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  1. One of the main sources of uncertainty for understanding global warming is understanding the formation of larger secondary aerosols.

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    Free, publicly-accessible full text available September 14, 2024
  2. This paper presents a comprehensive study of the theory of entangled two-photon emission/absorption (E2P-EA) between a many-level cascade donor and a many-level acceptor (which could be quantum dots or molecules) using second-order perturbation theory and where the donor–acceptor pair is in a homogeneous but dispersive medium. To understand the mechanism of E2P-EA, we analyze how dipole orientation, radiative lifetime, energy detuning between intermediate states, separation distance, and entanglement time impact the E2P-EA rate. Our study shows that there are quantum interference effects in the E2P-EA rate expression that lead to oscillations in the rate as a function of entanglement time. Furthermore, we find that the E2P-EA rate for a representative system consisting of two quantum dots can be comparable to one-photon emission/absorption (OP-EA) when donor and acceptor are within a few nm. However, the E2P-EA rate falls off much more quickly with separation distance than does OP-EA. 
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    Free, publicly-accessible full text available August 21, 2024
  3. Abstract Developing an eco-friendly, efficient, and highly selective gold-recovery technology is urgently needed in order to maintain sustainable environments and improve the utilization of resources. Here we report an additive-induced gold recovery paradigm based on precisely controlling the reciprocal transformation and instantaneous assembly of the second-sphere coordinated adducts formed between β-cyclodextrin and tetrabromoaurate anions. The additives initiate a rapid assembly process by co-occupying the binding cavity of β-cyclodextrin along with the tetrabromoaurate anions, leading to the formation of supramolecular polymers that precipitate from aqueous solutions as cocrystals. The efficiency of gold recovery reaches 99.8% when dibutyl carbitol is deployed as the additive. This cocrystallization is highly selective for square-planar tetrabromoaurate anions. In a laboratory-scale gold-recovery protocol, over 94% of gold in electronic waste was recovered at gold concentrations as low as 9.3 ppm. This simple protocol constitutes a promising paradigm for the sustainable recovery of gold, featuring reduced energy consumption, low cost inputs, and the avoidance of environmental pollution. 
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    Free, publicly-accessible full text available December 1, 2024
  4. Multiphoton absorption of entangled photons offers ways for obtaining unique information about chemical and biological processes. Measurements with entangled photons may enable sensing biological signatures with high selectivity and at very low light levels to protect against photodamage. In this paper, we present a theoretical and experimental study of the excitation wavelength dependence of the entangled two-photon absorption (ETPA) process in a molecular system, which provides insights into how entanglement affects molecular spectra. We demonstrate that the ETPA excitation spectrum can be different from that of classical TPA as well as that for one-photon resonant absorption (OPA) with photons of doubled frequency. These results are modeled by assuming the ETPA cross-section is governed by a two-photon excited state radiative linewidth rather than by electron-phonon interactions, and this leads to excitation spectra that match the observed results. Further, we find that the two-photon-allowed states with highest TPA and ETPA intensities have high electronic entanglements, with ETPA especially favoring states with the longest radiative lifetimes. These results provide concepts for the development of quantum light–based spectroscopy and microscopy that will lead to much higher efficiency of ETPA sensors and low-intensity detection schemes. 
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    Free, publicly-accessible full text available August 29, 2024
  5. Becker, Anke (Ed.)
    ABSTRACT The transcriptional regulator PecS is encoded by select bacterial pathogens. For instance, in the plant pathogen Dickeya dadantii , PecS controls a range of virulence genes, including pectinase genes and the divergently oriented gene pecM , which encodes an efflux pump through which the antioxidant indigoidine is exported. In the plant pathogen Agrobacterium fabrum (formerly named Agrobacterium tumefaciens ), the pecS-pecM locus is conserved. Using a strain of A. fabrum in which pecS has been disrupted, we show here that PecS controls a range of phenotypes that are associated with bacterial fitness. PecS represses flagellar motility and chemotaxis, which are processes that are important for A. fabrum to reach plant wound sites. Biofilm formation and microaerobic survival are reduced in the pecS disruption strain, whereas the production of acyl homoserine lactone (AHL) and resistance to reactive oxygen species (ROS) are increased when pecS is disrupted. AHL production and resistance to ROS are expected to be particularly relevant in the host environment. We also show that PecS does not participate in the induction of vir genes. The inducing ligands for PecS, urate, and xanthine, may be found in the rhizosphere, and they accumulate within the plant host upon infection. Therefore, our data suggest that PecS mediates A. fabrum fitness during its transition from the rhizosphere to the host plant. IMPORTANCE PecS is a transcription factor that is conserved in several pathogenic bacteria, where it regulates virulence genes. The plant pathogen Agrobacterium fabrum is important not only for its induction of crown galls in susceptible plants but also for its role as a tool in the genetic manipulation of host plants. We show here that A. fabrum PecS controls a range of phenotypes, which would confer the bacteria an advantage while transitioning from the rhizosphere to the host plant. This includes the production of signaling molecules, which are critical for the propagation of the tumor-inducing plasmid. A more complete understanding of the infection process may inform approaches by which to treat infections as well as to facilitate the transformation of recalcitrant plant species. 
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    Free, publicly-accessible full text available July 25, 2024
  6. Free, publicly-accessible full text available April 1, 2024
  7. Abstract

    Climate change is impacting global crop productivity, and agricultural land suitability is predicted to significantly shift in the future. Responses to changing conditions and increasing yield variability can range from altered management strategies to outright land use conversions that may have significant environmental and socioeconomic ramifications. However, the extent to which agricultural land use changes in response to variations in climate is unclear at larger scales. Improved understanding of these dynamics is important since land use changes will have consequences not only for food security but also for ecosystem health, biodiversity, carbon storage, and regional and global climate. In this study, we combine land use products derived from the Moderate Resolution Imaging Spectroradiometer with climate reanalysis data from the European Centre for Medium-Range Weather Forecasts Reanalysis v5 to analyze correspondence between changes in cropland and changes in temperature and water availability from 2001 to 2018. While climate trends explained little of the variability in land cover changes, increasing temperature, extreme heat days, potential evaporation, and drought severity were associated with higher levels of cropland loss. These patterns were strongest in regions with more cropland change, and generally reflected underlying climate suitability—they were amplified in hotter and drier regions, and reversed direction in cooler and wetter regions. At national scales, climate response patterns varied significantly, reflecting the importance of socioeconomic, political, and geographic factors, as well as differences in adaptation strategies. This global-scale analysis does not attempt to explain local mechanisms of change but identifies climate-cropland patterns that exist in aggregate and may be hard to perceive at local scales. It is intended to supplement regional studies, providing further context for locally-observed phenomena and highlighting patterns that require further analysis.

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  8. Free, publicly-accessible full text available May 1, 2024
  9. Free, publicly-accessible full text available July 1, 2024