Abstract
The fabrication of nanomaterials from the top-down gives precise structures but it is costly, whereas bottom-up assembly methods are found by trial and error. Nature evolves materials ...discovery by refining and transmitting the blueprints using DNA mutations autonomously. Genetically inspired optimisation has been used in a range of applications, from catalysis to light emitting materials, but these are not autonomous, and do not use physical mutations. Here we present an autonomously driven materials-evolution robotic platform that can reliably optimise the conditions to produce gold-nanoparticles over many cycles, discovering new synthetic conditions for known nanoparticle shapes using the opto-electronic properties as a driver. Not only can we reliably discover a method, encoded digitally to synthesise these materials, we can seed in materials from preceding generations to engineer more sophisticated architectures. Over three independent cycles of evolution we show our autonomous system can produce spherical nanoparticles, rods, and finally octahedral nanoparticles by using our optimized rods as seeds.
In external galaxies, molecular composition may be influenced by extreme environments such as starbursts and galaxy mergers. To study such molecular chemistry, we observed the luminous infrared ...galaxy and merger NGC 3256 using the Atacama Large Millimeter/submillimeter Array. We covered most of the 3 and 1.3 mm bands for a multispecies, multitransition analysis. We first analyzed intensity ratio maps of selected lines such as HCN/HCO+, which shows no enhancement at an active galactic nucleus. We then compared the chemical compositions within NGC 3256 at the two nuclei, tidal arms, and positions with influence from galactic outflows. We found the largest variation in SiO and CH3OH, species that are likely to be enhanced by shocks. Next, we compared the chemical compositions in the nuclei of NGC 3256, NGC 253, and Arp 220; these galactic nuclei have varying star formation efficiencies. Arp 220 shows higher abundances of SiO and HC3N than NGC 3256 and NGC 253. Abundances of most species do not show a strong correlation with star formation efficiencies, although the CH3CCH abundance seems to have a weak positive correlation with the star formation efficiency. Lastly, the chemistry of spiral arm positions in NGC 3256 is compared with that of W51, a Galactic molecular cloud complex in a spiral arm. We found higher fractional abundances of shock tracers, and possibly also a higher dense gas fraction in NGC 3256 compared with W51.
El balance presupuestario del gobierno mexicano es el indicador principal para evaluar la política fiscal y su impacto macroeconómico. El objetivo de este artículo es confrontar las series del ...balance fiscal de las fuentes primarias y secundarias y discernir cuál puede ser la más adecuada en la investigación histórico-económica de la etapa del desarrollo con inflación, 1934-1956, en México. Nuestra hipótesis señala que la fuente primaria en términos brutos que utiliza la metodología ingreso-egreso-balance no es la adecuada para evaluar la política gubernamental debido a que incluye rubros que distorsionan el balance fiscal y su impacto macro. La fuente primaria a utilizar es la que aplica la metodología del cálculo del balance fiscal vía su financiamiento. Las fuentes secundarias que usan la primera opción reproducen la deficiencia anotada, lo cual implica problemas de interpretación histórica. Al respecto, realizamos un análisis metodológico de la historiografía sobre el comportamiento de las finanzas públicas.
Significance
The detection of ethanolamine (
N
H
2
C
H
2
C
H
2
OH) in a molecular cloud in the interstellar medium confirms that a precursor of phospholipids is efficiently formed by interstellar ...chemistry. Hence, ethanolamine could have been transferred from the proto-Solar nebula to planetesimals and minor bodies of the Solar System and thereafter to our planet. The prebiotic availability of ethanolamine on early Earth could have triggered the formation of efficient and permeable amphiphilic molecules such as phospholipids, thus playing a relevant role in the evolution of the first cellular membranes needed for the emergence of life.
Cell membranes are a key element of life because they keep the genetic material and metabolic machinery together. All present cell membranes are made of phospholipids, yet the nature of the first membranes and the origin of phospholipids are still under debate. We report here the presence of ethanolamine in space,
N
H
2
C
H
2
C
H
2
OH, which forms the hydrophilic head of the simplest and second-most-abundant phospholipid in membranes. The molecular column density of ethanolamine in interstellar space is
N
= (1.51
±
0.07)
×
10
13
c
m
−
2
, implying a molecular abundance with respect to
H
2
of
(
0.9
−
1.4
)
×
10
−
10
. Previous studies reported its presence in meteoritic material, but they suggested that it is synthesized in the meteorite itself by decomposition of amino acids. However, we find that the proportion of the molecule with respect to water in the interstellar medium is similar to the one found in the meteorite (
10
−
6
). These results indicate that ethanolamine forms efficiently in space and, if delivered onto early Earth, could have contributed to the assembling and early evolution of primitive membranes.
