Atmospheric chemistry-climate feedbacks

We extend the theory of climate feedbacks to include atmospheric chemistry. A change in temperature caused by a radiative forcing will include, in general, a contribution from the chemical change that is fed back into the climate system; likewise, the change in atmospheric burdens caused by a chemical forcing will include a contribution from the associated climate change that is fed back into the chemical system. The theory includes two feedback gains, G_(che) and G_(cli). G_(che) is defined as the ratio of the change in equilibrium global mean temperature owing to long-lived greenhouse gas radiative forcing, under full climate-chemistry coupling, to that in the absence of coupling. G_(cli) is defined as the ratio of the change in equilibrium mean aerosol or gas-phase burdens owing to chemical forcing under full coupling, to that in the absence of coupling. We employ a climate-atmospheric chemistry model based on the Goddard Institute for Space Studies (GISS) GCM II', including tropospheric gas-phase chemistry, sulfate, nitrate, ammonium, black carbon, and organic carbon. While the model describes many essential couplings between climate and atmospheric chemistry, not all couplings are accounted for, such as indirect aerosol forcing and the role of natural dust and sea salt aerosols. Guided by the feedback theory, we perform perturbation experiments to quantify G_(che) and G_(cli). We find that G_(che) for surface air temperature is essentially equal to 1.00 on a planetary scale. Regionally, G_(che) is estimated to be 0.80–1.30. The gains are small compared to those of the physical feedbacks in the climate system (e.g., water vapor, and cloud feedbacks). These values for G_(che) are robust for the specific model used, but may change when using more comprehensive climate-atmospheric chemistry models. Our perturbation experiments do not allow one to obtain robust values for G_(cli). Globally averaged, the values range from 0.99 to 1.28, depending on the chemical species, while, in areas of high pollution, G_(cli) can be up to 1.15 for ozone, and as large as 1.40 for total aerosol. These preliminary values indicate a significant role of climate feedbacks in the atmospheric chemistry system

Multiferroic and Ferroic Topological Order in Ligand-Functionalized Germanene and Arsenene

Two-dimensional (2D) materials that exhibit ferroelectric, ferromagnetic, or topological order have been a major focal topic of nanomaterials research in recent years. The latest efforts in this field explore 2D quantum materials that host multiferroic or concurrent ferroic and topological order. We present a computational discovery of multiferroic state with coexisting ferroelectric and ferromagnetic order in recently synthesized CH2OCH3-functionalized germanene. We show that an electric-field-induced rotation of the ligand CH2OCH3 molecule can serve as the driving mechanism to switch the electric polarization of the ligand molecule, while unpassivated Ge p(z) orbits generate ferromagnetism. Our study also reveals coexisting ferroelectric and topological order in ligand-functionalized arsenene, which possesses a switchable electric polarization and a Dirac transport channel. These findings offer insights into the fundamental physics underlying these coexisting quantum orders and open avenues for achieving states of matter with multiferroic or ferroic-topological order in 2D-layered materials for innovative memory or logic device implementations

Beyond the single-atom response in absorption lineshapes: Probing a dense, laser-dressed helium gas with attosecond pulse trains

We investigate the absorption line shapes of laser-dressed atoms beyond the single-atom response, by using extreme ultraviolet (XUV) attosecond pulse trains to probe an optically thick helium target under the influence of a strong infrared (IR) field. We study the interplay between the IR-induced phase shift of the microscopic time-dependent dipole moment and the resonant-propagation-induced reshaping of the macroscopic XUV pulse. Our experimental and theoretical results show that as the optical depth increases, this interplay leads initially to a broadening of the IR-modified line shape, and subsequently to the appearance of new, narrow features in the absorption line.Comment: 5 pages, 5 figure

A probable aculeacin A acylase from the Ralstonia solanacearum GMI1000 is N-acyl-homoserine lactone acylase with quorum-quenching activity

