Synthesis of highly substituted 2,3-dihydropyrimido[4,5-<Emphasis Type="Italic">d</Emphasis>]pyrimidin-4(1<Emphasis Type="Italic">H</Emphasis>)-ones from 4,6-dichloro-5-formylpyrimidine,amines and aldehydes

A practical strategy was developed for the preparation of highly substituted 2,3-dihydropyrimido[4,5-d]pyrimidin-4(1H)-ones from 4,6-dichloro-5-formylpyrimidine, primary amines, and aldehydes. The key step for this synthesis entails a cyclization reaction involving an intramolecular amide addition to an iminium intermediate formed in situ from 4-amino-pyrimidine-5-carboxamide 2 and aldehydes to form the pyrimido[4,5-d]pyrimidine core with a strategically placed 5-Cl group for further derivatization. The utility of this methodology was demonstrated through the preparation of a 27-membered library of representative 2,3-dihydropyrimido[4,5-d]pyrimidin-4(1H)-ones in moderate to good yields.     

An efficient and facile synthesis of new tetracyclic fused pyrazolo[4,3-<Emphasis Type="Italic">c</Emphasis>][1,2,4]triazino[4,5-<Emphasis Type="Italic">a</Emphasis>]quinolin-4(5<Emphasis Type="Italic">H</Emphasis>)-ones

Reaction of amidrazones 1a–1i with (1,5-dihydro-3-methyl-5-oxo-1-phenyl-4H-pyrazol-4-ylidene)propanedinitrile (2) in ethyl acetate solution in one-step reaction led to the formation of unprecedented pyrazolo[4,3-c][1,2,4]triazino[4,5-a]quinolin-4(5H)-ones 3a–3g along with pyrazolo[4,3-c][1,2,4]triazino[4,5-a]quinolin-12b-oles 3h–3m in moderate to excellent yields. These novel heterocycles were formed via a Michael addition reaction followed by intramolecular cyclization via a dearomatization process.     

Synthesis of cyano-2,3-dihydropyrrolo[1,2-<Emphasis Type="Italic">f</Emphasis>]phenanthridine derivatives via a domino-Knoevenagel-cyclization

Abstract  

In a new multicomponent reaction phenanthridine reacts with isocyanides and malonitrile in the presence of benzaldehyde derivatives to produce 2-aryl-3-(alkyl- or arylimino)-2,3-dihydropyrrolo[1,2-f]phenanthridine-1,1(12b H)-dicarbonitrile in a simple, mild, and efficient protocol in excellent yields.     

Electron paramagnetic resonance of spin-variable metallomesogens [Fe<Emphasis Type="Italic">L</Emphasis><Subscript>2</Subscript>]<Emphasis Type="Italic">X</Emphasis> (<Emphasis Type="Italic">X</Emphasis> = PF<Subscript>6</Subscript>, SCN)

Significant differences in the manifestation of spin-crossover properties of the mesogen compounds [FeL ₂]X with oxysalicylidene-N′-ethyl-N-ethylenediamine ligands L and anions X = PF₆⁻ and SCH⁻ have been found by means of electron paramagnetic resonance. The electron paramagnetic resonance data and the quantum-chemical calculation within the density functional theory enables us to establish that the observed specific features are associated with the incorporation of the SCH⁻ ion into the first coordination sphere of the Fe(III) ion. The role of the transition of the material to the liquid-state phase in the formation of a low-dimensional (two-dimensional) structure with stronger intermolecular interactions has been revealed.     

Diversity oriented heterocyclizations of pyruvic acids,aldehydes and 5-amino-<Emphasis Type="Italic">N</Emphasis>-aryl-1<Emphasis Type="Italic">H</Emphasis>-pyrazole-4-carboxamides: catalytic and temperature control of chemoselectivity

Heterocyclization reactions of pyruvic acids, aromatic aldehydes and 5-amino-N-aryl-1H-pyrazole-4-carboxamides yielding four different types of final compounds are described. The reactions involving arylidenpyruvic acids lead with high degree of selectivity to either 4,7-dihydropyrazolo[1,5-a]pyrimidine-5-carboxylic acids or 5-[(2-oxo-2,5-dihydrofuran-3-yl)amino]-1H-pyrazoles, depending on the catalyst type or temperature regime. The interactions based on arylpyruvic acids can take place under kinetic or thermodynamic control producing 7-hydroxy-4,5,6,7-tetrahydropyrazolo[1,5-a]pyrimidine-7-carboxylic acids or 3-hydroxy-1-(1H-pyrazol-5-yl)-1,5-dihydro-2H-pyrrol-2-ones, respectively.     

