Observation of a Tricyclic[4.1.0.0 2,4]heptane During a Michael Addition-Ring Closure Reaction and a Computational Study on Its Mechanism of Formation

We describe the formation of a bis-cyclopropane product, a tricyclic[4.1.0.02,4]heptane, that is formed during a Johnson-Corey-Chaykovsky reaction on a cyclopentenone. Two (of four possible) bicyclic products are selectively formed by addition of a COOEt-stabilized sulfur ylide onto the Michael acceptor. The tricyclic product is formed subsequently via a retro Michael elimination of a hindered ether followed by addition of a further cyclopropyl moiety, affecting only one of the two bicyclic products initially formed. The experimental reaction outcome was rationalized using density functional theory (DFT), investigating the different Michael-addition approaches of the sulfur ylide, the transition state (TS) energies for the formation of possible zwitterionic intermediates and subsequent reactions that give rise to cyclopropanation. Selective formation of only two of the four possible products occurs due to the epimerization of unreactive intermediates from the other two pathways, as revealed by energy barrier calculations. The formation of the tricyclic product was rationalized by evaluation of energy barriers for proton abstraction required to form the intermediate undergoing the second cyclopropanation. The selectivity-guiding factors discussed for the single and double cyclopropanation of this functionalized Michael-acceptor will be useful guidelines for the synthesis of future singly and doubly cyclopropanated compounds

Negative refraction and the spectral filtering of terahertz radiation by a photonic crystal prism

We demonstrate how micromachined photonic crystals can be used to negatively refract terahertz frequency light. The photonic crystals, which are constructed from conventional dielectric materials, manipulate the incident beam via interaction with their photonic bands. Consequently, we show that different components of a broadband beam incident on the structure may be positively or negatively refracted, depending upon its frequency and that the structure can be used as an effective spectral filter of THz radiation

Complete Analysis of Baryon Magnetic Moments in 1/N_c

We generate a complete basis of magnetic moment operators for the N_c = 3 ground-state baryons in the 1/N_c expansion, and compute and tabulate all associated matrix elements. We then compare to previous results derived in the literature and predict additional relations among baryon magnetic moments holding to subleading order in 1/N_c and flavor SU(3) breaking. Finally, we predict all unknown diagonal and transition magnetic moments to <= 0.15 mu_N accuracy, and suggest possible experimental measurements to improve the analysis even further.Comment: 28 pages (including 11 tables), ReVTeX. One reference and grant acknowledgment adde

Magnetic Coherence in Cuprate Superconductors

Recent inelastic neutron scattering (INS) experiments on La$_{2-x}$Sr$_x$CuO$_4$ observed a {\it magnetic coherence effect}, i.e., strong frequency and momentum dependent changes of the spin susceptibility, $\chi''$, in the superconducting phase. We show that this effect is a direct consequence of changes in the damping of incommensurate antiferromagnetic spin fluctuations due to the appearance of a d-wave gap in the fermionic spectrum. Our theoretical results provide a quantitative explanation for the weak momentum dependence of the observed spin-gap. Moreover, we predict {\bf (a)} a Fermi surface in La$_{2-x}$Sr$_x$CuO$_4$ which is closed around $(\pi,\pi)$ up to optimal doping, and {\bf (b)} similar changes in $\chi''$ for all cuprates with an incommensurate magnetic response.Comment: 5 pages, 4 figures, Fig.3 is in colo

Hopping Conduction in Disordered Carbon Nanotubes

We report electrical transport measurements on individual disordered carbon nanotubes, grown catalytically in a nanoporous anodic aluminum oxide template. In both as-grown and annealed types of nanotubes, the low-field conductance shows as exp[-(T_{0}/T)^{1/2}] dependence on temperature T, suggesting that hopping conduction is the dominant transport mechanism, albeit with different disorder-related coefficients T_{0}. The field dependence of low-temperature conductance behaves an exp[-(xi_{0}/xi)^{1/2}] with high electric field xi at sufficiently low T. Finally, both annealed and unannealed nanotubes exhibit weak positive magnetoresistance at low T = 1.7 K. Comparison with theory indicates that our data are best explained by Coulomb-gap variable range hopping conduction and permits the extraction of disorder-dependent localization length and dielectric constant.Comment: 10 pages, 5 figure

