance general hydrologic modeling efforts held by the USGS. The results of this study illustrated that, while aquatic vegetation can be detected by satellites with up to moderate spatial resolution (30 m), temporal resolution is a major limiting factor for tracking movements in floating aquatic vegetation and identifying predictive measures for these events. In addition, correlation results suggest a possible negative relationship between grassing events and river discharge (-0.875 correlation coefficient). In the future, pairing these results with ground control surveys and sensors with higher temporal capabilities would allow our project partners to predict and proactively address future grassing events, ensuring the reliable operation of the Dresden Generating Station.

Marisa Smedsrud↗

Multiwavelength Observations of a Dramatic High-Energy Flare in the Blazar 3C 279

The blazar 3C 279, one of the brightest identified extragalactic objects in the gamma-ray sky, underwent a large (factor of approximately 10 in amplitude) flare in gamma-rays toward the end of a 3 week pointing by Compton Gamma Ray Observatory (CGRO), in 1996 January-February. The flare peak represents the highest gamma-ray intensity ever recorded for this object. During the high state, extremely rapid gamma-ray variability was seen, including an increase of a factor of 2.6 in approximately 8 hr, which strengthens the case for relativistic beaming. Coordinated multifrequency observations were carried out with Rossi X-Ray Timing Explorer (RXTE), Advanced Satellite for Cosmology and Astrophysics (ASCA; or, Astro-D), Roentgen Satellite (ROSAT), and International Ultraviolet Explorer (IUE) and from many ground-based observatories, covering most accessible wavelengths. The well-sampled, simultaneous RXTE light curve shows an outburst of lower amplitude (factor of approximately = 3) well correlated with the gamma-ray flare without any lag larger than the temporal resolution of approximately 1 day. The optical-UV light curves, which are not well sampled during the high-energy flare, exhibit more modest variations (factor of approximately 2) and a lower degree of correlation. The flux at millimetric wavelengths was near a historical maximum during the gamma-ray flare peak, and there is a suggestion of a correlated decay. We present simultaneous spectral energy distributions of 3C 279 prior to and near to the flare peak. The gamma-rays vary by more than the square of the observed IR-optical flux change, which poses some problems for specific blazar emission models. The synchrotron self-Compton (SSC) model would require that the largest synchrotron variability occurred in the mostly unobserved submillimeter/far-infrared region. Alternatively, a large variation in the external photon field could occur over a time-scale of a few days. This occurs naturally in the "mirror" model wherein the flaring region in the jet photoionizes nearby broad emission line clouds, which, in turn, provide soft external photons that are Comptonized to gamma-ray energies.

Wehrle, A. E.↗

Multiwavelength Observations of a Dramatic High-Energy Flare in the Blazar 3C 279

The blazar 3C 279, one of the brightest identified extragalactic objects in the gamma-ray sky, underwent a large (factor of approx. 10 in amplitude) flare in gamma-rays toward the end of a 3 week pointing by Compton Gamma Ray Observatory (CGRO), in 1996 January-February. The flare peak represents the highest gamma-ray intensity ever recorded for this object. During the high state, extremely rapid gamma-ray variability was seen, including an increase of a factor of 2.6 in approx. 8 hrs., which strengthens the case for relativistic beaming. Coordinated multifrequency observations were carried out with Rossi X-Ray Timing Explorer (RXTE), Advanced Satellite for Cosmology and Astrophysics (ASCA; or, Astro-D), Roentgen Satellite (ROSAT), and International Ultraviolet Explorer (IUE) and from many ground-based observatories, covering most accessible wavelengths. The well-sampled, simultaneous RXTE light curve shows an outburst of lower amplitude (factor of approx. or equal to 3) well correlated with the gamma-ray flare without any lag larger than the temporal resolution of approx. 1 day. The optical-UV light curves, which are not well sampled during the high-energy flare, exhibit more modest variations (factor of approx. 2) and a lower degree of correlation. The flux at millimetric wavelengths was near a historical maximum during the gamma-ray flare peak, and there is a suggestion of a correlated decay. We present simultaneous spectral energy distributions of 3C 279 prior to and near to the flare peak. The gamma-rays vary by more than the square of the observed IR-optical flux change, which poses some problems for specific blazar emission models. The synchrotron self-Compton (SSC) model would require that the largest synchrotron variability occurred in the mostly unobserved submillimeter/far-infrared region. Alternatively, a large variation in the external photon field could occur over a time scale of a few days. This occurs naturally in the "mirror" model wherein the flaring region in the jet photoionizes nearby broad emission line clouds, which, in turn, provide soft external photons that are Comptonized to gamma-ray energies.

