Transport of degenerate electron-hole plasmas in Si and Ge

At low crystal temperatures, pulsed-laser excitation of Si and Ge can produce a mobile electron-hole plasma with a Fermi energy much larger than k_BT. The motion of this degenerate plasma away from the excitation surface depends intimately on its interactions with high-frequency phonons. Momentum damping and phonon-wind forces are principal factors which determine the plasma motion on nanosecond and longer time scales. A variety of luminescence and heat-pulse experiments are reviewed here which characterize the transport behavior of photo-generated electron-hole plasma in these indirect-gap semiconductors.     

Channeling of acoustic phonons in silicon: the polarization dependence in elastic scattering

Ballistic phonon flux in crystals at low temperatures is highly directional due to phonon focusing. In this paper, a phonon-imaging experiment is reported which shows that scattered phonons, too, can retain a highly directed flux. Basically, the combination of phonon focusing and the elastic-scattering selection rule act to channel phonons along the ballistic focusing directions. Together with Monte Carlo simulations, the experiments show that the scattered phonon flux is indeed due to elastic scattering processes, which depend on the polarizations of the scattering phonons. Isotropic scattering is inconsistent with the data. The experimental technique shows promise for quantifying the microscopic scattering processes and revealing the dynamics of a phonon hot spot.     

A new synthesis of aryl hetaryl ketones via SRN1 reactions of halogenated heterocycles with potassiophenylacetonitrile followed by phase-transfer catalyzed decyanation

Reaction of halogenated pyridines, quinolines, pyrimidines, and pyrazines with potassiophenylacetonitrile ( 5 ) in liquid ammonia under near-uv irradiation affords secondary nitriles, which then undergo oxidative decyanation under phase-transfer catalytic conditions to afford aryl hetaryl ketones in excellent yields.     

Separate Mott and liquid-gas transitions in a coulomb gas: Photoexcited germanium

The phase diagram of photoexcited electron-hole (e-h) pairs, which are confined to a strain well in stressed Ge, is investigated via measurements of energy spectra and spatial distributions of e-h recombination luminescence. Above a triple-point temperature of 3.7 ± 0.2K, a Mott (metal-insulator) transition is observed at lower densities than the liquid-gas (LG) transition. The measured critical temperatures of the Mott and LG transitions are 6.5 ± 0.5K and 4.5 ± 0.2K respectively.     

A characterization of Lévy probability distribution functions on Euclidean spaces

In 1937, Paul Lévy proved two theorems that characterize one-dimensional distribution functions of class L. In 1972, Urbanik generalized Lévy's first theorem. In this note, we generalize Lévy's second theorem and obtain a new characterization of Lévy probability distribution functions on Euclidean spaces. This result is used to obtain a new characterization of operator stable distribution functions on Euclidean spaces and to show that symmetric Lévy distribution functions on Euclidean spaces need not be symmetric unimodal.     

Synthesis and antibiofilm activity of a second-generation reverse-amide oroidin library: a structure-activity relationship study

A second-generation library of 2-aminoimidazole-based derivatives incorporating a "reversed amide" (RA) motif in comparison to the marine natural product oroidin were synthesized and subsequently assayed for antibiofilm activity against the medically relevant Gram-negative proteobacteria P. aeruginosa and A. baumannii. Most notably, an in-depth activity profile is reported for the most active subclass of derivatives that bear linear aliphatic chains off the amide bond. Additionally, further structural modifications of the core template, such as removal of the amide bond or substitution with a triazole isostere, resulted in the discovery of analogues with antibiofilm activities that varied with respect to their inhibition and dispersal properties of P. aeruginosa and A. baumannii biofilms.     

Synthesis,asymmetric aldol reactions,and x‐ray crystallography of some oxadiazinanone derivatives

A series of N₄‐substituted oxadiazinanones have been synthesized from (1R,2S)‐norephedrine by a process of either reductive alkylation or arylation, N‐nitrosation, reduction and cyclization. These derivatives (R = ‐CH₂Ph, ‐CH₂C(CH₃)₃, ‐cyclo‐C₆H₁₁, ‐C₆H₅) have been acylated with propanoyl chloride and employed in the asymmetric Aldol reaction. The observed diastereoselectivities for the formation of the “non‐Evans” syn‐adduct ranged from 88:12 to 99:1. The hydrolysis of the Aldol adducts varied with the nature of the nitrogen substituent.     

Quantification of Lysine Acetylation and Succinylation Stoichiometry in Proteins Using Mass Spectrometric Data-Independent Acquisitions (SWATH)

Post-translational modification of lysine residues by N_?-acylation is an important regulator of protein function. Many large-scale protein acylation studies have assessed relative changes of lysine acylation sites after antibody enrichment using mass spectrometry-based proteomics. Although relative acylation fold-changes are important, this does not reveal site occupancy, or stoichiometry, of individual modification sites, which is critical to understand functional consequences. Recently, methods for determining lysine acetylation stoichiometry have been proposed based on ratiometric analysis of endogenous levels to those introduced after quantitative per-acetylation of proteins using stable isotope-labeled acetic anhydride. However, in our hands, we find that these methods can overestimate acetylation stoichiometries because of signal interferences when endogenous levels of acylation are very low, which is especially problematic when using MS1 scans for quantification. In this study, we sought to improve the accuracy of determining acylation stoichiometry using data-independent acquisition (DIA). Specifically, we use SWATH acquisition to comprehensively collect both precursor and fragment ion intensity data. The use of fragment ions for stoichiometry quantification not only reduces interferences but also allows for determination of site-level stoichiometry from peptides with multiple lysine residues. We also demonstrate the novel extension of this method to measurements of succinylation stoichiometry using deuterium-labeled succinic anhydride. Proof of principle SWATH acquisition studies were first performed using bovine serum albumin for both acetylation and succinylation occupancy measurements, followed by the analysis of more complex samples of E. coli cell lysates. Although overall site occupancy was low (<1%), some proteins contained lysines with relatively high acetylation occupancy.

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Fully ferrocenated hexanethiolate monolayer-protected gold clusters

The synthesis and compositional analysis of four different gold clusters with protecting monolayers comprised solely of ferrocene hexanethiolate ligands is described. The gold nanoparticles have average core diameters of 1.4, 1.6, 2.0, and 2.2 nm with estimated average atom counts of 55, 140, 225, and 314 Au atoms and average monolayer coverages of 37, 39, 43, and 58 ferrocenated ligands, respectively. The data show unequivocally that the number of ferrocene hexanethiolate ligands bound to each core size is constrained by the steric requirements of the ferrocene head group; the ligand numbers are significantly smaller than those for hexanethiolate ligands bonded to analogous-sized Au cores. Voltammetry of dilute solutions of these nanoparticles shows a large ferrocene oxidation wave and, at more negative potentials, smaller one-electron waves for the quantized double-layer charging of the Au cores. Together, the ferrocenes and core of the ferrocenated Au314 nanoparticle deliver 60 electrons at the ferrocene oxidation potential, which amounts to a very large volume charge capacity, 7x10(9) C/m3, for an undiluted nanoparticle sample.     

Mild conditions for the synthesis of functionalized pyrrolidines via Pd-catalyzed carboamination reactions

[reaction: see text] The palladium-catalyzed carboamination of N-protected gamma-aminoalkenes with aryl bromides and triflates has been achieved under new, mild reaction conditions using the weak base Cs(2)CO(3) in dioxane solvent. These reactions tolerate a wide variety of functional groups, including enolizable ketones, nitro groups, methyl esters, and acetates, which are not compatible with previously described conditions.