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831.
Harrison N Mielke CH Christianson AD Brooks JS Tokumoto M 《Physical review letters》2001,86(8):1586-1589
ac susceptibility measurements of the charge-density-wave (CDW) compound alpha-(BEDT-TTF)(2)-KHg(SCN)(4) at magnetic fields, mu0H >23 T, above its Pauli paramagnetic limit, reveal unambiguously that the magnetic hysteresis observed previously within this CDW phase is diamagnetic and can only be explained by induced currents. It is argued that the ensemble of experimental techniques amounts to a strong case for dissipationless conductivity within this phase. 相似文献
832.
Shimon Brooks 《Israel Journal of Mathematics》2013,198(1):393-417
We consider spaces of high-energy quasimodes for the Laplacian on a compact hyperbolic surface, and show that when the spaces are large enough, one can find quasimodes that exhibit strong localization phenomena. Namely, take any constant c, and a sequence of cr j -dimensional spaces S j of quasimodes, where $\frac{1}{4} + r_j^2 \to \infty $ is an approximate eigenvalue for S j . Then we can find a sequence of vectors ψ j ∈ S j , such that any weak-* limit point of the microlocal lifts of |ψ j |2 localizes a positive proportion of its mass on a singular set of codimension 1. This result is sharp, in light of the QUE result of [BL12] for certain joint quasimodes that include spaces of size o(r j ), with arbitrarily slow decay. 相似文献
833.
We formalize an algorithm for solving the -norm best-fit hyperplane problem derived using first principles and geometric insights about projection and regression. The procedure follows from a new proof of global optimality and relies on the solution of a small number of linear programs. The procedure is implemented for validation and testing. This analysis of the -norm best-fit hyperplane problem makes the procedure accessible to applications in areas such as location theory, computer vision, and multivariate statistics. 相似文献
834.
Abstract In this article we discuss the problem of assessing the performance of Markov chain Monte Carlo (MCMC) algorithms on the basis of simulation output. In essence, we extend the original ideas of Gelman and Rubin and, more recently, Brooks and Gelman, to problems where we are able to split the variation inherent within the MCMC simulation output into two distinct groups. We show how such a diagnostic may be useful in assessing the performance of MCMC samplers addressing model choice problems, such as the reversible jump MCMC algorithm. In the model choice context, we show how the reversible jump MCMC simulation output for parameters that retain a coherent interpretation throughout the simulation, can be used to assess convergence. By considering various decompositions of the sampling variance of this parameter, we can assess the performance of our MCMC sampler in terms of its mixing properties both within and between models and we illustrate our approach in both the graphical Gaussian models and normal mixtures context. Finally, we provide an example of the application of our diagnostic to the assessment of the influence of different starting values on MCMC simulation output, thereby illustrating the wider utility of our method beyond the Bayesian model choice and reversible jump MCMC context. 相似文献
835.
Paul P. Brooks Adrian Natalello John N. Hall E. Alex L. Eccles Solomon M. Kimani Karina Bley Lian R. Hutchings 《Macromolecular Symposia》2013,323(1):42-50
Alternating copolymers containing diphenylethylene (DPE) or diphenylethylene derivatives were prepared by living anionic polymerization using kinetic control. Due to steric hindrance DPE cannot homopolymerize. Therefore alternating copolymers can be prepared by ensuring the rate of cross-propagation (k12) of the co-monomer is favoured over the rate of self-propagation (k11). This reactivity ratio (r1 = k11/k12) can be controlled by many different factors, such as choice of monomer, electron-donating or withdrawing substituents on DPE, choice of solvent, etc. We report our progress on preparing alternating copolymers by varying these factors. 相似文献
836.
Egiyan KS Asryan G Gevorgyan N Griffioen KA Laget JM Kuhn SE Adams G Amaryan MJ Ambrozewicz P Anghinolfi M Audit G Avakian H Bagdasaryan H Baillie N Ball JP Baltzell NA Barrow S Batourine V Battaglieri M Bedlinskiy I Bektasoglu M Bellis M Benmouna N Berman BL Biselli AS Blaszczyk L Bouchigny S Boiarinov S Bradford R Branford D Briscoe WJ Brooks WK Bültmann S Burkert VD Butuceanu C Calarco JR Careccia SL Carman DS Cazes A Chen S Cole PL Collins P Coltharp P Cords D Corvisiero P Crabb D Crede V 《Physical review letters》2007,98(26):262502
The reaction 2H(e,e'p)n has been studied with full kinematic coverage for photon virtuality 1.75NN transition is the primary contribution at higher momenta. 相似文献
837.