Wehrle, A. E.↗

Phase Transition Dynamics in a Complex Oxide Heterostructure

Understanding the behavior of defects in the complex oxides is key to controlling myriad ionic and electronic properties in these multifunctional materials. The observation of defect dynamics, however, requires a unique probe-one sensitive to the configuration of defects as well as its time evolution. Here, we present measurements of oxygen vacancy ordering in epitaxial thin films of SrCoO x and the brownmillerite-perovskite phase transition employing x-ray photon correlation spectroscopy. These and associated synchrotron measurements and theory calculations reveal the close interaction between the kinetics and the dynamics of the phase transition, showing how spatial and temporal fluctuations of heterointerface evolve during the transformation process. The energetics of the transition are correlated with the behavior of oxygen vacancies, and the dimensionality of the transformation is shown to depend strongly on whether the phase is undergoing oxidation or reduction. Finally, the experimental and theoretical methods described here are broadly applicable to in situ measurements of dynamic phase behavior and demonstrate how coherence may be employed for novel studies of the complex oxides as enabled by the arrival of fourth-generation hard x-ray coherent light sources.

36 MATERIALS SCIENCE↗

Coincident Occurrences of Tropical Individual Cirrus Clouds and Deep Convective Systems Derived from TRMM Observations

Measurements of cloud properties and atmospheric radiation taken between January and August 1998 by the Tropical Rainfall Measuring Mission (TRMM) satellite were used to investigate the effect of spatial and temporal scales on the coincident occurrences of tropical individual cirrus clouds (ICCs) and deep convective systems (DCSs). It is found that there is little or even negative correlation between instantaneous occurrences of ICC and DCS in small areas, in which both types of clouds cannot grow and expand simultaneously. When spatial and temporal domains are increased, ICCs become more dependent on DCSs due to the origination of many ICCs from DCSs and moisture supply from the DCS in the upper troposphere for the ICCs to grow, resulting in significant positive correlation between the two types of tropical high clouds in large spatial and long temporal scales. This result may suggest that the decrease of tropical high clouds with SST from model simulations is likely caused by restricted spatial domains and limited temporal periods. Finally, the radiative feedback due to the change in tropical high cloud area coverage with sea surface temperature appears small and about -0.14 W/sq m per degree Kelvin.

Lin, Bing↗

Spatial and temporal variability of infrared-observable properties of the Jovian atmosphere: A partial survey

Examination of infrared characteristics of the Jovian atmosphere are made using Voyager IRIS mapping from 1979, groud based scanning from 1979-1983, and ground based mapping from 1983 to the present. In general, there is a strong correlation between tropospheric thermal properties and the visual cloud albedo for all observations. The Voyager IRIS maps show no strong evidence for day/night differences. Temperature differences diminish with depth in the troposphere. Temporal changes over several weeks indicate a high correlation between thermal and visual properties, although no changes in the distribution of para H2 and ortho H2 are seen. Stratospheric banded organization is different from the troposphere, and there is a temperature enhancement near the north magnetic pole. The spatial distributions of ammonia gas and ammonia ice absorption are different. Stratospheric temperatures exhibit seasonal hemispheric asymmetry. Other temperature changes at and below the 150-mb level correlate with changes in the Jovian visual structure. The stratospheric temperature field is uncorrelated with visual features or temperatures below the 150-mb level. Elevated temperatures are observed near both north and south magnetic pole positions. Both the meridional positions and the relative intensities of stratospheric banded organization change significantly, especially after 1982. Ground based mapping confirms a correlation between temperatures and various measures of cloud distribution. Complex and unexpected characteristics are observed in the stratospheric temperature field; these include dramatic temporal changes on short time scales.

