Iodine(III)‐Catalyzed Rearrangements of Imides: A Versatile Route to α,α‐Dialkylated α‐Hydroxy Carboxylamides

A tertiary hydroxy group α to a carboxyl moiety comprises a key structural motif in many bioactive substances. With the herein presented metal‐free rearrangement of imides triggered by hypervalent λ³‐iodane, an easy and selective way to gain access to such a compound class, namely α,α‐disubstituted‐α‐hydroxy carboxylamides, was established. Their additional methylene bromide side chain constitutes a useful handle for rapid diversification, as demonstrated by a series of further functionalizations. Moreover, the in situ formation of an iodine(III) species under the reaction conditions was proven. Our findings clearly corroborate that hypervalent λ³‐benziodoxolones are involved in these organocatalytic reactions.     

Coherent States and Number-Phase Uncertainty Relations

The number-phase uncertainty relations arerevisited in view of the recent discovery of a propercovariant phase observable. The high-amplitude limits ofthe coherent-state expectations of the moment operators of the phase observable are determined and thebehavior of the number-phase uncertainty product in thatlimit is investigated.     

Spin-dependent shot noise of inelastic transport through molecular quantum dots

Here we present a theoretical analysis of the effect of inelastic electron scattering on spin-dependent transport characteristics (conductance, current–voltage dependence, magnetoresistance, shot noise spectrum, Fano factor) for magnetic nanojunction. Such device is composed of molecular quantum dot (with discrete energy levels) connected to ferromagnetic electrodes (treated within the wide-band approximation), where molecular vibrations are modeled as dispersionless phonons. Non-perturbative computational scheme, used in this work, is based on the Green's function theory within the framework of mapping technique (GFT–MT), which transforms the many-body electron–phonon interaction problem into a single-electron multi-channel scattering problem. The consequence of the localized electron–phonon coupling is polaron formation. It is shown that polaron shift and additional peaks in the transmission function completely change the shape of considered transport characteristics.     

Approximating schedules for dynamic process graphs efficiently

A model for parallel and distributed programs, the dynamic process graph (DPG), is investigated under graph-theoretic and complexity aspects. Such graphs embed constructors for parallel programs, synchronization mechanisms as well as conditional branches. They are capable of representing all possible executions of a parallel or distributed program in a very compact way. The size of this representation can be as small as logarithmic with respect to the size of any execution of the program.

In a preceding paper [A. Jakoby, et al., Scheduling dynamic graphs, in: Proc. 16th Symposium on Theoretical Aspects in Computer Science STACS'99, LNCS, vol. 1563, Springer, 1999, pp. 383–392] we have analysed the expressive power of the general model and various variants of it. We have considered the scheduling problem for DPGs given enough parallelism taking into account communication delays between processors when exchanging data. Given a DPG the question arises whether it can be executed (that means whether the corresponding parallel program has been specified correctly), and what is its minimum schedule length.

In this paper we study a subclass of dynamic process graphs called -output DPGs, which are appropriate in many situations, and investigate their expressive power. In a previous paper we have shown that the problem to determine the minimum schedule length is still intractable for this subclass, namely this problem is -complete as is the general case. Here we will investigate structural properties of the executions of such graphs. A natural graph-theoretic conjecture that executions must always split into components that are isomorphic to subgraphs turns out to be wrong. We are able to prove a weaker property. This implies a quadratic upper bound on the schedule length that may be necessary in the worst case, in contrast to the general case, where the optimal schedule length may be exponential with respect to the size of the representing DPG. Making this bound constructive, we obtain an approximation to a -complete problem. Computing such a schedule and then executing the program can be done on a parallel machine in polynomial time in a highly distributive fashion.     

Synthesis of 1-(3-alkyl-2,3-dideoxy-D-pentofuranosyl)uracils with potential anti-HIV activity.

