44,759 research outputs found
P. D. Grogan and H. J. Hindle
No full text"SX16247 Pte. P. D. Grogan
SX15874 Pte. H. J. Hindle
10/48 Bn. A.I.F. 1943 -1943"SX16247 Private P. D. Grogan.
SX15874 Private H. J. Hindle.
10/48 Battalion, Australian Imperial Forces 1942 - 1943
A 2 h periodic variation in the low-mass X-ray binary Ser X-1
No full textSpectroscopy of the low-mass X-ray binary Ser X-1 using the Gran Telescopio Canarias have revealed a ?2 h periodic variability that is present in the three strongest emission lines. We tentatively interpret this variability as due to orbital motion, making it the first indication of the orbital period of Ser X-1. Together with the fact that the emission lines are remarkably narrow, but still resolved, we show that a main-sequence K dwarf together with a canonical 1.4 M? neutron star gives a good description of the system. In this scenario, the most likely place for the emission lines to arise is the accretion disc, instead of a localized region in the binary (such as the irradiated surface or the stream-impact point), and their narrowness is due instead to the low inclination (?10°) of Ser X-1
CONTINUOUS MONITORING OF PHOTOLYSIS PRODUCTS BY THZ SPECTROSCOPY
No full textWe demonstrate the potential of THz spectroscopy to monitor the real time evolution of the gas phase concentration of photolysis products and determine the kinetic reaction rate constantfootnote{H. M. Pickett and T. L. Boyd, Chem. Phys. Lett, Vol 58, 446-449, (1978) }. In the primary work, we have chosen to examine the photolysis of formaldehyde (HCO) footnote{S. Eliet, A. Cuisset, M Guinet, F. Hindle, G. Mouret, R. Bocquet, and J. Demaison, Journal of Molecular Spectroscopy, Vol 279, 12-15 (2012). }. Exposure of HCO to a UVB light (250 to 360 nm) in a single pass of 135 cm length cell leads to decomposition via two mechanisms: the radical channel with production of HCO and the molecular channel with production of CO. A commercial THz source footnote{G. Mouret, M. Guinet, A. Cuisset, L. Croiz, S. Eliet, R. Bocquet and F. Hindle, Sensors Journal. IEEE, Vol 13, 133-138, (2013)} (frequency multiplication chain) operating in the range 600-900 GHz was used to detect and quantify the various chemical species as a function of time. Monitoring the concentrations of CO and HCO via rotational transitions, allowed the kinetic rate of HCO consummation to be obtained, and an estimation of the rate constants for both the molecular and radical photolysis mechanisms.
We have modified our experimental setup to increase the sensitivity of the spectrometer and changed sample preparation protocol specifically to quantify the HCO concentration. Acetaldehyde was used as the precursor for photolysis by UVC resulting in the decompositon mechanism can be described by:
Frequency modulation of the source and Zeeman modulation is used to achieve the high sensitivity required. Particular attention has been paid to the mercury photosensitization effect that allowed us to increase the HCO production enabling quantification of the monitored radical. We quantify the HCO radical and start a spectroscopic study of the line positions.Made available in DSpace on 2016-01-05T20:03:51Z (GMT). No. of bitstreams: 3