A new synthetic approach to functionalize pyrimido[4,5-<Emphasis Type="Italic">b</Emphasis>]quinoline-2,4(1<Emphasis Type="Italic">H</Emphasis>,3<Emphasis Type="Italic">H</Emphasis>)-diones via a three-component one-pot reaction

Functionalized pyrimido[4,5-b]quinoline-2,4 (1H,3H)-diones were synthesized by a three-component one-pot reaction involving barbituric acid, aldehydes, and anilines. The use of commercially available anilines allowed the facile syntheses of pyrimido[4,5-b]quinolinediones substituted in all the positions on the benzene ring with electron donor or electron withdrawing groups. This straightforward method circumvents the preparation of unstable substituted 2-aminobenzaldehydes that limits the scope of previously described syntheses. Furthermore, access to the 5-substituted derivatives is now also possible starting from aliphatic or aromatic aldehydes. Our strategy and methodology offer significant and practical improvements over other methodologies.     

A new one-pot three-component synthesis of 2,4-diamino-5<Emphasis Type="Italic">H</Emphasis>-chromeno[2,3-<Emphasis Type="Italic">b</Emphasis>]pyridine-3-carbonitrile derivatives

In this study, a three-component one-pot synthesis of new 2,4-diamino-5H-chromeno[2,3-b]pyridine-3-carbonitriles derived from 2-amino-1,1,3-tricyanopropene, salicylic aldehydes and secondary cyclic amines is reported. The reaction is conducted in ethanol at ambient temperature in good-to-excellent yields.     

Substituted <Emphasis Type="Italic">N</Emphasis>-aminothioglycolurils containing thiosemicarbazone moiety and their cytotoxic activity in vitro

A library of hybrid molecules bearing thioglycoluril and (hetero)aromatic aldehyde thiosemicarbazone moieties was synthesized via a tandem hydrazone formation—ring contraction reaction of 5,7-dialkyl-3-thioxoperhydroimidazo[4,5-e]-1,2,4-triazin-6-ones with (hetero)aromatic aldehydes. All synthesized compounds were tested for their cytotoxic activity against rhabdomyosarcoma, A549, and MS human cancer cell lines by MTT-assay. Among the derivatives, (E)-4-benzylideneamino-1,3-dimethyl-5-thioxohexahydroimidazo[4,5-d]imidazol-2(1H)-one 1f was found to have the most marked antiproliferative activity toward the tested cell lines (1f: IC\(_{50}= 20.6,\) 23.7, and 6.4 \(\upmu \)M, respectively). The IC\(_{50}\) value of thioglycoluril 1f against normal human embryonic kidney cells HEK293 was 72.5 \(\upmu \)M, which appeared to be 3–11-fold higher than IC\(_{50}\) values of 1f against human cancer cells.     

Noncommutative Manifolds from Graph and <Emphasis Type="Italic">k</Emphasis>-Graph <Emphasis Type="Italic">C</Emphasis>*-Algebras

In [PRen] we constructed smooth (1, ∞)-summable semifinite spectral triples for graph algebras with a faithful trace, and in [PRS] we constructed (k, ∞)-summable semifinite spectral triples for k-graph algebras. In this paper we identify classes of graphs and k-graphs which satisfy a version of Connes’ conditions for noncommutative manifolds.     

