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At least 343 records · Page 19

DRILL Interface Makes Ion Soft Landing Broadly Accessible for Energy Science and Applications

Polyoxometalates (POM) have been deposited onto carbon nanotube (CNT) electrodes using benchtop ion soft landing (SL) enabled by a vortex-confined electrohydrodynamic desolvation process. The device is based on the dry ion localization and locomotion (DRILL) mass spectrometry interface of Fedorov and co-workers. By adding electrospray emitters, heating the desolvation gas, and operating at high gas flow rates, it is possible to obtain stable ion currents up to -15 nA that are ideal for deposition. Coupled with ambient ion optics, this interface enables desolvated ions to be delivered to surfaces while excluding solvent and counterions. Electron microscopy of surfaces prepared using the device reveal discrete POM and no aggregation that degrades electrode performance. Characterization of POM-coated CNT electrodes in a supercapacitor showed an energy storage capacity similar to that achieved with SL in vacuum. For solutions that produce primarily a single ion by electrospray ionization, benchtop SL offers a simpler and less costly approach for surface modification with applications in catalysis, energy storage, and beyond.

Johnson, Grant E.↗

An overview of the Earth system science of solar geoengineering: Overview of the earth system science of solar geoengineering

Solar geoengineering has been proposed as a means to cool the planet by increasing the reflection of sunlight back to space, for example by injecting reflective aerosol particles into the middle atmosphere. Such proposals are not able to physically substitute for mitigation of greenhouse gas emissions as a response to the risks of climate change, but might eventually be applied as a complementary approach to reduce climate risks. Thus, the Earth system consequences of solar geoengineering are central to understanding its potentials and risks. Here we review the state-of-the-art knowledge about geoengineering by stratospheric sulphate aerosol injection. We examine the common responses found in studies of an idealized form of solar geoengineering, in which the intensity of incoming sunlight is directly reduced in models. The studies reviewed are consistent in suggesting that solar geoengineering would generally reduce the differences in climate in comparison to future scenarios with elevated greenhouse gas concentrations and no solar geoengineering. However, it is clear that a solar geoengineered climate would be novel in some respects, for example a notable reduction in the intensity of the hydrological cycle. We provide an overview of the unique aspects of the response to stratospheric aerosol injection and the uncertainties around its consequences. We also consider the issues raised by the partial control over the climate that solar geoengineering would allow. Finally, this overview also highlights the key research gaps that will need to be resolved in order to effectively guide future decisions on the potential use of solar geoengineering.

58 GEOSCIENCES↗

Data Science-Driven Analysis of Substrate-Permissive Diketopiperazine Reverse Prenyltransferase NotF: Applications in Protein Engineering and Cascade Biocatalytic Synthesis of (-)-Eurotiumin A

Prenyltransfer is an early-stage carbon-hydrogen bond (C-H) functionalization prevalent in the biosynthesis of a diverse array of biologically active bacterial, fungal, plant, and metazoan diketopiperazine (DKP) alkaloids. Toward the development of a unified strategy for biocatalytic construction of prenylated DKP indole alkaloids, we sought to identify and characterize a substrate-permissive C2 reverse prenyltransferase (PT). As the first tailoring event within the biosynthesis of cytotoxic notoamide metabolites, PT NotF catalyzes C2 reverse prenyltransfer of brevianamide F. Solving a crystal structure of NotF (in complex with native substrate and prenyl donor mimic dimethylallyl S-thiolodiphosphate (DMSPP)) revealed a large, solvent-exposed active site, intimating NotF may possess a significantly broad substrate scope. To assess the substrate selectivity of NotF, we synthesized a panel of 30 sterically and electronically differentiated tryptophanyl DKPs, the majority of which were selectively prenylated by NotF in synthetically useful conversions (2 to > 99%). Quantitative representation of this substrate library and development of a descriptive statistical model provided insight into the molecular origins of NotF's substrate promiscuity. This approach enabled the identification of key substrate descriptors (electrophilicity, size, and flexibility) that govern the rate of NotF-catalyzed prenyltransfer, and the development of an "induced fit docking (IFD)-guided" engineering strategy for improved turnover of our largest substrates. We further demonstrated the utility of NotF in tandem with oxidative cyclization using flavin monooxygenase, BvnB. This one-pot, in vitro biocatalytic cascade enabled the first chemoenzymatic synthesis of the marine fungal natural product, (-)-eurotiumin A, in three steps and 60% overall yield.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Earth Sciences Are the Model Sciences of the Anthropocene

After 4.5 billion years as a dynamic and evolving planet, Earth today continues to evolve but with new dynamics. Earth scientists writ large have special opportunities and responsibilities to accelerate our understanding of the changes that are transforming our most remarkable home.