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Impaired visuospatial transformation but intact sequence processing in parkinson disease
No full textObjective: we examined whether visuospatial deficits in Parkinson disease (PD) can be explained by a domain-general, nonspatial impairment in the sequencing or serial chaining of mental operations. Background: PD has been shown to be associated with impaired visuospatial processing, but the mechanisms of this impairment remain unclear. Methods: thirteen patients with PD and 20 age-matched, neu-rologically normal controls performed a visuospatial grid navigation task requiring sequential spatial transformations. The participants also performed a control task of serial number subtraction designed to assess their nonvisuospatial sequencing. The tasks were matched in structure and difficulty. Results: The patients were impaired on the visuospatial task but not in serial number subtraction. This finding suggests that vi-suospatial processing impairments in PD do not derive from a general impairment affecting sequencing or serial chaining. Conclusions: we argue that visuospatial deficits in PD result from impairments to spatial transformation routines involved in the computation of mappings between spatial locations. These routines are mediated by dopaminergic pathways linking the basal ganglia, prefrontal cortex, supplementary motor area, and parietal cortex.</p
Rearrangement of alkylchlorocarbenes: 1,2-H shift in free carbene, carbene-olefin complex, and excited states of carbene precursors
No full textPhotolysis of alkylchlorodiazirines (1) in the presence of olefins gives a cyclopropane (3) by addition of the generated carbene to the olefin and a vinyl chloride derivative (2) resulting from a 1,2-H shift rearrangement. This rearrangement may occur either in the carbene or in some excited state, precursor of the carbene (RIES mechanism), or in a ''carbene + olefin complex'' on the way to the formation of 3 (COC mechanism). Results obtained by time-resolved photoacoustic calorimetry as well as by thermolysis and photolysis of ClCH2C(N-2)Cl and CH3(CH2)(2)C(N-2)Cl in the presence of tetramethylethylene clearly indicate that both the RIES and COC mechanisms play a role but with efficiencies which greatly depend on the nature of the diazirine. Reexamination of the results previously obtained with benzylchlorodiazirines indicates that, for this class of diazirines, the RIES mechanism is temperature dependent and has a very low efficiency at room temperature and below, whereas the nonlinearity of the plots [3]/[2] vs [olefin] is mainly due to the COC mechanism.PT: J; CR: BIGOT B, 1978, J AM CHEM SOC, V100, P8575 CHANG KT, 1979, J AM CHEM SOC, V101, P5082 FREY HM, 1966, ADV PHOTOCHEM, V4, P225 GANZER GA, 1986, J AM CHEM SOC, V108, P1517 GRAHAM WH, 1965, J AM CHEM SOC, V87, P4396 HEIHOFF K, 1987, BIOCHEMISTRY-US, V22, P1422 HOUK KN, 1984, J AM CHEM SOC, V106, P4291 HOUK KN, 1984, J AM CHEM SOC, V106, P4293 JACKSON JE, 1994, ADV CARBENE CHEM, V1 KANABUSKAMINSKA JM, 1987, J AM CHEM SOC, V109, P5267 LAVILLA JA, 1989, J AM CHEM SOC, V111, P6877 LAVILLA JA, 1989, J AM CHEM SOC, V111, P712 LAVILLA JA, 1990, TETRAHEDRON