<Emphasis Type="Italic">EPJdirect</Emphasis>

Quark mass effects are analyzed at high Q² in the current fragmentation region of DIS. It is found that the linear combination F ₂ -2.75F ^c ₂ scales at large Q² and small x. We obtained a lower bound for the ratio F ^c ₂/F ₂ which lies very close to the data from HERA. Received: 14 January 2002 / Revised version: 9 October 2002 Published online: 9 December 2002 RID="a" ID="a" e-mail: ryutin@th1.ihep.su     

Reconstruction of some cosmological models in <Emphasis Type="Italic">f</Emphasis>(<Emphasis Type="Italic">R</Emphasis>,<Emphasis Type="Italic">T</Emphasis>) cosmology

In this paper, we reconstruct cosmological models in the framework of f(R,T) gravity, where R is the Ricci scalar and T is the trace of the stress-energy tensor. We show that the dust fluid reproduces ΛCDM, phantom–non-phantom era and phantom cosmology. Further, we reconstruct different cosmological models, including the Chaplygin gas, and scalar field with some specific forms of f(R,T). Our numerical simulation for the Hubble parameter shows good agreement with the BAO observational data for low redshifts, z<2.     

A note on <Emphasis Type="Italic">q</Emphasis>-Bernstein polynomials

Recently, Simsek-Acikgoz [17] and Kim-Jang-Yi [9] have studied the q-extension of Bernstein polynomials. In the present paper, we suggest q-extensions of Bernstein polynomials of degree n which differ from the q-Bernstein polynomials of Simsek-Acikgoz [17] and Kim-Jang-Yi [9]. Using these q-Bernstein polynomials, we derive fermionic p-adic integral representations of several q-Bernstein-type polynomials. Finally, we investigate identities between q-Bernstein polynomials and q-Euler numbers.     

Supramolecular Interaction of Two Tryptophans with <Emphasis Type="Italic">p</Emphasis>-sulfonated calix[<Emphasis Type="Italic">4,6,8</Emphasis>]arene

The complex characteristics of p-sulfonated calix[n]arene (SCnA) and two tryptophans N-[(tert-butoxy) carbonyl]-tryptophan (trp-A) and N-carbobenzoxy-tryptophane (trp-B) were examined through various techniques. Spectrofluorimetry was performed at different temperatures to determine the stability constants and evaluate the thermodynamic parameters of the two complexes. The effect of pH on complex formation was estimated. According to the fluorescence data, the assumption about the steric hindrance of the tert-butyl group of trp-A and the phenyl group of trp-B was put forward. ¹H NMR was also performed to determine the binding interaction mechanism. Results showed that the indole benzene rings of the two tryptophans partly penetrated into the cavity of p-sulfonated calix[n]arene. The shift in Ha, Hb and Hc, Hd positions became more significant as the number of phenolic units of the calixarene ring increased. Molecular modeling of the complexes elucidated the assumption about the steric hindrance of the tert-butyl group of trp-A and the phenyl group of trp-B. These observations of molecular modeling computation are consistent with previous fluorescence data and ¹H NMR results.     

<Emphasis Type="Italic">f</Emphasis>(<Emphasis Type="Italic">R</Emphasis>) Cosmology from <Emphasis Type="Italic">q</Emphasis>-theory

From a macroscopic theory of the quantum vacuum in terms of conserved relativistic charges (generically denoted by q ^(a) with label a), we have obtained, in the low-energy limit, a particular type of f(R) model relevant to cosmology. The macroscopic quantum-vacuum theory allows us to distinguish between different phenomenological f(R) models on physical grounds. The text was submitted by the authors in English.     

The <Emphasis Type="Italic">B</Emphasis>(<Emphasis Type="Italic">E</Emphasis>1) strength of <Superscript>11</Superscript>Be extracted from the Coulomb excitation measurements

We have extracted the B(E1) strength for the transition 1/2⁺ → 1/2⁻ occurring in ¹¹Be from the recent Coulomb excitation measurements using the nonrelativistic and intermediate-energy Coulomb-excitation (IECE) theory and have found that the results of IECE theory are in good agreement with the adopted value of B(E1). When the survival probability of the projectile is taken into account the agreement between the calculated and the adopted value of B(E1) strength improves further. We have also studied the effect of diffuseness parameter of survival probability on the B(E1) strength. The text was submitted by the authors in English.     