1-(3-Alkyl-2,3-dideoxy-alpha,beta-D-erythro-pentofuranosyl)uracils and 1-(3-alkyl-2,3-dideoxy-alpha,beta-D-threo-pentofuranosyl)uracils have been prepared from (E)-4,5-di-O-acetyl-2,3-dideoxy-aldehydo-D-glycero-pent-2-enose by a Michael addition reaction of the appropriate organocopper reagent followed in subsequent order by glycosidation of the resulting 3-alkyl-4,5-diacetoxypentanal with methanolic hydrogen chloride, protection with p-methoxybenzoyl chloride, and trimethylsilyl triflate catalyzed coupling with 2,4-di-O-(trimethylsilyl)uracil. The nucleosides were deprotected by treatment with 33% methylamine in absolute ethanol and separated by reversed-phase HPLC.     

Coulomb blockade in molecular quantum dots

The rate-equation approach is used to describe sequential tunneling through a molecular junction in the Coulomb blockade regime. Such device is composed of molecular quantum dot (with discrete energy levels) coupled with two metallic electrodes via potential barriers. Based on this model, we calculate nonlinear transport characteristics (conductance-voltage and current-voltage dependences) and compare them with the results obtained within a self-consistent field approach. It is shown that the shape of transport characteristics is determined by the combined effect of the electronic structure of molecular quantum dots and by the Coulomb blockade. In particular, the following phenomena are discussed in detail: the suppression of the current at higher voltages, the charging-induced rectification effect, the charging-generated changes of conductance gap and the temperature-induced as well as broadening-generated smoothing of current steps.     

A four-level “Ξ-system”: Exact solvability and effective evolution operators via multiple scales

Properties of a four-level atomic system interacting with one and two modes of the electromagneticfield in a “Ξ”-configuration are investigated. By linearization of the Hamiltonians we show that the corresponding mathematical models are exactly solvable. To obtain simpler effective Hamiltonians the perturbative method of multiple scales is applied. The lowest-order corrections to the resulting effective evolution operators are also calculated.     

N‐{3‐[(2‐Ammonioethyl)amino]propyl}ethane‐1,2‐diaminium tris(trifluoromethanesulfonate): a salt of a folded triply protonated tetramine

The structure of a trifluoromethanesulfonate salt of a nontypical triply protonated linear tetramine, C₇H₂₃N₄³⁺·3CF₃SO₃⁻, with a layered crystal structure is presented. One N atom remains unprotonated. The conformation of the cation is enforced by intra‐ and intermolecular hydrogen bonds. The crystal structure is built of ca 10 Å deep layers, within which cations and anions are hydrogen bonded. Each layer is only weakly bound to its neighbours. This study shows a rare example of an unsymmetrically protonated polyamine and the relation between the lack of protonation, intramolecular hydrogen bonding and the conformation of the cation.     

Template atom transfer radical polymerization of a diaminopyrimidine‐derivatized monomer in the presence of a uracil‐containing polymer

Uracil‐derivatized monomer 6‐undecyl‐1‐(4‐vinylbenzyl)uracil and diaminopyrimidine‐derivatized monomer 2,6‐dioctanoylamido‐4‐methacryloyloxypyrimidine (DMP) were synthesized and polymerized by atom transfer radical polymerization (ATRP). A well‐defined, highly soluble, uracil‐containing polymer, poly[6‐undecyl‐1‐(4‐vinylbenzyl)uracil] (PUVU), was prepared in dioxane at 90 °C with CuBr/1,1,4,7,10,10‐hexamethyltriethylenetetramine as the catalyst and methyl α‐bromophenylacetate as the initiator. PUVU was further used as a template for the ATRP of DMP. The enhanced apparent rate constant of the DMP polymerization in the presence of PUVU indicated that the ATRP of DMP occurred along the PUVU template. The template polymerization produced a stable and insoluble macromolecular complex, PUVU/poly(2,6‐dioctanoylamido‐4‐methacryloyloxypyrimidine). An X‐ray diffraction study confirmed that the complex had strandlike domains. © 2006 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 44: 6607–6615, 2006     

In-trees and plane embeddings of outerplanar graphs

A notion of anin-tree is introduced. It is then used to characterize and count plane embeddings of outerplanar graphs. In-trees have also been applied in the study of independent vertex covers of faces in outerplanar graphs.This research was partially supported by the grant RP.I.09, from the Institute of Informatics, University of Warsaw. Hospitality of the Institute of Datalogy, University of Copenhagen where this research has been completed is gratefully acknowledged.