LETT, V31, P5109 LIU MTH, 1987, J ORG CHEM, V52, P4223 LIU MTH, 1989, J CHEM SOC CHEM COMM, P12 LIU MTH, 1990, J AM CHEM SOC, V112, P3915 MODARELLI DA, 1991, J AM CHEM SOC, V113, P8985 MODARELLI DA, 1992, J AM CHEM SOC, V114, P7034 MOSS RA, 1993, J CHEM SOC CHEM COMM, P1597 MOSS RA, 1994, ADV CARBENE CHEM, V1 MULDER P, 1988, J AM CHEM SOC, V110, P4090 MULLERREMMERS PL, 1985, J AM CHEM SOC, V107, P7275 NI T, 1989, J AM CHEM SOC, V111, P457 NICKON A, 1993, ACCOUNTS CHEM RES, V26, P84 RUDZKI JE, 1985, J AM CHEM SOC, V107, P7849 SKELL PS, 1969, J AM CHEM SOC, V91, P7131 TOMIOKA H, 1984, J AM CHEM SOC, V106, P454 TURRO NJ, 1982, J AM CHEM SOC, V104, P1754 WARNER PM, 1984, TETRAHEDRON LETT, V25, P4211 WESTRICK JA, 1987, BIOCHEMISTRY-US, V26, P8313 WHITE WR, 1992, J ORG CHEM, V57, P2841 WIERLACHER S, 1993, J AM CHEM SOC, V115, P8943 YAMAMOTO N, 1994, J AM CHEM SOC, V116, P2064; NR: 33; TC: 30; J9: J AMER CHEM SOC; PG: 9; GA: UG695Source type: Electronic(1
Catalytic P-H activation by Ti and Zr catalysts
No full textCatalytic dehydrocoupling of phosphines was investigated using the anionic zirconocene trihydride salts [Cp*Zr-2(mu-H)(3)Li](3) (1a) or [Cp*Zr-2(mu-H)(3)K(thf)(4)] (1b), and the metallocycles [CpTi(NPtBu3)(CH2)(4)] (6) and [Cp*M(NPtBu3)(CH2)(4)] (M = Ti 20, Zr 21) as catalyst precursors. Dehydrocoupling of primary phosphines RPH2 (R = Ph, C6H2Me3, Cy, C10H7) gave both dehydrocoupled dimers RP(H)P(H)R or cyclic oligophosphines (RP)(n) (n = 4, 5) while reaction of tBu(3)C(6)H(2)PH(2) gave the phosphaindoline tBu(2)(Me2CCH2)C6H2PH (9). Stoichiometric reactions of these catalyst precursors with primary phosphines afforded [Cp*Zr-2((PR)(2))H][K(thf)(4)] (R = Ph 2, Cy 3, C6H2Me3 4), [Cp*Zr-2((PPh)(3))H] [K(thf)(4)] (5), [CpTi(NPtBu3)(PPh)(3)] (7) and [CpTi(NPtBu3)(mu-PHPh)](2) (8), while reaction of 6 with (C(6)H(2)tBu3)PH2 in the presence of PMe3 afforded [CpTi(NPtBu3)(PMe3)(p(C(6)H(2)tBu(3))] (10). The secondary phosphines Ph2PH and (PhHPCH2)(2)CH2 also undergo dehydrocoupling affording (Ph2P)(2) and (PhPCH2)(2)CH2. The bisphosphines (CH2PH2)(2) and C6H4(PH2)(2) are dehydrocoupled to give (PCH2CH2PH)(2) (12) and (C6H4P(PH))(2) (13) while prolonged reaction of 13 gave (C6H4P2)(8) (14). The analogous bisphosphine Me2C6H4(PH)(2) (17) was prepared and dehydrocoupling catalysis afforded (Me2C6H2P(PH))(2) (18) and subsequently [(Me2C6H2P2)(2)(mu-Me2C6H2P2)](2) (19). Stoichiometric reactions with these bisphosphines gave [Cp*Zr-2(H)(PH)(2)C6H4] [Li(thf)(4)] (22), [Cp*Ti(NPtBu3)(PH)(2)C6H4](2) (23) and [Cp*Ti(NPtBu3)(PH)(2)C6H4] (24). Mechanistic implications are discussed.PT: J; CR: ALBRAND JP, 1976, J CHEM SOC CHEM COMM, P876 ANSELME JP, 1969, TETRAHEDRON, V25, P855 BASULI F, 2003, J AM CHEM SOC, V125, P10170 BAUDLER M, 1976, Z NATURFORSCH B, V31, P558 BAUDLER M, 1978, CHEM BER, V111, P1210 BAUDLER M, 1978, CHEM BER, V111, P1217 BAUDLER M, 1983, CHEM BER, V116, P2711 BAUDLER M, 1984, Z NATURFORSCH B, V39, P438 BAZAN GC, 1991, J AM CHEM SOC, V113, P6899 BOHM VPW, 2001, ANGEW CHEM, V113, P4832 CHAUVIN Y, 1971, MAKROMOL CHEM, V141, P161 COREY JY, 2004, ADV ORGANOMET CHEM, V51, P1 COURET C, 1986, ORGANOMETALLICS, V5, P113 COWLEY AH, 1984, TETRAHEDRON LETT, V25, P2125 COWLEY AH, 