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Influence of Longer Range Transfer of Vapor Interface Modified Caging Constraints on the Spatially Heterogeneous Dynamics of Glass-Forming Liquids
Based on the elastically collective nonlinear Langevin equation (ECNLE) theory of bulk relaxation in glass-forming liquids, and our recent ideas of how interface-nucleated modification of caging constraints are spatially transferred into the interior of a thick film, we present a force-based theory for dynamical gradients in thick films with one vapor interface that includes collective elasticity effects. Quantitative applications to the foundational hard sphere fluid and polymer melts of diverse fragilities are presented. In this work, we predict a roughly exponential spatial variation of the total activation barrier which is nonperturbatively modified to similar to 10 particle diameters into the film. This leads, to leading order, to the prediction of a reduced alpha relaxation time gradient of a double-exponential form characterized by a nearly constant spatial decay length, in qualitative accord with simulations. The relaxation acceleration at the surface grows exponentially with increasing packing fraction or decreasing temperature. The rate of increase with cooling of the alpha time strongly weakens upon approaching the vapor interface, with the top two layers remaining liquid-like down to similar to ~80-85% of the bulk glass transition temperature. These spatially heterogeneous changes of the temperature variation of the alpha time result in a large and long-range gradient of the local glass transition temperature. An average interfacial layer thickness relevant to ensemble-averaged dielectric and other experiments is also computed. It is predicted to be rather large at the bulk glass transition temperature, decreasing roughly linearly with heating. Remarkably, to leading order the ratio of this layer-averaged interfacial relaxation time to its bulk analogue is invariant to chemistry, volume fraction, and temperature and of modest absolute magnitude. Spatially inhomogeneous power law decoupling of the alpha relaxation time from its bulk value is predicted, with an effective exponent that decays to zero with distance from the free surface in a nearly exponential manner, trends which are in qualitative accord with recent simulations. Finally, this behavior and the double-exponential alpha time gradient are related and can be viewed as consequences of an effective quasi-universal factorization of the total barrier in films into the product of its bulk-temperature-dependent value times a function solely of location in the film.
A Potent d -Protein Antagonist of VEGF-A is Nonimmunogenic, Metabolically Stable, and Longer-Circulating in Vivo
Not Available
Protein Electric Fields Enable Faster and Longer-Lasting Covalent Inhibition of β-Lactamases
The widespread design of covalent drugs has focused on crafting reactive groups of proper electrophilicity and positioning towards targeted amino-acid nucleophiles. In this work, we found that environmental electric fields projected onto a reactive chemical bond, an overlooked design element, play essential roles in the covalent inhibition of TEM-1 beta-lactamase by avibactam. Using the vibrational Stark effect, the magnitudes of the electric fields that are exerted by TEM active sites onto avibactam’s reactive C=O were measured and demonstrate an electrostatic gating effect that promotes bond formation yet relatively suppresses the reverse dissociation. These results suggest new principles of covalent drug design and off-target site prediction. Unlike shape and electrostatic complementary which address binding constants, electrostatic catalysis drives reaction rates, essential for covalent inhibition, and deepens our understanding of chemical reactivity, selectivity, and stability in complex systems.
Comment on “Five Decades of Observed Daily Precipitation Reveal Longer and More Variable Drought Events Across Much of the Western United States”
Abstract Changes in precipitation patterns with climate change could have important impacts on human and natural systems. Zhang et al. (2021, https://doi.org/10.1029/2020gl092293 ) report trends in daily precipitation patterns over the last five decades in the western United States, focusing on meteorological drought. They report that dry intervals (calculated at the annual or seasonal level) have increased across much of the southwestern U.S., with statistical assessment suggesting the results are statistically robust. However, Zhang et al. (2021, https://doi.org/10.1029/2020gl092293 ) preprocess their annual (or seasonal) averages to compute 5‐year moving window averages before using established statistical techniques for trend analysis that assume independence about some fixed trend. Here we show that the moving window preprocessing violates that independence assumption and inflates the statistical significance of their trend estimates. This raises questions about the robustness of their results. We conclude by discussing the difficulty of adjusting for spatial structure when assessing time trends in a regional context.
