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811.
812.
A family of iron(II) complexes that coordinate dinitrogen, diazene, hydrazine, and ammonia are presented. This series of complexes is unusual in that the complexes within it feature a common auxiliary ligand set and differ only by virtue of the nitrogenous N(x)H(y) ligand that occupies the sixth binding site. The ability of an iron center to bind N(2), N(2)H(2), N(2)H(4), and NH(3) is important to establish in the context of evaluating catalytic N(2) reduction schemes that invoke these nitrogenous species. Such a scenario has been proposed as an iron-mediated, alternating reduction scheme within the cofactor of nitrogenase enzymes. 相似文献
813.
Little JL Cleven CD Brown SD 《Journal of the American Society for Mass Spectrometry》2011,22(2):348-359
In many cases, an unknown to an investigator is actually known in the chemical literature. We refer to these types of compounds
as “known unknowns.” Chemical Abstracts Service (CAS) Registry is a particularly good source of these substances as it contains
over 54 million entries. Accurate mass measurements can be used to query the CAS Registry by either molecular formulae or
average molecular weights. Searching the database by the web-based version of SciFinder is the preferred approach when molecular
formulae are available. However, if a definitive molecular formula cannot be ascertained, searching the database with STN
Express by average molecular weights is a viable alternative. The results from either approach are refined by employing the
number of associated references or minimal sample history as orthogonal filters. These approaches were shown to be successful
in identifying “known unknowns” noted in LC-MS and even GC-MS analyses in our laboratory. In addition, they were demonstrated
in the identification of a variety of compounds of interest to others. 相似文献
814.
Curtis P. Rinsland Ming Luo Peter F. Bernath Linda Chiou 《Journal of Quantitative Spectroscopy & Radiative Transfer》2008,109(10):1931-1942
High spectral resolution Fourier transform spectrometer (FTS) measurements of tropospheric carbon monoxide (CO) distributions show mixing ratios over Indonesia during October 2006 of ∼200 ppbv (10−9 per unit volume) in the middle troposphere. The elevated emissions were caused by intense and widespread Indonesian peat and forest fire emissions elevated compared to other years by the impact of a moderate El Niño/Soutern Oscillation (ENSO) event, which delayed that year's monsoon season and produced very dry conditions. Moderate resolution imaging spectrometer (MODIS) fire counts, atmospheric chemistry experiment (ACE) measurements of elevated mixing ratios of fire emission products and near infrared extinction, and back trajectory calculations for a sample measurement location near the time of maximum emissions provide additional evidence that the elevated 2006 emissions resulted primarily from the Indonesia fires. Lower CO mixing ratios measured by ACE and fewer MODIS fire counts in Indonesia during October 2005 indicate lower emissions than during 2006. Coincident profiles from the ACE agree within the uncertainties with those from the tropospheric emission spectrometer (TES) for pressure ranges and time periods with good TES sensitivity after accounting for its lower vertical sensitivity compared with the ACE FTS. 相似文献
815.
We demonstrate the preservation of entanglement of an energy-time entangled biphoton through a slow light medium. Using the D(1) and D(2) fine structure resonances of Rubidium, we delay one photon of the 1.5 THz biphoton by approximately 1.3 correlation lengths and measure the fourth order correlation fringes. After the group delay the fringe visibility is reduced from 97.0+/-4.4% to 80.0+/-4.8%, but is still sufficient to violate a Bell inequality. We show that temporal broadening is the primary mechanism for reducing the fringe visibility and that smaller bandwidths lead to greatly reduced broadening. 相似文献
816.
Miles?L.?Morgan Alexander?Holder Dan?J.?Curtis Davide?DeganelloEmail authorView authors OrcID profile 《Rheologica Acta》2018,57(2):105-112
Model elastic inks were formulated, rheologically characterised in shear and extension, and printed via flexography to assess the impact of ink elasticity on print uniformity. Flexography is a roll-to-roll printing process with great potential in the mass production of printed electronics for which understanding layer uniformity and the influence of rheology is of critical importance. A new set of flexo-printable Boger fluids was formulated by blending polyvinyl alcohol and high molecular weight polyacrylamide to provide inks of varying elasticity. During print trials, the phenomenon of viscous fingering was observed in all prints, with those of the Newtonian ink exhibiting a continuous striping in the printing direction. Increasing elasticity significantly influenced this continuity, disrupting it and leading to a quantifiable decrease in the overall relative size of the printed finger features. As such, ink elasticity was seen to have a profound effect on flexographic printing uniformity, showing the rheological tuning of inks may be a route to obtaining specific printed features. 相似文献
817.
818.
Organic materials with Inverted Singlet-Triplet (INVEST) gaps are interesting for their potential use in photocatalytic small molecule transformations such as the entirely solar-driven water splitting reaction. However, only a few INVEST emitters are thermodynamically able to split water requiring a first singlet excited dark state, S1, above 1.27 or 1.76 eV, and absorption near solar the maximum, 2.57 eV. These requirements and the INVEST character are key for achieving a long-lived photocatalyst for water splitting. The only known INVEST emitters that conform to these criteria are large triangular boron carbon nitrides with unknown synthesis pathways. Using ADC(2), a quantum-mechanical method, we describe three triangulenes. 3 a is a cyano azacyclopenta[cd]phenalene derivative while 3 b and 3 c are cycl[3.3.3]azine derivatives. 3 b has a previously undescribed disulfide bridge. Overall, 3 a fulfills requirements for photocatalytic four-electron reduction of water while the S1 states of 3 b and 3 c are likely slightly low for the two-electron reduction process. By analyzing impacts of ligands, we find that there are guidelines describing how S1-S5 energies and oscillator strengths, T1 energies, and ΔES1T1 gaps are affected, requiring deep-learning algorithms for which studies will be presented by us in due time. The impact of ground-state geometries, solvation effects, as well as reduced-cost ADC(2) algorithms on our findings are also discussed. 相似文献
819.
820.