<p>Abstract</p> <p>Background</p> <p>The infection and virulence functions of diverse plant and animal pathogens that possess quorum sensing systems are regulated by <it>N</it>-acylhomoserine lactones (AHLs) acting as signal molecules. AHL-acylase is a quorum quenching enzyme and degrades AHLs by removing the fatty acid side chain from the homoserine lactone ring of AHLs. This blocks AHL accumulation and pathogenic phenotypes in quorum sensing bacteria.</p> <p>Results</p> <p>An <it>aac </it>gene of undemonstrated function from <it>Ralstonia solanacearum </it>GMI1000 was cloned, expressed in <it>Escherichia coli</it>; it inactivated four AHLs that were tested. The sequence of the 795 amino acid polypeptide was considerably similar to the AHL-acylase from <it>Ralstonia </it>sp. XJ12B with 83% identity match and shared 39% identity with an aculeacin A acylase precursor from the gram-positive actinomycete <it>Actinoplanes utahensis</it>. Aculeacin A is a neutral lipopeptide antibiotic and an antifungal drug. An electrospray ionisation mass spectrometry (ESI-MS) analysis verified that Aac hydrolysed the amide bond of AHL, releasing homoserine lactone and the corresponding fatty acids. However, ESI-MS analysis demonstrated that the Aac could not catalyze the hydrolysis of the palmitoyl moiety of the aculeacin A. Moreover, the results of MIC test of aculeacin A suggest that Aac could not deacylate aculeacin A. The specificity of Aac for AHLs showed a greater preference for long acyl chains than for short acyl chains. Heterologous expression of the <it>aac </it>gene in <it>Chromobacterium violaceum </it>CV026 effectively inhibited violacein and chitinase activity, both of which were regulated by the quorum-sensing mechanism. These results indicated that Aac could control AHL-dependent pathogenicity.</p> <p>Conclusion</p> <p>This is the first study to find an AHL-acylase in a phytopathogen. Our data provide direct evidence that the functioning of the <it>aac </it>gene (NP520668) of <it>R. solanacearum </it>GMI1000 is via AHL-acylase and not via aculeacin A acylase. Since Aac is a therapeutic potential quorum-quenching agent, its further biotechnological applications in agriculture, clinical and bio-industrial fields should be evaluated in the near future.</p

Probing autoionizing states of molecular oxygen with XUV transient absorption: Electronic symmetry dependent lineshapes and laser induced modification

The dynamics of autoionizing Rydberg states of oxygen are studied using attosecond transient absorption technique, where extreme ultraviolet (XUV) initiates molecular polarization and near infrared (NIR) pulse perturbs its evolution. Transient absorption spectra show positive optical density (OD) change in the case of $ns\sigma_g$ and $nd\pi_g$ autoionizing states of oxygen and negative OD change for $nd\sigma_g$ states. Multiconfiguration time-dependent Hartree-Fock (MCTDHF) calculation are used to simulate the transient absorption spectra and their results agree with experimental observations. The time evolution of superexcited states is probed in electronically and vibrationally resolved fashion and we observe the dependence of decay lifetimes on effective quantum number of the Rydberg series. We model the effect of near-infrared (NIR) perturbation on molecular polarization and find that the laser induced phase shift model agrees with the experimental and MCTDHF results, while the laser induced attenuation model does not. We relate the electron state symmetry dependent sign of the OD change to the Fano parameters of the static absorption lineshapes.Comment: 15 pages, 8 figure

Color-complexity enabled exhaustive color-dots identification and spatial patterns testing in images

Targeted color-dots with varying shapes and sizes in images are first exhaustively identified, and then their multiscale 2D geometric patterns are extracted for testing spatial uniformness in a progressive fashion. Based on color theory in physics, we develop a new color-identification algorithm relying on highly associative relations among the three color-coordinates: RGB or HSV. Such high associations critically imply low color-complexity of a color image, and renders potentials of exhaustive identification of targeted color-dots of all shapes and sizes. Via heterogeneous shaded regions and lighting conditions, our algorithm is shown being robust, practical and efficient comparing with the popular Contour and OpenCV approaches. Upon all identified color-pixels, we form color-dots as individually connected networks with shapes and sizes. We construct minimum spanning trees (MST) as spatial geometries of dot-collectives of various size-scales. Given a size-scale, the distribution of distances between immediate neighbors in the observed MST is extracted, so do many simulated MSTs under the spatial uniformness assumption. We devise a new algorithm for testing 2D spatial uniformness based on a Hierarchical clustering tree upon all involving MSTs. Our developments are illustrated on images obtained by mimicking chemical spraying via drone in Precision Agriculture.Comment: 21 pages, 21 figure