Arctic cyclones have become more intense and longer-lived over the past seven decades
Intense cyclones driving extreme Arctic weather and climate events have been more frequently observed during recent years, causing dramatic environmental and socioeconomic impacts. However, inconsistencies have emerged about long-term changes in Arctic cyclone activity. Here we analyze multiple reanalysis datasets covering a multidecadal period with improvements to the cyclone tracking algorithm and the integrated cyclone activity metric. The results indicate an intensification of Arctic cyclone activity over the last seven decades. There has been a long-term shift of the maximum cyclone counts from weaker to stronger cyclones and a pronounced lengthening of the duration of strong cyclones. Spatial analysis shows increased strong cyclone frequency over the Arctic, driven by enhanced lower troposphere baroclinicity, amplified winter jet stream waves over the subpolar North Atlantic, and a strengthened summer tropospheric vortex over the central Arctic. The stratospheric vortex has also intensified the tropospheric waves and vortex with distinct dynamics between winter and summer. Recently enhanced baroclinicity over large areas of the Arctic and midlatitudes suggests more complicated atmospheric dynamics than what is hypothesized with Arctic-amplification-induced decrease in meridional temperature gradients.
Fundamental difference of subpicosecond laser interaction compared to longer pulses for ultrahigh acceleration
Interaction of picosecond laser pulses above terawatt power with high density plasmas shows a nearly 100% conversion of the laser energy into directed acceleration of the electron cloud by nonlinear (ponderomotive) forces giving the ion cloud accelerations several orders of magnitude higher than comparable nanosecond interaction based on thermal pressure processes.
Longer than 1.9 μm photoluminescence emission from InAs quantum structure on GaAs (001) substrate
We report on photoluminescence (PL) emission with long wavelength for quantum structure by the sub-monolayer (SML) growth technique on GaAs (001) substrate. It is found that the PL emission wavelength can be controlled by controlling the SML InAs deposition amount. At 12 K, the PL peak position of the grown samples changes from about 1.66 to 1.78 μm. At 120 K, the PL emission of a sample reaches 1.91 μm. The physical mechanism responsible for the measured long wavelength PL emission may be related to strong In segregation and intermixing effects occurred in the structure grown by SML growth technique.
Beyond H {sub 0} and q {sub 0}: Cosmology is no longer just two numbers
For decades, H {sub 0} and q {sub 0} were the quest of cosmology, as they promised to characterize our 'world model' without reference to a specific cosmological framework. Using Monte Carlo simulations, we show that q {sub 0} cannot be directly measured using distance indicators with both accuracy (without offset away from its true value) and precision (small error bar). While H {sub 0} can be measured with accuracy and precision, to avoid a small bias in its direct measurement (of order 5%) we demonstrate that the pair H {sub 0} and Ω {sub M} (assuming flatness and w = –1) is a better choice of two parameters, even if our world model is not precisely ΛCDM. We illustrate this with analysis of the Constitution set of supernovae and indirectly infer q {sub 0} = –0.57 ± –0.04. Finally, we show that it may be possible to directly determine q {sub 0} with both accuracy and precision using the time dependence of redshifts ('redshift drift').
The typecasting of active galactic nuclei: Mrk 590 no longer fits the role
We present multiwavelength observations that trace more than 40 yr in the life of the active galactic nucleus (AGN) in Mrk 590, traditionally known as a classic Seyfert 1 galaxy. From spectra recently obtained from Hubble Space Telescope, Chandra, and the Large Binocular Telescope, we find that the activity in the nucleus of Mrk 590 has diminished so significantly that the continuum luminosity is a factor of 100 lower than the peak luminosity probed by our long-baseline observations. Furthermore, the broad emission lines, once prominent in the UV/optical spectrum, have all but disappeared. Since AGN type is defined by the presence of broad emission lines in the optical spectrum, our observations demonstrate that Mrk 590 has now become a 'changing-look' AGN. If classified by recent optical spectra, Mrk 590 would be a Seyfert ∼1.9–2, where the only broad emission line still visible in the optical spectrum is a weak component of Hα. As an additional consequence of this change, we have definitively detected UV narrow-line components in a Type 1 AGN, allowing an analysis of these emission-line components with high-resolution COS spectra. These observations challenge the historical paradigm that AGN type is only a consequence of the line-of-sight viewing angle toward the nucleus in the presence of a geometrically flattened, obscuring medium (i.e., the torus). Our data instead suggest that the current state of Mrk 590 is a consequence of the change in luminosity, which implies the black hole accretion rate has significantly decreased.
