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At least 19 records

A "Warm Formamide" Scenario for the Origins of Life Might not be so Hot: Comment on "Formamide and the Origin of Life"

In this review, Saladino et al. present an intriguing hypothesis surrounding the role of formamide in the origins of life on Earth, backed by experimental results supporting each step from formamide to RNA polymers. The overall premise is that, from formamide and inorganic phosphate, RNA molecules over 100 nucleotides in length can be produced. In addition, many carboxylic acids likely relevant to prebiotic metabolism, are formed along the way. Thus, from a rather simple organic molecule that has been observed in outer space (formamide), you can generate many of the compounds necessary for the origins of life. However, because high temperatures (160 C) are required for the formamide reactions, it remains unclear where the "warm formamide" scenario could have occurred. Low-temperature, aqueous hydrogen cyanide-based prebiotic chemistry that we know actually happened has been shown to produce many of the molecules invoked in the formamide hypothesis: amino acids, carboxylic acids, sugar acids, and nucleobases have all been found in meteorites recovered on Earth, providing a plausible route for their synthesis and delivery. In contrast, a large portion of the formamide hypothesis is based on relatively hightemperature reactions, A plausible milieu for high-temperature reactions with concentrated formamide is yet to be described, and is critical for this hypothesis to be validated. Hydrothermal vents are attractive heat sources, and the higher boiling point of formamide has been invoked as a mechanism to concentrate it from an aqueous solution, Unless the water can actually evaporate, however, there would be no net enrichment. For example, in the context of a deep-sea vent, any water "removed" by heating would be quickly replaced. Some of the individual reactions underpinning the present hypothesis have been met with skepticism because they go against conventional wisdom, To name a few of the surprising results: the observation that nucleosides can be converted to cyclic phosphates when heated in the presence of minerals and inorganie phosphate; that 3'-5' cGMP and cAMP nucleotides polymerize rapidly into RNA oligomers, even in the absence of monovalent counterions and that end-to-end ligation reactions between RNA oligomers occur in essentially pure water, without requiring any activating groups or counterions. Because the polymerization reactions are simply transesterification reactions, that they readily occur in the absence of cations makes one wonder why nearly all ribozyme-catalyzed transesterification reactions are metal-ion dependent; similarly, that the end-to-end ligation reactions do not require activation runs counter to the observation that all protein-catalyzed ligation and polymerization reactions of RNA and DNA require activated substrates. Detailed mechanistic studies of the reported reactions are warranted and could provide important insights for understanding the chemistry behind the origins of life. Because the authors have produced many of the experimental results supporting their hypothesis, they could demonstrate the validity of their hypothesis by converting formamide into approx 100 nucleotide RNA oligomers, using the products of one reaction as the reactants for the next reaction, under specific conditions plausible on the pre-biotic Earth. Such a demonstration would represent a milestone for our understanding of the origins of life.

Burton, Aaron S.↗

Origins of Solar Systems Workshop: The Origin, Evolution, and Detectability of Short Period Comets

The origin of the short period comets (SPC) (periods less than 200 years), the dynamical formation of their present reservoir(s), the cause and rate of their transport to the inner planetary region where they can be detected, and the magnitude of selection effects in their discovery are important research questions directly coupled to the goals of understanding the origin and evolution of the Solar System. To address these questions in an intensive way, an interdisciplinary, five month long Workshop from Jan. to May 1993 at Southwest Research Institute (SwRI) in San Antonio was convened. The goal of this Workshop was to advance the state of understanding about the origins, dynamical evolution, and present location of short period comets and their reservoir(s).

Stern, S. Alan↗

Comparison of Origin 2000 and Origin 3000 Using NAS Parallel Benchmarks

This report describes results of benchmark tests on the Origin 3000 system currently being installed at the NASA Ames National Advanced Supercomputing facility. This machine will ultimately contain 1024 R14K processors. The first part of the system, installed in November, 2000 and named mendel, is an Origin 3000 with 128 R12K processors. For comparison purposes, the tests were also run on lomax, an Origin 2000 with R12K processors. The BT, LU, and SP application benchmarks in the NAS Parallel Benchmark Suite and the kernel benchmark FT were chosen to determine system performance and measure the impact of changes on the machine as it evolves. Having been written to measure performance on Computational Fluid Dynamics applications, these benchmarks are assumed appropriate to represent the NAS workload. Since the NAS runs both message passing (MPI) and shared-memory, compiler directive type codes, both MPI and OpenMP versions of the benchmarks were used. The MPI versions used were the latest official release of the NAS Parallel Benchmarks, version 2.3. The OpenMP versiqns used were PBN3b2, a beta version that is in the process of being released. NPB 2.3 and PBN 3b2 are technically different benchmarks, and NPB results are not directly comparable to PBN results.