Adler SS Afanasiev S Aidala C Ajitanand NN Akiba Y Al-Jamel A Alexander J Aoki K Aphecetche L Armendariz R Aronson SH Averbeck R Awes TC Babintsev V Baldisseri A Barish KN Barnes PD Bassalleck B Bathe S Batsouli S Baublis V Bauer F Bazilevsky A Belikov S Bjorndal MT Boissevain JG Borel H Brooks ML Brown DS Bruner N Bucher D Buesching H Bumazhnov V Bunce G Burward-Hoy JM Butsyk S Camard X Chand P Chang WC Chernichenko S Chi CY Chiba J Chiu M Choi IJ Choudhury RK Chujo T Cianciolo V Cobigo Y 《Physical review letters》2007,98(1):012002
Cross sections for midrapidity production of direct photons in p+p collisions at the Relativistic Heavy Ion Collider (RHIC) are reported for transverse momenta of 3 < pT < 16 GeV/c. Next-to-leading order perturbative QCD (pQCD) describes the data well for pT >5 GeV/c, where the uncertainties of the measurement and theory are comparable. We also report on the effect of requiring the photons to be isolated from parton jet energy. The observed fraction of isolated photons is well described by pQCD for pT >7 GeV/c. 相似文献
838.
Jones BA Facchetti A Wasielewski MR Marks TJ 《Journal of the American Chemical Society》2007,129(49):15259-15278
Structural and electronic criteria for ambient stability in n-type organic materials for organic field-effect transistors (OFETs) are investigated by systematically varying LUMO energetics and molecular substituents of arylene diimide-based materials. Six OFETs on n+-Si/SiO2 substrates exhibit OFET response parameters as follows: N,N'-bis(n-octyl)perylene-3,4:9,10-bis(dicarboximide) (PDI-8): mu = 0.32 cm2 V(-1) s(-1), Vth = 55 V, I(on)/I(off) = 10(5); N,N'-bis(n-octyl)-1,7- and N,N'-bis(n-octyl)-1,6-dibromoperylene-3,4:9,10-bis(dicarboximide) (PDI-8Br2): mu = 3 x 10(-5) cm2 V(-1) s(-1), Vth = 62 V, I(on)/I(off) = 10(3); N,N'-bis(n-octyl)-1,6,7,12-tetrachloroperylene-3,4:9,10-bis(dicarboximide) (PDI-8Cl4): mu = 4 x 10(-3) cm2 V(-1) (s-1), Vth = 37 V, I(on)/I(off) = 10(4); N,N'-bis(n-octyl)-2-cyanonaphthalene-1,4,5,8-bis(dicarboximide) (NDI-8CN): mu = 4.7 x 10(-3) cm2 V(-1) s(-1), Vth = 28, I(on)/I(off) = 10(5); N,N'-bis(n-octyl)-1,7- and N,N'-bis(n-octyl)-1,6-dicyanoperylene-3,4:9,10-bis(dicarboximide) (PDI-8CN2): mu = 0.13 cm2 V(-1) s(-1), Vth = -14 V, I(on)/I(off) = 10(3); and N,N'-bis(n-octyl)-2,6-dicyanonaphthalene-1,4,5,8-bis(dicarboximide) (NDI-8CN2): mu = 0.15 cm2 V(-1) s(-1), Vth = -37 V, I(on)/I(off) = 10(2). Analysis of the molecular geometries and energetics in these materials reveals a correlation between electron mobility and substituent-induced arylene core distortion, while Vth and I(off) are generally affected by LUMO energetics. Our findings also indicate that resistance to ambient charge carrier trapping observed in films of N-(n-octyl)arylene diimides occurs at a molecular reduction potential more positive than approximately -0.1 V (vs SCE). OFET threshold voltage shifts between vacuum and ambient atmosphere operation suggest that, at E(red1) < -0.1 V, the interfacial trap density increases by greater than approximately 1 x 10(13) cm(-2), while, for semiconductors with E(red1) > -0.1 V, the trap density increase is negligible. OFETs fabricated with the present n-type materials having E(red1) > -0.1 V operate at conventional gate biases with minimal hysteresis in air. This reduction potential corresponds to an overpotential for the reaction of the charge carriers with O2 of approximately 0.6 V. N,N'-1H,1H-Perfluorobutyl derivatives of the perylene-based semiconductors were also synthesized and used to fabricate OFETs, resulting in air-stable devices for all fluorocarbon-substituted materials, despite generally having E(red1) < -0.1 V. This behavior is consistent with a fluorocarbon-based O2 barrier mechanism. OFET cycling measurements in air for dicyanated vs fluorinated materials demonstrate that energetic stabilization of the charge carriers results in greater device longevity in comparison to the OFET degradation observed in air-stable semiconductors with fluorocarbon barriers. 相似文献
839.