Ionic liquid-promoted multi-component reaction: novel and efficient preparation of pyrazolo[3,4-<Emphasis Type="Italic">b</Emphasis>]pyridinone,pyrazolo[3,4-<Emphasis Type="Italic">b</Emphasis>]-quinolinone and their hybrids with pyrimidine nucleoside

The utilization of an ionic liquid, [bmim][BF₄] as both reaction medium and promoter for a multi-component reaction of aldehyde (1) and 5-amino-3-methyl-1-phenylpyrazole (2) with Meldrum acid (3) or dimedone (5) is studied. From this reaction, pyrazolo[3,4-b]pyridinone (4) and pyrazolo[3,4-b]quinolinone (6) derivatives were prepared in high yields. This novel procedure showed such advantages as environmentally benign nature, enhanced efficiency, simple operation process, and mild reaction conditions. As an application, the procedure was successfully used in the preparation of a set of pyrimidine nucleoside–pyrazolo[3,4-b]pyridine and pyrazolo[3,4-b]quinolinone hybrids with potential biological activities.     

Exact Results for Topological Strings on Resolved <Emphasis Type="Italic">Y</Emphasis><Superscript><Emphasis Type="Italic"> p</Emphasis>,<Emphasis Type="Italic">q</Emphasis></Superscript> Singularities

We obtain exact results in α′ for open and closed A-model topological string amplitudes on a large class of toric Calabi-Yau threefolds by using their correspondence with five dimensional gauge theories. The toric Calabi-Yaus that we analyze are obtained as minimal resolution of cones over Y ^p,q manifolds and give rise via M-theory compactification to SU(p) gauge theories on . As an application we present a detailed study of the local case and compute open and closed genus zero Gromov-Witten invariants of the orbifold. We also display the modular structure of the topological wave function and give predictions for higher genus amplitudes. The mirror curve in this case is the spectral curve of the relativistic A ₁ Toda chain. Our results also indicate the existence of a wider class of relativistic integrable systems associated to generic Y ^p,q geometries.     

Cosmological Models with Variable <Emphasis Type="Italic">G</Emphasis> in <Emphasis Type="Italic">C</Emphasis>-Field Cosmology

Cosmological models with variable G in C-field cosmology for barotropic fluid distribution in FRW space-time are investigated. To get the deterministic model of the universe, we have assumed that G=R ⁿ where R is the scale factor and n the constant. To obtain the results in terms of cosmic time t, we have assumed n=−1. We find that for n=−1, Creation field (C) and spatial volume increase with time, G and ρ (matter density) decreases with time, the model represent accelerating universe. Thus inflationary scenario exists in the model. The model is also free from horizon. The results so obtained match with the astronomical observations.     

On the Unitarity of <Emphasis Type="Italic">D</Emphasis> = 9, 10, 11 Conformal Supersymmetry

We consider the unitarity of D = 9, 10, 11 conformal supersymmetry using the recently established classification of the UIRs of the superalgebras osp(12n, ).     

The emission spectrum of <Emphasis Type="Italic">p</Emphasis>-AlGaAs/GaAsP/<Emphasis Type="Italic">n</Emphasis>-AlGaAs diodes under uniaxial compression

New experimental data are presented on the effects of uniaxial compression of up to 4 kbar along the [110] and [1$ \bar 1 $ \bar 1 0] crystallographic directions on the spectra of electroluminescence and the current-voltage characteristics of diodes based on n-Al _x Ga_{1 − x} As/GaAs _y P_{1 − y} /p-Al _x Ga_{1 − x} As (y = 0.84) heterostructures that were designed for injection lasers. With increasing pressure, the spectra show a shift to shorter wavelengths, reaching 25 meV at 3 kbar; the intensity increases 2–3 times as well. Numerical calculations were carried out on the band structure of the investigated heterostructures under compression along the [110] axis, which indicate the increase in the effective band gap in the quantum well (QW) GaAs _y P_{1 − y} , with a pressure coefficient of about 8.5 meV/kbar and reduction of the barrier height at the boundaries of the QW. The calculations predict the possibility that light and heavy holes crossover at pressures above 4.5–5 kbar. The increase in the effective band gap completely describes the experimental data on the shift of the electroluminescence spectra. The mixing of light and heavy holes when approaching the band crosspoint is the probable cause of an increase in the intensity of radiation under uniaxial compression.