Orton, Glenn S.↗

Probing the γ -Ray Emission Origin of Two Star-forming Galaxies NGC 2403 and NGC 3424 with the Fermi-LAT

Star-forming galaxies (SFGs) are a subclass of γ-ray emitters, and a correlation between their γ-ray luminosity (L γ ) and the total infrared (IR) luminosity (L IR ) has been established based on the Fermi Large Area Telescope (LAT) data. NGC 2403 and NGC 3424 have been reported as outliers in the L γ –L IR correlation with light curves showing significant variability, which contrasts with the temporally stable γ-ray emission in other SFGs, originating primarily from cosmic rays interacting with interstellar medium. In this study, we reanalyze the γ-ray emission in the directions of NGC 2403 and NGC 3424 using more than 16.5 yr Fermi-LAT data. NGC 3424 is found to be spatially coincident with the detected γ-ray source, while NGC 2403 is significantly offset from the nearest γ-ray source, suggesting an implausible association. We confirm the previously reported variability of both γ-ray sources and the significant deviation from the L γ –L IR correlation when assuming an association of both γ-ray sources with the two galaxies. Our findings lend further support to the interpretation that their γ-ray emission is driven primarily by alternative radiative processes—rather than by star formation activity—such as the ejecta of the Type IIP supernova SN 2004dj in NGC 2403 interacting with a surrounding high-density shell and an obscured active galactic nucleus in NGC 3424.

Liu, Linjie [Chinese Academy of Sciences (CAS), Ku↗

Earth Science Data Analytics: Preparing for Extracting Knowledge from Information

Data analytics is the process of examining large amounts of data of a variety of types to uncover hidden patterns, unknown correlations and other useful information. Data analytics is a broad term that includes data analysis, as well as an understanding of the cognitive processes an analyst uses to understand problems and explore data in meaningful ways. Analytics also include data extraction, transformation, and reduction, utilizing specific tools, techniques, and methods. Turning to data science, definitions of data science sound very similar to those of data analytics (which leads to a lot of the confusion between the two). But the skills needed for both, co-analyzing large amounts of heterogeneous data, understanding and utilizing relevant tools and techniques, and subject matter expertise, although similar, serve different purposes. Data Analytics takes on a practitioners approach to applying expertise and skills to solve issues and gain subject knowledge. Data Science, is more theoretical (research in itself) in nature, providing strategic actionable insights and new innovative methodologies. Earth Science Data Analytics (ESDA) is the process of examining, preparing, reducing, and analyzing large amounts of spatial (multi-dimensional), temporal, or spectral data using a variety of data types to uncover patterns, correlations and other information, to better understand our Earth. The large variety of datasets (temporal spatial differences, data types, formats, etc.) invite the need for data analytics skills that understand the science domain, and data preparation, reduction, and analysis techniques, from a practitioners point of view. The application of these skills to ESDA is the focus of this presentation. The Earth Science Information Partners (ESIP) Federation Earth Science Data Analytics (ESDA) Cluster was created in recognition of the practical need to facilitate the co-analysis of large amounts of data and information for Earth science. Thus, from a to advance science point of view: On the continuum of ever evolving data management systems, we need to understand and develop ways that allow for the variety of data relationships to be examined, and information to be manipulated, such that knowledge can be enhanced, to facilitate science. Recognizing the importance and potential impacts of the unlimited ways to co-analyze heterogeneous datasets, now and especially in the future, one of the objectives of the ESDA cluster is to facilitate the preparation of individuals to understand and apply needed skills to Earth science data analytics. Pinpointing and communicating the needed skills and expertise is new, and not easy. Information technology is just beginning to provide the tools for advancing the analysis of heterogeneous datasets in a big way, thus, providing opportunity to discover unobvious scientific relationships, previously invisible to the science eye. And it is not easy It takes individuals, or teams of individuals, with just the right combination of skills to understand the data and develop the methods to glean knowledge out of data and information. In addition, whereas definitions of data science and big data are (more or less) available (summarized in Reference 5), Earth science data analytics is virtually ignored in the literature, (barring a few excellent sources).

data analytics↗

Lifetime-resolved photon-correlation Fourier spectroscopy

The excited state population of single solid-state emitters is subjected to energy fluctuations around the equilibrium driven by the bath and relaxation through the emission of phonons or photons. Simultaneous measurement of the associated spectral dynamics requires a technique with a high spectral and temporal resolution with an additionally high temporal dynamic range. We propose a pulsed excitation-laser analog of photon-correlation Fourier spectroscopy (PCFS), which extracts the linewidth and spectral diffusion dynamics along the emission lifetime trajectory of the emitter, effectively discriminating spectral dynamics from relaxation and bath fluctuations . This lifetime-resolved PCFS correlates photon-pairs at the output arm of a Michelson interferometer in both their time-delay between laser-excitation and photon-detection T and the time-delay between two photons τ . We propose the utility of the technique for systems with changing relative contributions to the emission from multiple states, for example, quantum emitters exhibiting phonon-mediated exchange between different fine-structure states.