1990, INORG SYNTH, V27, P235 CROMER DT, 1974, INT TABLES CRYSTALLO, V4, P71 ETKIN N, 1997, J AM CHEM SOC, V119, P11420 ETKIN N, 1997, J AM CHEM SOC, V119, P2954 ETKIN N, 1997, ORGANOMETALLICS, V16, P3504 FEHLNER TP, 1992, INORGANOMETALLLICS FERMIN MC, 1995, J AM CHEM SOC, V117, P12645 FERMIN MC, 1995, ORGANOMETALLICS, V14, P4247 FU GC, 1993, J AM CHEM SOC, V115, P9856 GAUVIN F, 1998, ADV ORGANOMET CHEM, V42, P363 GRAHAM TW, 2004, ORGANOMETALLICS, V23, P3309 GRUBBS RH, 1972, J AM CHEM SOC, V94, P2538 GRUBBS RH, 2003, HDB METATHESIS HEY E, 1988, CHEM BER, V121, P561 HEY E, 1989, J ORGANOMET CHEM, V378, P375 HO JW, 1991, ORGANOMETALLICS, V10, P3001 HO JW, 1994, INORG CHEM, V33, P865 HOFFMAN PR, 1975, INORG CHEM, V14, P1997 HOSKIN AJ, 2001, ANGEW CHEM, V113, P1917 HOU ZM, 1993, ORGANOMETALLICS, V12, P3158 INAGAKI Y, 1980, B CHEM SOC JPN, V53, P205 ISSLEIB K, 1972, ANGEW CHEM, V84, P582 ISSLEIB K, 1987, J ORGANOMET CHEM, V330, P17 JACOBSEN EN, 1988, J AM CHEM SOC, V110, P1968 KATSUKI T, 1980, J AM CHEM SOC, V102, P5974 KAUFFMANN T, 1984, TETRAHEDRON LETT, V25, P1963 KAUFFMANN T, 1985, CHEM BER, V118, P1022 KITAMURA M, 1988, J AM CHEM SOC, V110, P629 KNOWLES WS, 1983, ACCOUNTS CHEM RES, V16, P106 KOEPF H, 1981, CHEM BER, V114, P2731 KOHLER EP, 1935, J AM CHEM SOC, V57, P367 KYBA EP, 1983, ORGANOMETALLICS, V2, P1877 MILLER AR, 1976, J AM CHEM SOC, V98, P1860 MILLER SJ, 1996, J AM CHEM SOC, V118, P9606 MIYASHITA A, 1980, J AM CHEM SOC, V102, P7932 MURDZEK JS, 1987, ORGANOMETALLICS, V6, P1373 NGUYEN ST, 1992, J AM CHEM SOC, V114, P3974 NGUYEN ST, 1993, J AM CHEM SOC, V115, P9858 NOVAK BM, 1988, J AM CHEM SOC, V110, P960 OHKUMA T, 1995, J AM CHEM SOC, V117, P2675 OHTA T, 1988, INORG CHEM, V27, P566 OSHIKAWA T, 1985, CHEM IND-LONDON, P126 ROCKLAGE SM, 1981, J AM CHEM SOC, V103, P1440 SCHOLL M, 1999, TETRAHEDRON LETT, V40, P2247 SCHROCK RR, 1974, J AM CHEM SOC, V96, P6796 SCHROCK RR, 1980, J MOL CATAL, V8, P73 SCHROCK RR, 1988, J MOL CATAL, V46, P243 SCHROCK RR, 1990, J AM CHEM SOC, V112, P3875 SCHWAB P, 1995, ANGEW CHEM INT EDIT, V34, P2039 SCHWAB P, 1995, ANGEW CHEM, V107, P2179 SCHWAB P, 1996, J AM CHEM SOC, V118, P100 SENDERIKHIN AI, 1988, ZH OBSHCH KHIM+, V58, P1662 SENDERIKHIN AI, 1989, ZH OBSHCH KHIM+, V59, P2141 SEYFERTH D, 1969, J ORG CHEM, V34, P1483 SHELDRICK GM, 2000, SHELXTL SHU RH, 1998, J AM CHEM SOC, V120, P12988 SMIT CN, 1983, TETRAHEDRON LETT, V24, P2031 SOUFFLET JP, 1973, CR ACAD SCI C CHIM, V276, P169 STEPHAN DW, 2000, ANGEW CHEM, V112, P322 STEPHAN DW, 2005, ORGANOMETALLICS, V24, P2548 STRADIOTTO M, 2001, HELV CHIM ACTA, V84, P2958 TILLEY TD, 1990, COMMENTS INORG CHEM, V10, P37 TILLEY TD, 1993, ACCOUNTS CHEM RES, V26, P22 TVERDOMED SN, 2003, RUSS J GEN CHEM+, V73, P319 VANDENWINKEL Y, 1991, J ORGANOMET CHEM, V405, P183 WATERMAN R, 2006, ANGEW CHEM INT EDIT, V45, P2926 WATERMAN R, 2006, ANGEW CHEM, V118, P2992 WEAST RC, 1974, HDB CHEM PHYS, P2436 WOOD CD, 1979, J AM CHEM SOC, V101, P3210 WU Z, 1995, J AM CHEM SOC, V117, P5503 XIN SX, 1997, J AM CHEM SOC, V119, P5307; NR: 85; TC: 0; J9: CHEM-EUR J; PG: 12; GA: 113PJSource type: Electronic(1
Evidence for the decay B0→J/ψω and measurement of the relative branching fractions of meson decays to J/ψη and J/ψη′