Turney, Raymond D.↗

A 'Warm Formamide' Scenario for the Origins of Life Might Not Be so Hot Comment on 'Formamide and the Origin of Life' by E. Di Mauro Et Al.

In this review, Saladino et al. present an intriguing hypothesis surrounding the role of formamide in the originsof life on Earth, backed by experimental results supporting each step from formamide to RNA polymers [1]. The overall premise is that, from formamide and inorganic phosphate, RNA molecules over 100 nucleotides in length canbe produced. In addition, many carboxylic acids likely relevant to prebiotic metabolism are formed along the way. Thus, from a rather simple organic molecule that has been observed in outer space (formamide), you can generatemany of the compounds necessary for the origins of life. However, because high temperatures (160 C) are requiredfor the formamide reactions, it remains unclear where the warm formamide scenario could have occurred.Low-temperature, aqueous hydrogen counter to the observation that all protein-catalyzed ligation and polymerization reactions of RNA and DNA requireactivated substrates. Detailed mechanistic studies of the reported reactions are warranted and could provide important insights for understanding the chemistry behind the origins of life.Because the authors have produced many of the experimental results supporting their hypothesis, they coulddemonstrate the validity of their hypothesis by converting formamide into 100 nucleotide RNA oligomers, usingthe products of one reaction as the reactants for the next reaction, under specific conditions plausible on the pre-bioticEarth. Such a demonstration would represent a milestone for our understanding of the origins of life.cyanide-based prebiotic chemistry that we know actually happened has beenshown to produce many of the molecules invoked in the formamide hypothesis: amino acids, carboxylic acids, sugaracids, and nucleobases have all been found in meteorites recovered on Earth [e.g. [24]], providing a plausible routefor their synthesis and delivery. In contrast, a large portion of the formamide hypothesis is based on relatively high-temperature reactions. A plausible milieu for high-temperature reactions with concentrated formamide is yet to bedescribed, and is critical for this hypothesis to be validated. Hydrothermal vents are attractive heat sources, and the higher boiling point of formamide has been invoked as a mechanism to concentrate it from an aqueous solution.Unless the water can actually evaporate, however, there would be no net enrichment. For example, in the context of a deep-sea vent, any water removed by heating would be quickly replaced.Some of the individual reactions underpinning the present hypothesis [1] have been met with skepticism becausethey go against conventional wisdom. To name a few of the surprising results: the observation that nucleosides can beconverted to cyclic phosphates when heated in the presence of minerals and inorganic phosphate [5]; that 35 cGMPand cAMP nucleotides polymerize rapidly into RNA oligomers, even in the absence of monovalent counterions [6];and that end-to-end ligation reactions between RNA oligomers occur in essentially pure water, without requiring any activating groups or counterions [7,8]. Because the polymerization reactions are simply transesterification reactions,that they readily occur in the absence of cations makes one wonder why nearly all ribozyme-catalyzed transesterification reactions are metal-ion dependent; similarly, that the end-to-end ligation reactions do not require activation runs.

life↗

Kinetic Probes of the Origin of Activity in MOF-Based C–H Oxidation Catalysis

The development of homogeneous catalysis is enabled by the availability of a rich toolkit of kinetics experiments, such as the Hgdrop test, that differentiate catalytic activity at ligand-supported metal complexes from potential heterogeneous catalysts derived from decomposition of molecular species. Metal-organic frameworks (MOFs) have garnered significant attention as platforms for catalysis at site-isolated, interstitial catalyst sites. Unlike homogeneous catalysis, relatively few strategies have been advanced to evaluate the origin of catalytic activity in MOF-promoted reactions. Many of the MOFs that have been examined as potential catalysts are comprised of molecular constituents that represent viable catalysts in the absence of the extended MOF lattice, and thus interfacial sites and leached homogeneous species represent potential sources of catalyst activity. Here, we demonstrate that analysis of deuterium kinetic isotope effects (KIEs) and olefin epoxidation diastereoselectivity provides probes of the origin of catalytic activity in MOF-promoted oxidation reactions. These analyses support involvement of lattice-based Fe sites in the turnover-limiting step of C–H activation with Fe-MOF-74-based materials (i.e., the MOF functions as a bona fide catalyst) and evidence that Cu 2 -based MOF MIL-125-Cu 2 O 2 functions as a solid-state initiator for solution-phase oxidation chemistry and is not involved in the turnover limiting step (i.e., the MOF does not function as a catalyst for substrate functionalization). furthermore, we anticipate that the simple experiments described here will provide a valuable tool for clarifying the role of MOFs in C–H oxidation reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Comparison of 250 MHz R10K Origin 2000 and 400 MHz Origin 2000 Using NAS Parallel Benchmarks