More Model-Independent Analysis of b->s Processes

We study model-independently the implications of non-standard scalar and pseudoscalar interactions for the decays b ->s gamma, b -> s g, b -> s l^+l^- (l=e,mu) and B_s -> mu^+ mu^-. We find sizeable renormalization effects from scalar and pseudoscalar four-quark operators in the radiative decays and at O(alpha_s) in hadronic b decays. Constraints on the Wilson coefficients of an extended operator basis are worked out. Further, the ratios R_H = BR(B -> H mu^+ mu^-)/BR(B -> H e^+ e^-), for H=K^(*), X_s, and their correlations with B_s -> mu^+ mu^- decay are investigated. We show that the Standard Model prediction for these ratios defined with the same cut on the dilepton mass for electron and muon modes, R_H= 1 + O(m^2_mu/m^2_b), has a much smaller theoretical uncertainty (<1%) than the one for the individual branching fractions. The present experimental limit R_K < 1.2 puts constraints on scalar and pseudoscalar couplings, which are similar to the ones from current data on BR(B_s -> mu^+ mu^-). We find that new physics corrections to R_{K*} and R_{X_s} can reach 13% and 10%, respectively.Comment: 28 pages, 6 figures; Table 1 updated, two refs added (to appear in PRD

Large N_c, Constituent Quarks, and N, Delta Charge Radii

We show how one may define baryon constituent quarks in a rigorous manner, given physical assumptions that hold in the large-N_c limit of QCD. This constituent picture gives rise to an operator expansion that has been used to study large-N_c baryon observables; here we apply it to the case of charge radii of the N and Delta states, using minimal dynamical assumptions. For example, one finds the relation r_p^2 - r_{Delta^+}^2 = r_n^2 - r_{Delta^0}^2 to be broken only by three-body, O(1/N_c^2) effects for any N_c.Comment: 15 pages, 1 eps figure. Version to appear in Phys. Rev.

Microwave conductivity of YBa2_2Cu3_3O6.99_{6.99} including inelastic scattering

The fluctuation spectrum responsible for the inelastic scattering in YBa$_2$Cu$_3$O$_{6.99}$ which was recently determined from consideration of the in-plane optical conductivity in the infrared, is used to calculate the temperature dependence of the microwave conductivity at several measured frequencies. Reasonable overall agreement can only be achieved if, in addition, some impurity scattering is included within a model potential intermediate between weak (Born) and strong (unitary) limit.Comment: 15 pages, 5 figures accepted for publication in Phys. Rev.

Average Lattice Symmetry and Nanoscale Structural Correlations in Magnetoresistive Manganites

We report x-ray scattering studies of nanoscale structural correlations in the paramagnetic phases of the perovskite manganites La$_{0.75}$(Ca$_{0.45}$Sr$_{0.55}$)$_{0.25}$MnO$_3$, La$_{0.625}$Sr$_{0.375}$MnO$_3$, and Nd$_{0.45}$Sr$_{0.55}$MnO$_3$. We find that these correlations are present in the orthorhombic $O$ phase in La$_{0.75}$(Ca$_{0.45}$Sr$_{0.55}$)$_{0.25}$MnO$_3$, but they disappear abruptly at the orthorhombic-to-rhombohedral transition in this compound. The orthorhombic phase exhibits increased electrical resistivity and reduced ferromagnetic coupling, in agreement with the association of the nanoscale correlations with insulating regions. In contrast, the correlations were not detected in the two other compounds, which exhibit rhombohedral and tetragonal phases. Based on these results, as well as on previously published work, we propose that the local structure of the paramagnetic phase correlates strongly with the average lattice symmetry, and that the nanoscale correlations are an important factor distinguishing the insulating and the metallic phases in these compounds.Comment: a note on recent experimental work, and a new reference adde

Theory of NMR as a local probe for the electronic structure in the mixed state of the high-TcT_c cuprates

We argue that nuclear magnetic resonance experiments are a site-sensitive probe for the electronic spectrum in the mixed state of the high-$T_c$ cuprates. Within a spin-fermion model, we show that the Doppler-shifted electronic spectrum arising from the circulating supercurrent changes the low-frequency behavior of the imaginary part of the spin-susceptibility. For a hexagonal vortex lattice, we predict that these changes lead to {\it (a)} a unique dependence of the $^{63}$Cu spin lattice relaxation rate, $1/T_1$, on resonance frequency, and {\it (b)} a temperature dependence of $T_1$ which varies with frequency. We propose a nuclear quadrupole experiment to study the effects of a uniform supercurrent on the electronic structure and predict that $T_1$ varies with the direction of the supercurrent.Comment: RevTex, 5 pages, 3 figures embedded in the tex