No full textFirst evidence of the B 0 → J / ψ ω decay is found and the B s 0 → J / ψ η and B s 0 → J / ψ η ′ decays are studied using a dataset corresponding to an integrated luminosity of 1.0 fb -1 collected by the LHCb experiment in proton-proton collisions at a centre-of-mass energy of sqrt(s) = 7 TeV. The branching fractions of these decays are measured relative to that of the B 0 → J / ψ ρ 0 decay:frac(B (B 0 → J / ψ ω), B (B 0 → J / ψ ρ 0)) = 0.89 ± 0.19 (stat) - 0.13 + 0.07 (syst),frac(B (B s 0 → J / ψ η), B (B 0 → J / ψ ρ 0)) = 14.0 ± 1.2 (stat) - 1.5 + 1.1 (syst) - 1.0 + 1.1 (frac(f d, f s)),frac(B (B s 0 → J / ψ η ′), B (B 0 → J / ψ ρ 0)) = 12.7 ± 1.1 (stat) - 1.3 + 0.5 (syst) - 0.9 + 1.0 (frac(f d, f s)), where the last uncertainty is due to the knowledge of f d / f s, the ratio of b-quark hadronization factors that accounts for the different production rate of B 0 and B s 0 mesons. The ratio of the branching fractions of B s 0 → J / ψ η ′ and B s 0 → J / ψ η decays is measured to befrac(B (B s 0 → J / ψ η ′), B (B s 0 → J / ψ η)) = 0.90 ± 0.09 (stat) - 0.02 + 0.06 (syst)
Molecules Probed With A Slow Chirped-pulse Excitation: Analytical Model Of The Free-induction-decay Signal
No full textA chirped pulse experiment is a powerful means to rapidly obtain an high-resolution spectrum of molecules on a large frequency band. The theoretical paper from McGurk \textit{et al.}\footnote{J. C. McGurk, T. G. Schmalz, and W. H. Flygare, J. Chem. Phys. \textbf{60}, 4181 (1974).} is the main reference paper to describe the polarization induced by fast chirped pulses generated with microwave sources.
We built a chirped pulse spectrometer operating at 200 GHz for astrophysical applications.\footnote{F. Hindle, C. Bray, K. Hickson, D. Fontanari, M. Mouelhi, A. Cuisset, G. Mouret and R. Bocquet, J. Infrared Millim. Te. \textbf{39}, 105 (2018).} It works in the millimeter domain with slower chirped pulses. In such a situation, the paper of McGurk \textit{et al.} does not capture all the physics involved in the polarization step. In particular, the intensity of a molecular transition is dependent on its temporal position inside the chirped pulse, as discovered by Abeysekera et al.\footnote{C. Abeysekera, L. N. Zack, G. B. Park, B. Joalland, J. M. Oldham, K. Prozument, N. M. Ariyasingha, I. R. Sims, R. W. Field, and A. G. Suits, J. Chem. Phys. \textbf{141}, 214203 (2014).}
A theoretical study of the polarization of molecules subjected to a slow chirped pulse is presented for three typical cases: the cell, the uniform flow and the molecular beam. Analytical expressions are proposed alongside the numerical solution and are used in the expression of the free induction decay signal. We test the analytical expression on the rotational emission spectra of OCS molecules. In the thermalized case, a relation between the pulse duration, the line position in the chirped pulse, and the signal amplitude is proposed to correct the line intensities.\footnote{D. Fontanari, C. Bray, G. Dhont, G. Mouret, A. Cuisset, F. Hindle, R. Bocquet, and K. M. Hickson, Phys. Rev. A \textbf{100}, 043407 (2019).}Made available in DSpace on 2021-09-24T21:08:56Z (GMT). No. of bitstreams: 2