36 MATERIALS SCIENCE↗

Observations of stratospheric temperature changes coincident with the recent Antarctic ozone depletions

A high degree of correlation between the recent decline in Antarctic total ozone and cooling of the stratosphere during Austral spring has been noted in several recent studies (e.g., Sekiguchi, 1986; Angel, 1986). This study analyzes the observed temperature trends in detail, focusing on the spatial and temporal aspects of the observed cooling. Ozone losses and stratospheric cooling can be correlated for several reasons: (1) ozone losses (from an unspecified cause) will directly reduce temperatures due to decreased solar ultraviolet absorption (Shine, 1986), and/or (2) changes in both ozone and temperature structure due to modification of stratospheric circulation patterns (Mahlman and Fels, 1986). In order to scrutinize various ozone depletion scenarios, detailed information on the observed temperature changes is necessary; the goal is to provide such data. The data used are National Meteorological Center (NMC) Climate Analysis Center (CAC) derived temperatures, covering 1000 to 1 mb (0 to 48 km), for the period 1979 to 1987. Discussions on data origin and quality (assessed by extensive comparisons with radiosonde observations), along with other details of these observations, can be found in Newman and Randel (1988).

Randel, William J.↗

Tau accumulation and atrophy predict amyloid independent cognitive decline in aging

INTRODUCTION: Amyloid beta (Aβ) and tau pathology are cross-sectionally associated with atrophy and cognitive decline in aging and Alzheimer's disease (AD). METHODS: We investigated relationships between concurrent longitudinal measures of Aβ (Pittsburgh compound B [PiB] positron emission tomography [PET]), tau (flortaucipir [FTP] PET), atrophy (structural magnetic resonance imaging), episodic memory (EM), and non-memory (NM) in 78 cognitively healthy older adults (OA). RESULTS: Entorhinal FTP change was correlated with EM decline regardless of Aβ, but meta-temporal FTP and global PiB change were only associated with EM and NM decline in Aβ+ OA. Voxel-wise analyses revealed significant associations between temporal lobe FTP change and EM decline in all groups. PiB and FTP change were not associated with structural change, suggesting a functional or microstructural mechanism linking these measures to cognitive decline. DISCUSSION: Our results show that longitudinal Aβ is linked to cognitive decline only in the presence of elevated Aβ, but longitudinal temporal lobe tau is associated with memory decline regardless of Aβ status.

60 APPLIED LIFE SCIENCES↗

Dynamic Nanoscale Spatial Heterogeneity in a Perovskite-to-Brownmillerite Topotactic Phase Transformation

Phase transitions are omnipresent in modern condensed matter physics and its applications. In solids, first-order phase transformations typically occur by nucleation and growth under nonequilibrium conditions. Under constant external conditions, e.g., constant annealing temperature and pressure, the nucleation and growth dynamics are often thought of as spatially and temporally independent. Here, in situ Bragg X-ray photon correlation spectroscopy (XPCS) reveals nanoscale spatial and dynamical heterogeneity in the perovskite-to-brownmillerite topotactic phase transformation in La 0.7 Sr 0.3 CoO 3 thin films annealed under constant reducing conditions over a time span of multiple hours. Specifically, a time scale associated with domain growth remains stable, with a corresponding domain wall speed of v d = 6 ± 0.5 × 10 –4 nm/s (2 ± 0.2 nm/h), while a slower time scale, associated with temperature-driven depinning of domains, leads to accelerating dynamics with time scales following an aging power law with exponent −2.2 ± 0.5. This experiment demonstrates that Bragg XPCS is a powerful tool to study nanoscale dynamics in structural phase transformations, with the ability to extract quantitative average values related to nanodomain motion in situ. Furthermore, the results are relevant for phase engineering of phase-change devices, as they show that nanoscale dynamics, linked to domain and domain-wall motion, can continuously evolve and speed up with time, even hours after the initiation of the phase transformation, with potential repercussions on electrical performance.

X-ray photon correlation spectroscopy↗