The increasing interest and applications of photocatalysis, namely hydrogen production, artificial photosynthesis, and water remediation and disinfection, still face several drawbacks that prevent ...this technology from being fully implemented at the industrial level. The need to improve the performance of photocatalytic processes and extend their potential working under visible light has boosted the synthesis of new and more efficient semiconductor materials. Thus far, semiconductor–semiconductor heterojunction is the most remarkable alternative. Not only are the characteristics of the new materials relevant to the process performance, but also a deep understanding of the charge transfer mechanisms and the relationship with the process variables and nature of the semiconductors. However, there are several different charge transfer mechanisms responsible for the activity of the composites regardless the synthesis materials. In fact, different mechanisms can be carried out for the same junction. Focusing primarily on the photocatalytic generation of hydrogen, the objective of this review is to unravel the charge transfer mechanisms after the in-depth analyses of already reported literature and establish the guidelines for future research.
One of the proposed scenarios for the origin of life is the primordial RNA world, which considers that RNA molecules were likely responsible for the storage of genetic information and the catalysis ...of biochemical reactions in primitive cells, before the advent of proteins and DNA. In the last decade, experiments in the field of prebiotic chemistry have shown that RNA nucleotides can be synthesized from relatively simple molecular precursors, most of which have been found in space. An important exception is hydroxylamine, NH2OH, which, despite several observational attempts, it has not been detected in space yet. Here we present the first detection of NH2OH in the interstellar medium toward the quiescent molecular cloud G+0.693-0.027 located in the Galactic Center. We have targeted the three groups of transitions from the J = 2−1, 3−2, and 4−3 rotational lines, detecting five transitions that are unblended or only slightly blended. The derived molecular abundance of NH2OH is (2.1 0.9) × 10−10. From the comparison of the derived abundance of NH2OH and chemically related species, with those predicted by chemical models and measured in laboratory experiments, we favor the formation of NH2OH in the interstellar medium via hydrogenation of NO on dust grain surfaces, with possibly a contribution of ice-mantle NH3 oxidation processes. Further laboratory studies and quantum chemical calculations are needed to completely rule out the formation of NH2OH in the gas phase.
Brownian diffusion of spherical nanoparticles is usually exploited to ascertain the rheological properties of complex media. However, the behavior of the tracer particles is affected by a number of ...phenomena linked to the interplay between the dynamics of the particles and polymer coils. For this reason, the characteristic lengths of the dispersed entities, depletion phenomena, and the presence of sticking conditions have been observed to affect the translational diffusion of the probes. On the other hand, the retardation effect of the host fluid on the rotational diffusion of nonspherical particles is less understood. We explore the possibility of studying this phenomenon by analyzing the electro-orientation of the particles in different scenarios in which we vary the ratio between the particle and polymer characteristic size, and the geometry of the particles, including both elongated and oblate shapes. We find that the Stokes–Einstein relation only applies if the radius of gyration of the polymer is much shorter than the particle size and when some repulsive interaction between both is present.
The chemical compounds carrying the thiol group (-SH) have been considered essential in recent prebiotic studies regarding the polymerization of amino acids. We have searched for this kind of ...compound toward the Galactic Center quiescent cloud G+0.693–0.027. We report the first detection in the interstellar space of the trans-isomer of monothioformic acid (t-HC(O)SH) with an abundance of ∼1 נ10−10. Additionally, we provide a solid confirmation of the gauche isomer of ethyl mercaptan (g-C2H5SH) with an abundance of ∼3 נ10−10, and we also detect methyl mercaptan (CH3SH) with an abundance of ∼5 נ10−9. Abundance ratios were calculated for the three SH-bearing species and their OH analogs, revealing similar trends between alcohols and thiols with increasing complexity. Possible chemical routes for the interstellar synthesis of t-HC(O)SH, CH3SH, and C2H5SH are discussed, as well as the relevance of these compounds in the synthesis of prebiotic proteins in the primitive Earth.
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