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Benzylchlorocarbene: origins of Arrhenius curvature in the kinetics of the 1,2-H shift rearrangement
No full textBenzylchlorocarbene (1, BCC) was generated photochemically from benzylchlorodiazirine (2) in isooctane, methylcyclohexane (MCH), and tetrachloroethane (TCE) at temperatures from similar to 30 to -75 degrees C. At -70 degrees C in isooctane, the identified products included Z/E-beta-chlorostyrenes 4 (46.6%), alpha-chlorostyrene 5 (2.4%), 1,1-dichloro-2-phenylethane 6 (1.9%), a BCC-isooctane insertion product 8 (5.5%), carbene dimers 9 (3.8%), and azine 3 (30%). The significant incursion of intermolecular products 3, 8, and 9 implies that laser flash photolytic (LFP) kinetic data for the decay of BCC obtained at low temperature is biased and should not be employed in Arrhenius analyses. Accordingly, previously obtained curved Arrhenius correlations for BCC do not necessarily implicate quantum mechanical tunneling (QMT) in the 1,2-H shift rearrangement of BCC to 4. Similarly in MCH, where BCC affords a solvent insertion product in similar to 44-53% yield, the curved Arrhenius correlation (Figure 1) cannot be readily interpreted. In polar solvents such as TCE, clean H-shift reactions of BCC are obtained even at -71 degrees C; an Arrhenius correlation of LFP kinetic data is linear from 3 to -71 degrees C (Figure 2), affording E-a = 3.2 kcal mol(-1) and log A = 10.0 s(-1). Therefore, QMT does not appear to play a major role in the 1,2-H shift rearrangement of BCC at ambient or near ambient temperature in solution.PT: J; CR: BONNEAU R, 1996, J AM CHEM SOC, V118, P3829 DEAN JA, 1992, LANGES HDB CHEM DIX EJ, 1993, J AM CHEM SOC, V115, P10424 DOX AW, 1941, ORG SYNTH, V1, P5 GRAHAM WH, 1965, J AM CHEM SOC, V87, P4396 ISAACS NS, 1995, PHYSICAL ORGANIC CHE, P304 JACKSON JE, 1988, J AM CHEM SOC, V110, P5595 KAZANIS S, 1991, J PHYS CHEM-US, V95, P4430 KEATING AE, 1997, COMMUNICATION 0804 LAVILLA JA, 1989, J AM CHEM SOC, V111, P6877 LAVILLA JA, 1990, TETRAHEDRON LETT, V31, P5109 LIU MTH, 1984, TETRAHEDRON, V40, P887 LIU MTH, 1985, CHEM COMMUN, P982 LIU MTH, 1985, J ORG CHEM, V50, P3218 LIU MTH, 1990, J AM CHEM SOC, V112, P3915 LIU MTH, 1992, J AM CHEM SOC, V114, P3604 LIU MTH, 1992, J PHOTOCH PHOTOBIO A, V63, P115 LIU MTH, 1994, ACCOUNTS CHEM RES, V27, P287 LIU MTH, 1994, J PHOTOCH PHOTOBIO A, V84, P133 MODARELLI DA, 1992, J AM CHEM SOC, V114, P7034 MODARELLI DA, 1993, J AM CHEM SOC, V115, P470 MOSS RA, 1987, J AM CHEM SOC, V109, P4341 MOSS RA, 1990, J AM CHEM SOC, V112, P1638 MOSS RA, 1994, ADV CARBENE CHEM, V1, P59 MOSS RA, 1996, J AM CHEM SOC, V118, P12588 MOSS RA, 1997, CHEM COMMUN 0321, P617 MOSS RA, 1997, TETRAHEDRON LETT, V38, P7049 STORER JW, 1993, J AM CHEM SOC, V115, P10426 SUGIYAMA MH, 1992, J AM CHEM SOC, V114, P966 TOMIOKA H, 1984, J AM CHEM SOC, V106, P454 WHITE WR, 1992, J ORG CHEM, V57, P2841 WIERLACHER S, 1993, J AM CHEM SOC, V115, P8943 YEN VQ, 1962, ANN CHIM, V7, P785; NR: 33; TC: 8; J9: J ORG CHEM; PG: 7; GA: ZM109Source type: Electronic(1
Transformation of the endostyle of the anadromous sea lamprey, Petromyzon-marinus L, during metamorphosis .2. Electron-microscopy
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