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  1. Accelerated reactions in microdroplets have been reported for a wide range of reactions with some microdroplet reactions occurring over a million times faster than the same reaction in bulk solution. Unique chemistry at the air–water interface has been implicated as a primary factor for accelerated reaction rates, but the role of analyte concentration in evaporating droplets has not been as well studied. Here, theta-glass electrospray emitters and mass spectrometry are used to rapidly mix two solutions on the low to sub-microsecond time scale and produce aqueous nanodrops with different sizes and lifetimes. We demonstrate that for a simple bimolecular reaction where surface chemistry does not appear to play a role, reaction rate acceleration factors are between 10 2 and 10 7 for different initial solution concentrations, and these values do not depend on nanodrop size. A rate acceleration factor of 10 7 is among the highest reported and can be attributed to concentration of analyte molecules, initially far apart in dilute solution, but brought into close proximity in the nanodrop through evaporation of solvent from the nanodrops prior to ion formation. These data indicate that analyte concentration phenomenon is a significant factor in reaction acceleration where droplet volume throughout the experiment is not carefully controlled. 
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    Free, publicly-accessible full text available May 10, 2024
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  5. ABSTRACT

    Fast radio bursts (FRBs) are millisecond-time-scale radio transients, the origins of which are predominantly extragalactic and likely involve highly magnetized compact objects. FRBs undergo multipath propagation, or scattering, from electron density fluctuations on sub-parsec scales in ionized gas along the line of sight. Scattering observations have located plasma structures within FRB host galaxies, probed Galactic and extragalactic turbulence, and constrained FRB redshifts. Scattering also inhibits FRB detection and biases the observed FRB population. We report the detection of scattering times from the repeating FRB 20190520B that vary by up to a factor of 2 or more on minutes to days-long time-scales. In one notable case, the scattering time varied from 7.9 ± 0.4 ms to less than 3.1 ms ($95{{\ \rm per\ cent}}$ confidence) over 2.9 min at 1.45 GHz. The scattering times appear to be uncorrelated between bursts or with dispersion and rotation measure variations. Scattering variations are attributable to dynamic, inhomogeneous plasma in the circumsource medium, and analogous variations have been observed from the Crab pulsar. Under such circumstances, the frequency dependence of scattering can deviate from the typical power law used to measure scattering. Similar variations may therefore be detectable from other FRBs, even those with inconspicuous scattering, providing a unique probe of small-scale processes within FRB environments.

     
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  6. The Owens Valley Radio Observatory Long Wavelength Array is a low radio frequency all-sky imaging radio interferometer. The full 352-element array will generate more than 2 TB of visibility data per hour of observation. One of the array’s primary science cases, the search for variable radio emission from exoplanets and for transients, require fast and high dynamic range interferometric imaging. Here we detail the design and implementation of a two-pipeline infrastructure that minimizes development cost: an offline pipeline that facilitates experimentation with existing pack-ages, and a real-time pipeline that minimizes overhead. 
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  7. Abstract

    The first fast radio burst (FRB) to be precisely localized was associated with a luminous persistent radio source (PRS). Recently, a second FRB/PRS association was discovered for another repeating source of FRBs. However, it is not clear what makes FRBs or PRS or how they are related. We compile FRB and PRS properties to consider the population of FRB/PRS sources. We suggest a practical definition for PRS as FRB associations with luminosity greater than 1029erg s−1Hz−1that are not attributed to star formation activity in the host galaxy. We model the probability distribution of the fraction of FRBs with PRS for repeaters and nonrepeaters, showing there is not yet evidence for repeaters to be preferentially associated with PRS. We discuss how FRB/PRS sources may be distinguished by the combination of active repetition and an excess dispersion measure local to the FRB environment. We use CHIME/FRB event statistics to bound the mean per-source repetition rate of FRBs to be between 25 and 440 yr−1. We use this to provide a bound on the density of FRB-emitting sources in the local universe of between 2.2 × 102and 5.2 × 104Gpc−3assuming a pulsar-like beamwidth for FRB emission. This density implies that PRS may comprise as much as 1% of compact, luminous radio sources detected in the local universe. The cosmic density and phenomenology of PRS are similar to that of the newly discovered, off-nuclear “wandering” active galactic nuclei (AGN). We argue that it is likely that some PRS have already been detected and misidentified as AGN.

     
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  8. Abstract Satellite observations of tropical maritime convection indicate an afternoon maximum in anvil cloud fraction that cannot be explained by the diurnal cycle of deep convection peaking at night. We use idealized cloud-resolving model simulations of single anvil cloud evolution pathways, initialized at different times of the day, to show that tropical anvil clouds formed during the day are more widespread and longer lasting than those formed at night. This diurnal difference is caused by shortwave radiative heating, which lofts and spreads anvil clouds via a mesoscale circulation that is largely absent at night, when a different, longwave-driven circulation dominates. The nighttime circulation entrains dry environmental air that erodes cloud top and shortens anvil lifetime. Increased ice nucleation in more turbulent nighttime conditions supported by the longwave cloud-top cooling and cloud-base heating dipole cannot compensate for the effect of diurnal shortwave radiative heating. Radiative–convective equilibrium simulations with a realistic diurnal cycle of insolation confirm the crucial role of shortwave heating in lofting and sustaining anvil clouds. The shortwave-driven mesoscale ascent leads to daytime anvils with larger ice crystal size, number concentration, and water content at cloud top than their nighttime counterparts. Significance Statement Deep convective activity and rainfall peak at night over the tropical oceans. However, anvil clouds that originate from the tops of deep convective clouds reach their largest extent in the afternoon hours. We study the underlying physical mechanisms that lead to this discrepancy by simulating the evolution of anvil clouds with a high-resolution model. We find that the absorption of sunlight by ice crystals lofts and spreads the daytime anvil clouds over a larger area, increasing their lifetime, changing their properties, and thus influencing their impact on climate. Our findings show that it is important not only to simulate the correct onset of deep convection but also to correctly represent anvil cloud evolution for skillful simulations of the tropical energy balance. 
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  9. Abstract

    Cellulases are largely afflicted by inhibition from their reaction products, especially at high-substrate loading, which represents a major challenge for biomass processing. This challenge was overcome for endoglucanase 1 (E1) from Acidothermus cellulolyticus by identifying a large conformational change involving distal residues upon binding cellobiose. Having introduced alanine substitutions at each of these residues, we identified several mutations that reduced cellobiose inhibition of E1, including W212A, W213A, Q247A, W249A and F250A. One of the mutations (W212A) resulted in a 47-fold decrease in binding affinity of cellobiose as well as a 5-fold increase in the kcat. The mutation further increased E1 activity on Avicel and dilute-acid treated corn stover and enhanced its productivity at high-substrate loadings. These findings were corroborated by funnel metadynamics, which showed that the W212A substitution led to reduced affinity for cellobiose in the +1 and +2 binding sites due to rearrangement of key cellobiose-binding residues.

     
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  10. null (Ed.)