Formation of bi-aryls via a domino palladium catalysis

Synthesis of bi-aryls via a domino Pd-catalyzed reaction of 1-(2-bromophenyl)-2-methylpropan-1-ones/(2-bromophenyl)(cyclohexyl)methanones is presented. The mechanism of the reaction is believed to proceed through a five membered palladacycle that combines with a second molecule of halo-arene to yield the bi-aryls. This method is quite successful to deliver highly sterically crowded bi-aryls with dense functionalities on the aromatic rings

A domino palladium catalysis: Synthesis of 7-methyl-5 H -dibenzo[ a, c ][7] annulen-5-ones

A domino Pd-catalyzed reaction of 1-(2-bromophenyl)ethanones for the synthesis of novel 7-methyl-5H-dibenzo[a,c][7]annulen-5-ones, a carbon core structure present in colchicinoid natural products, is presented. The reaction is proposed to proceed via intermolecular homobiaryl coupling and intramolecular aldol condensatio

Palladium-catalyzed selective α-arylation of ortho -bromoacetophenones

Synthesis of 1-(2-bromophenyl)-2-phenylethanones via an intermolecular Pd-catalyzed α-arylation of 1-(2-bromophenyl)ethanones is presented. The method relies on selective C-H activation (α-arylation) of relatively more reactive external iodo-arenes as coupling partners without affecting the bromo-substituent. Moreover, the scope and generality of the method has been well studied by employing the reaction with iodo-arenes as coupling partners bearing electron-withdrawing, simple, and electron-donating groups on the aromatic ring

Thermodynamic approach to the dewetting instability in ultrathin films

The fluid dynamics of the classical dewetting instability in ultrathin films is a non-linear process. However, the physical manifestation of the instability in terms of characteristic length and time scales can be described by a linearized form of the initial conditions of the films's dynamics. Alternately, the thermodynamic approach based on equating the rate of free energy decrease to the viscous dissipation [de Gennes, C. R. Acad. Paris.v298, 1984] can give similar information. Here we have evaluated dewetting in the presence of thermocapillary forces arising from a film-thickness (h) dependent temperature. Such a situation can be found during pulsed laser melting of ultrathin metal films where nanoscale effects lead to a local h-dependent temperature. The thermodynamic approach provides an analytical description of this thermocapillary dewetting. The results of this approach agree with those from linear theory and experimental observations provided the minimum value of viscous dissipation is equated to the rate of free energy decrease. The flow boundary condition that produces this minimum viscous dissipation is when the film-substrate tangential stress is zero. The physical implication of this finding is that the spontaneous dewetting instability follows the path of minimum rate of energy loss.Comment: 8 pages, 3 figures. Under revie

Was the Cosmic Web of Protogalactic Material Permeated by Lobes of Radio Galaxies During the Quasar Era?

Evidence for extended active lifetimes (> 10^8 yr) for radio galaxies implies that many large radio lobes were produced during the `quasar era', 1.5 < z < 3, when the comoving density of radio sources was 2 -- 3 dex higher than the present level. However, inverse Compton losses against the intense microwave background substantially reduce the ages and numbers of sources that are detected in flux-limited surveys. The realization that the galaxy forming material in those epochs was concentrated in filaments occupying a small fraction of the total volume then leads to the conclusion that radio lobes permeated much of the volume occupied by the protogalactic material during that era. The sustained overpressure in these extended lobes is likely to have played an important role in triggering the high inferred rate of galaxy formation at z > 1.5 and in the magnetization of the cosmic network of filaments.Comment: 5 pages, 0 figures, submitted to ApJ Letters; uses emulateapj

Entanglement Detection in the Stabilizer Formalism

We investigate how stabilizer theory can be used for constructing sufficient conditions for entanglement. First, we show how entanglement witnesses can be derived for a given state, provided some stabilizing operators of the state are known. These witnesses require only a small effort for an experimental implementation and are robust against noise. Second, we demonstrate that also nonlinear criteria based on uncertainty relations can be derived from stabilizing operators. These criteria can sometimes improve the witnesses by adding nonlinear correction terms. All our criteria detect states close to Greenberger-Horne-Zeilinger states, cluster and graph states. We show that similar ideas can be used to derive entanglement conditions for states which do not fit the stabilizer formalism, such as the three-qubit W state. We also discuss connections between the witnesses and some Bell inequalities.Comment: 15 pages including 2 figures, revtex4; typos corrected, presentation improved; to appear in PR