Woodcock HL Moran D Brooks BR Schleyer PV Schaefer HF 《Journal of the American Chemical Society》2007,129(12):3763-3770
The geometries and relative stabilities of the singlet and triplet states of phenyl- (Cs), diphenyl- (C2), 1-naphthyl- (Cs), di(1-naphthyl)- (C2), and 9-anthryl-substituted (Cs) carbenes were investigated at the B3LYP/6-311+G(d,p) + ZPVE level of density functional theory. The singlet-triplet energy separations (DeltaEST), 2.7, 2.9, 3.4, 3.7, and 5.7 kcal/mol, respectively, after including an empirical correction (2.8 kcal/mol) based on the error in the computed singlet-triplet gap for methylene versus experiment, are in good agreement with available experimental values. Consistent with literature reports, triplet di(9-anthryl)carbene has a linear, D2d symmetrical, allene structure with 1.336 A C=C bond lengths and considerable biradical character. B3LYP favors such cumulene biradical structures and triplet spin states and predicts a large (>15 kcal/mol) "di(9-anthryl)carbene" singlet-triplet (biradical) energy gap. The resonance stabilization of both singlet and triplet carbenes increases modestly with the size of the arene substituent and overall, (di)arylcarbenes, both singlet and triplet, are better stabilized by bigger substituents. For example, methylene is stabilized more by a naphthyl than a phenyl group (singlets, 26.6 versus 24.4; and triplets, 20.9 versus 18.1 kcal/mol, respectively). The carbene geometries are affected by both steric effects and arene-carbene orbital interactions (sigma-p and p-pi). For instance, the central angles at the carbene are widened by a second arene group, which leads to increased s-character and shorter carbene bond lengths (i.e., C-C, C-H). In general, the aromaticity of the substituted rings in triplet carbenes is most affected by the presence of the unpaired electrons. 相似文献
840.
Brooks PR Harland PW Harris SA Kennair T Redden C Tate JF 《Journal of the American Chemical Society》2007,129(50):15572-15580
Electron transfer from K atoms to oriented CH3CN, CH3NC, and CCl3CN is studied in crossed beams at energies near the threshold for forming an ion pair. For the methyl compounds, the dominant ions are K+ and CN-; the steric asymmetry is very small and energy-independent, characteristic of sideways attack with the electron apparently entering the pi*CN antibonding orbital. Migration of the electron to the sigma*CC orbital to break the C-C bond is greatly facilitated by interaction with the atomic donor. CH2CN- is formed in collisions preferring CH3-end attack, and the steric asymmetry becomes very large near threshold. CCl3CN mostly forms Cl- in collisions slightly favoring the CCl3 end with a small energy dependence with the electron apparently entering the sigma* LUMO. CN- is formed in much smaller yield with a slight preference for the CN end. The parent negative ion CCl3CN- is observed, and a lower limit for its electron affinity is estimated to be 0.3 eV. Fragment ions CCl2CN- and CClCN- are also observed with upper limits for the quantity bond dissociation energy - electron affinity (BDE - EA) estimated to be 0.6 and 1.0 eV, respectively. 相似文献