Longer thaw seasons increase nitrogen availability for leaching during fall in tundra soils
Not Available
Recovery of a Luther-Emery phase in the three-band Hubbard ladder with longer-range hopping
Not Available
Majorana zero modes in a quantum Ising chain with longer-ranged interactions
Not Available
The effect of longer-range waviness on X-ray reflectivity measurements
A model for calculating the X-ray reflectivity (XRR) of surfaces to extract both roughness and waviness features is presented. Expressions of reflectivity intensity are derived as a function of root-mean-square (RMS) roughness σ, RMS waviness σ L , and the cut-off frequency between the features ω 0 . Experiments were conducted at the Advanced Light Source at Lawrence Berkeley National Laboratory, beamline 8.3.2, on BK7 glass manufactured with a multi-step polishing process to validate the model, and were compared with atomic force microscopy (AFM), Fizeau interferometry and surface profilometry measurements. Here, the parameter results and their deviations for XRR measurements were σ = 2.9 ± 0.2 nm and σ L = 14.6 ± 0.5 nm with a wavelength cut-off of 1/(18 ± 2) µm –1 , while the results from the AFM, Fizeau and profilometry measurements were σ AFM = 3.4 ± 0.4 nm, σ L,Fizeau = 21.6 nm, σ prof = 4.0 ± 0.1 nm, and σ L,prof = 21.4 ± 0.1 nm with cut-offs for the profilometry and Fizeau measurements limited to frequencies of (1/16) µm –1 to (1/4) mm –1 .
Life-Cycle Analysis of Potentially Longer Life Expectancy CdTe PV Modules
Research on PV module longevity shows that with lower degradation rates and better encapsulation, PV modules can significantly outlast their current life expectancy of 25-30 years. The focus of this study is on alternative CdTe PV module back-contact and encapsulation materials that show the potential of increasing module operation lives from 30 to 40 and 50 years. Life-cycle-analyis shows that some alternative materials may slightly increase cradle-to-gate environmental impacts per m2 of module, but increased operational life more than counterbalances such impacts. The life-cycle carbn footprint of systems operating under average US insolation conditions of 1800 kWh/m2/yr is reduced from 10 gCO2eq/kWh to 6 gCO2eq/kWh when the operation life increases from 30 to 50 yrs. Similar reductions are noted for all life-cycle impact indicators, whereas the EROI of the considered system increases from 67 to 177 as life increases from 30 to 50 yrs.
Radiotherapy using hard wedges is no longer appropriate and should be discontinued
No abstract prepared.
Comparison of damage and ablation dynamics of multilayer dielectric films initiated by few-cycle pulses versus longer femtosecond pulses
The importance of high intensity few- to single-cycle laser pulses for applications such as intense isolated attosecond pulse generation is constantly growing, and with the breakdown of the monochromatic approximation in field ionization models, the few-cycle pulse (FCP) interaction with solids near the damage threshold has ushered a new paradigm of nonperturbative light–matter interaction. In this Letter, we systematically study and contrast how femtosecond laser-induced damage and ablation behaviors of SiO 2 /HfO 2 -based reflective multilayer dielectric thin film systems vary between FCP and 110 fs pulses. With time-resolved surface microscopy and ex situ analysis, we show that there are distinct differences in the interaction depending on the pulse duration, specifically in the “blister” morphology formation at lower fluences (damage) as well as in the dynamics of debris formation at higher fluences (ablation).