Richter, Daniel↗

A practical superconducting-microcalorimeter X-ray spectrometer for beamline and laboratory science

We describe a series of microcalorimeter X-ray spectrometers designed for a broad suite of measurement applications. The chief advantage of this type of spectrometer is that it can be orders of magnitude more efficient at collecting X-rays than more traditional high-resolution spectrometers that rely on wavelength-dispersive techniques. This advantage is most useful in applications that are traditionally photon-starved and/or involve radiation-sensitive samples. Each energy-dispersive spectrometer is built around an array of several hundred transition-edge sensors (TESs). TESs are superconducting thin films that are biased into their superconducting-to-normal-metal transitions. The spectrometers share a common readout architecture and many design elements, such as a compact, 65 mK detector package, 8-column time-division-multiplexed superconducting quantum-interference device readout, and a liquid-cryogen-free cryogenic system that is a two-stage adiabatic-demagnetization refrigerator backed by a pulse-tube cryocooler. We have adapted this flexible architecture to mate to a variety of sample chambers and measurement systems that encompass a range of observing geometries. There are two different types of TES pixels employed. The first, designed for X-ray energies below 10 keV, has a best demonstrated energy resolution of 2.1 eV (full-width-at-half-maximum or FWHM) at 5.9 keV. The second, designed for X-ray energies below 2 keV, has a best demonstrated resolution of 1.0 eV (FWHM) at 500 eV. Our team has now deployed seven of these X-ray spectrometers to a variety of light sources, accelerator facilities, and laboratory-scale experiments; these seven spectrometers have already performed measurements related to their applications. Another five of these spectrometers will come online in the near future. We have applied our TES spectrometers to the following measurement applications: synchrotron-based absorption and emission spectroscopy and energy-resolved scattering; accelerator-based spectroscopy of hadronic atoms and particle-induced-emission spectroscopy; laboratory-based time-resolved absorption and emission spectroscopy with a tabletop, broadband source; and laboratory-based metrology of X-ray-emission lines. Here, we discuss the design, construction, and operation of our TES spectrometers and show first-light measurements from the various systems. Finally, because X-ray-TES technology continues to mature, we discuss improvements to array size, energy resolution, and counting speed that we anticipate in our next generation of TES-X-ray spectrometers and beyond.

47 OTHER INSTRUMENTATION↗

Book Review: What Makes a Good Experiment? Reasons and Roles in Science

Classification is an arduous and sometimes controversial undertaking because of its inherent cultural particularity. One famous literary example is the fictitious nomenclature of animals found in Jorge Luis Borges’s ‘The Analytical Language of John Wilkins’. According to Borges, that taxonomy was discovered by a translator, F. Kuhn, in a Chinese source and divides all animals into fourteen categories, starting with ‘those that belong to the Emperor’ and ending with ‘those that from a long way off look like flies’. Physics of the twentieth century is a ramified full-fledged technical culture, and it should surprise no one that physics experiments can be classified in different ways, allowing certain experiments to belong to more than one category. Allan Franklin’s analysis of experiments is based on his classification, which substantially grasps the essence of the experimental enterprise. Although Franklin does not offer an explicit answer to the question posed in the title, he does include a detailed examination of several important physics and biology experiments in history

Pronskikh, Vitaly↗

Science with the space-based interferometer LISA. IV: probing inflation with gravitational waves

We investigate the potential for the LISA space-based interferometer to detect the stochastic gravitational wave background produced from different mechanisms during inflation. Focusing on well-motivated scenarios, we study the resulting contributions from particle production during inflation, inflationary spectator fields with varying speed of sound, effective field theories of inflation with specific patterns of symmetry breaking and models leading to the formation of primordial black holes. The projected sensitivities of LISA are used in a model-independent way for various detector designs and configurations. We demonstrate that LISA is able to probe these well-motivated inflationary scenarios beyond the irreducible vacuum tensor modes expected from any inflationary background.

79 ASTRONOMY AND ASTROPHYSICS↗