The IRAS 1-Jy Survey of Ultraluminous Infrared Galaxies: I. The sample and Luminosity Function

A complete flux-limited sample of 118 ultraluminous infrared galaxies (ULIGs) has been identified from the IRAS Faint Source Catalog (FSC). The selection criteria were a 60 micron flux density greater than 1 Jy in a region of the sky delta > -40 deg, |b| > 30 deg. All sources were subsequently reprocessed using coadded IRAS maps in order to obtain the best available flux estimates in all four IRAS wavelength bands. The maximum observed infrared luminosity is L_ir = 10^{12.90} L_{sun}, and the maximum redshift is z = 0.268. The luminosity function for ULIGs over the decade luminosity range L_ir = 10^{12} - 10^{13} L_{sun} can be approximated by a power law Phi (L) ~= L^{-2.35} Mpc^{-3} mag^{-1}. In the local Universe z < 0.1, the space density of ULIGs appears to be comparable to or slightly larger than that of optically selected QSOs at comparable bolometric luminosities. A maximum likelihood test suggests strong evolution for our sample; assuming density evolution proportional to (1+z)^{alpha} we find alpha = 7.6+/-3.2. Examination of the two-point correlation function shows a barely significant level of clustering, xi (r) = 1.6 +/- 1.2, on size scales r ~= 22 h^{-1} Mpc.Comment: 18 pages of text, 10 pages of figures 1 to 6, 6 pages of tables 1 to 3, ApJS accepte

東アジア共通農業政策の提案 : 自給率・関税率・財政負担・環境負荷

An efficient Pd-catalyzed domino reaction of α,α-dialkyl-(2- bromoaryl)methanols to 6,6-dialkyl-6H-benzo[c]chromenes is presented. Their formation can be explained via a five membered Pd(II)-cycle that efficiently involves a domino homocoupling with the second molecule, β-carbon cleavage, and finally intramolecular Buchwald-Hartwig cyclization. This domino process effectively involves breaking of five σ-bonds (2C-Br, 2O-H, and a C-C) and formation of two new σ-bonds (C-C and C-O). This mechanistic pathway is unprecedented and further illustrates the power of transition metal catalysi

Understanding BL Lac objects Structural & kinematic mode changes in the BL Lac object PKS 0735+178

Context. We present evidence that parsec-scale jets in BL Lac objects may be significantly distinct in kinematics from their counterparts in quasars. We argued this previously for the BL lac sources 1803+784 and 0716+714, report here a similar pattern for another well-known BL Lac object, PKS 0735+178, whose nuclear jet is found to exhibit kinematics atypical of quasars. Aims. A detailed study of the jet components' motion reveals that the standard AGN paradigm of apparent superluminal motion does not always describe the kinematics in BL Lac objects. We study 0735+178 here to augment and improve the understanding of the peculiar motions in the jets of BL Lac objects as a class. Methods. We analyzed 15 GHz VLBA (Very Long Baseline Array) observations (2cm/MOJAVE survey) performed at 23 epochs between 1995.27 and 2008.91. Results. We found a drastic structural mode change in the VLBI jet of 0735+178, between 2000.4 and 2001.8 when its twice sharply bent trajectory turned into a linear shape.We further found that this jet had undergone a similar transition sometime between December 1981 and June 1983. A mode change, occurring in the reverse direction (between mid-1992 and mid-1995) has already been reported in the literature. These structural mode changes are found to be reflected in changed kinematical behavior of the nuclear jet, manifested as an apparent superluminal motion and stationarity of the radio knots. In addition, we found the individual mode changes to correlate in time with the maxima in the optical light curve. The last two transitions occurred before a (modest) radio flare. The behavior of this pc-scale jet appears to favor a scenario involving non-ballistic motions of the radio knots, produced by the precession of a continuous jet within the ambient medium.Comment: Accepted for publication in A&A (Abstract reduced for astro-ph