This report describes results of benchmark tests on Steger, a 250 MHz Origin 2000 system with R10K processors, currently installed at the NASA Ames National Advanced Supercomputing (NAS) facility. For comparison purposes, the tests were also run on Lomax, a 400 MHz Origin 2000 with R12K processors. The BT, LU, and SP application benchmarks in the NAS Parallel Benchmark Suite and the kernel benchmark FT were chosen to measure system performance. Having been written to measure performance on Computational Fluid Dynamics applications, these benchmarks are assumed appropriate to represent the NAS workload. Since the NAS runs both message passing (MPI) and shared-memory, compiler directive type codes, both MPI and OpenMP versions of the benchmarks were used. The MPI versions used were the latest official release of the NAS Parallel Benchmarks, version 2.3. The OpenMP versions used were PBN3b2, a beta version that is in the process of being released. NPB 2.3 and PBN3b2 are technically different benchmarks, and NPB results are not directly comparable to PBN results.

Turney, Raymond D.↗

Detection of hot electrons originating from an upper valley at ∼1.7eV above the Γ valley in wurtzite GaN using electron emission spectroscopy

Using electron emission spectroscopy, measurement and analysis were conducted on the energy distribution of vacuum emitted electrons from electrically driven InGaN/GaN green (peak wavelengths 𝜆 ≈ 515nm) light-emitting diodes (LEDs) with and without a prewell superlattice (SL). Here, we report on the detection of a high-energy upper valley at ∼ 1.7eV above the Γ valley from samples with no prewell SL. We propose that these upper valley electrons originate predominantly from trap-assisted Auger recombination (TAAR) in green LEDs, as the intensity of these peaks is found to have quadratic dependence on the carrier density 𝑛 [see Espenlaub et al., J. Appl. Phys. 126, 184502 (2019)]. The high-energy upper valley peak was not observed in the sample with a prewell SL which is attributed to gettering by the prewell SL of still unidentified impurities that act as TAAR centers.

carrier generation & recombination↗

The intercrater plains of Mercury and the Moon: Their nature, origin and role in terrestrial planet evolution. Discussion of the nature, origin and role of the intercrater plains of Mercury and the Moon

The nature and origin of the intercrater plains of Mercury and the Moon as determined through geologic mapping, crater statistics, and remotely sensed data are summarized. Implications of these results regarding scarp formation, absolute ages, and terrestrial planet surfaces are included. The role of the intercrater plains is defined and future work which might lead to a better understanding of these units and terrestrial planet evolution is outlined.

Leake, M. A.↗

The Origins Survey Spectrometer (OSS): A Far-IR Discovery Machine for the Origins Space Telescope

The OSS on the Origins Space Telescope is designed to decode the cosmic history of nucleosynthesis, star formation, and supermassive black hole growth with wide-area spatial-spectral 3-D surveys across the full 25 to 590 micron band. Six wideband grating modules combine to cover the full band at R=300, each couples a long slit with 60–190 beams on the sky. OSS will have a total of 120,000 background-limited detector pixels in the six 2-D arrays which provide spatial and spectral coverage. The suite of grating modules can be used for pointed observations of targets of interest, and are particularly powerful for 3-D spectral spectral surveys. To chart the transition from interstellar material, particularly water, to planetary systems, two high-spectral-resolution modes are included. The first incorporates a Fourier-transform spectrometer (FTS) in front of the gratings providing resolving power of 25,000 (δv = 12 km/s) at 179µm to resolve water emission in protoplanetary disk spectra. The second boosts the FTS capability with an additional etalon (Fabry-Perot interferometer) to provide 2 km/s resolution in this line to enable detailed structural studies of disks in the various water and HD lines. Optical, thermal, and mechanical designs are presented, and the system approach to the detector readout enabling the large formats is described.

Pontoppidan, Klaus↗

On the Origin of Room-Temperature Amplified Spontaneous Emission in CsPbBr 3 Single Crystals

CsPbBr 3 is an all-inorganic halide perovskite with excellent photoluminescence (PL) properties for laser applications. Amplified spontaneous emission (ASE) is a prerequisite for lasing and typically observed from low-dimensional CsPbBr3 nanostructures, where quantum confinement enhances ASE. However, a gain medium for lasing should be prepared into a robust bulk form that works under intense light illumination. Here, we demonstrate that bulk CsPbBr 3 single crystals exhibit highly efficient ASE with a threshold of 46 MWcm -2 at 520 nm, if PL reabsorption via the indirect Rashba gap is properly suppressed by thickness control. Based on a series of spectroscopic and microscopic measurements, we show that this below-the-gap absorption can significantly alter the PL feature and even the apparent color of the crystal depending on the crystal size. Our results show that a thin CsPbBr 3 single crystal can be utilized for lasing applications when engineered into a submillimeter thickness for effective light–matter interaction.

36 MATERIALS SCIENCE↗