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PubMed2006

Fabrication and characterization of molecular beam epitaxy grown thin-film GaAs waveguides for mid-infrared evanescent field chemical sensing.

Thin-film GaAs waveguides were designed and fabricated by molecular beam epitaxy for use in mid-infrared (MIR) evanescent field liquid sensing. Waveguides were designed to facilitate the propagation of a single mode at a wavelength of 10.3 microm emitted from a distributed feedback quantum cascade laser, which overlaps with molecular selective absorption features of acetic anhydride. The characterization of the waveguides shows transmission across a broad MIR band. Evanescent field absorption measurements indicate a significant sensitivity enhancement in contrast to multimode planar silver halide waveguides.

Equipment Design↗
PubMedDate not supplied

Molecular design based on 3D pharmacophores. Applications to 5-HT7 receptors.

A definition of a pharmacophore for the 5-HT7 antagonists was carried out by searching the common chemical features of selective antagonists from the literature. A molecular design is described by analyzing the differences between this new pharmacophore and three other 3D serotonin pharmacophores previously described. This comparison led to the synthesis of a new series of potent 5-HT7 antagonists.

Models, Molecular↗
PubMed1996

A Bis(azo-imine)palladium(II) System with 10 Ligand pi Electrons. Synthesis, Structure, Serial Redox, and Relationship to Bis(azooximates) and Other Species.

The first azo-imine chelate system, Pd(N(H)C(R)NNPh)(2) (Pd(RA)(2)), has been isolated in the form of diamagnetic solids by the 6e(-)-6H(+) reduction of bis(phenylazooximato)palladium(II), Pd(N(O)C(R)NNPh)(2) (abbreviated Pd(RB)(2)), with ascorbic acid in a mixed solvent (R = Ph, alpha-naphthyl). Selected spectral features are described. The X-ray structures of Pd(PhA)(2) and Pd(PhB)(2) have revealed trans-planar geometry consistent with metal oxidation state of +2. Bond length trends within the chelate rings are rationalized in terms of steric and electronic factors. In Pd(PhA)(2) a total of 10 ligand pi electrons are present, each formally monoanionic ligand contributing five. Model EHMO studies have revealed that the filled HOMO (a(u)) in Pd(RA)(2) is a bonding combination of two ligand pi orbitals with large azo contributions. The LUMO (b(g)) is roughly the corresponding antibonding combination. The outer pi-electron configuration of Pd(RA)(2) is (a(u))(2)(b(g))(0). Four successive voltammetric responses, two oxidative and two reductive, are observed. The E(1/2) range is -1.3 to +0.8 V vs SCE for Pd(PhA)(2) in a 1:9 MeCN-CH(2)Cl(2) mixture (Pt electrode). EPR and electronic spectra of the electrogenerated one-electron-oxidized complex Pd(PhA)(2)(+) are described. The azo-imine system is compared with imine-imine and azo-azo systems. Crystal data for the complexes are as follows. Pd(PhA)(2): crystal system monoclinic; space group C2/c; a = 18.167(5) Å, b = 7.420(3) Å, c = 16.527(6) Å; beta = 92.70(3) degrees; V = 2225(1) Å(3); Z = 4; R = 2.61%, R(w) = 3.58%. Pd(PhB)(2): crystal system monoclinic; space group P2(1)/n; a = 5.735(5) Å, b = 10.797(6) Å, c = 18.022(11) Å; beta = 97.73(6) Å; V = 1105(1) Å(3); Z = 2; R = 3.37%; R(w) = 3.40%.

Journal Article↗
PubMed2006

A FRET-based approach to ratiometric fluorescence detection of hydrogen peroxide.

We report the synthesis, properties, and biological applications of Ratio-Peroxyfluor-1 (RPF1), a new ratiometric fluorescent reporter for hydrogen peroxide. RPF1 is comprised of a two-fluorophore cassette, where the spectral overlap between coumarin donor and fluoran/fluorescein acceptor partners can be controlled by the chemoselective peroxide-mediated deprotection of boronic ester pendants on the acceptor dye. RPF1 features good selectivity for hydrogen peroxide over a variety of reactive oxygen species, including superoxide and nitric oxide, a ca. 8-fold increase in fluorescence intensity ratio (lambda517/lambda464) upon H2O2 reaction, and excitation and emission profiles in the visible region. Experiments with viable yeast mitochondria show that RPF1 can monitor and quantify endogenous production of H2O2, establishing the potential utility of this approach for probing peroxide biology in living systems.

Fluorescein↗
PubMed2003

Synthesis and activity of new aryl- and heteroaryl-substituted pyrazole inhibitors of the transforming growth factor-beta type I receptor kinase domain.

Pyrazole-based inhibitors of the transforming growth factor-beta type I receptor kinase domain (TbetaR-I) are described. Examination of the SAR in both enzyme- and cell-based in vitro assays resulted in the emergence of two subseries featuring differing selectivity versus p38 MAP kinase. A common binding mode at the active site has been established by successful cocrystallization and X-ray analysis of potent inhibitors with the TbetaR-I receptor kinase domain.

3T3 Cells↗
PubMed2005

Factorizing selectivity determinants of inhibitor binding toward aldose and aldehyde reductases: structural and thermodynamic properties of the aldose reductase mutant Leu300Pro-fidarestat complex.

Structure of the Leu300Pro mutant of human aldose reductase (ALR2) in complex with the inhibitor fidarestat is determined. Comparison with the hALR2-fidarestat complex and the porcine aldehyde reductase (ALR1)-fidarestat complex indicates that the hydrogen bond between the Leu300 amino group of the wild-type and the exocyclic amide group of the inhibitor is the key determinant for the specificity of fidarestat for ALR2 over ALR1. Thermodynamic data also suggest an enthalpic contribution as the predominant difference in the binding energy between the aldose reductase mutant and the wild-type. An additional selectivity-determining feature is the difference in the interaction between the inhibitor and the side chain of Trp219, ordered in the present structure but disordered (corresponding Trp220) in the ALR1-fidarestat complex. Thus, the hydrogen bond ( approximately 7 kJ/mol) corresponds to a 23-fold difference in inhibitor potency while the differences in the interactions between Trp219(ALR2) and fidarestat and between Trp220(ALR1) and fidarestat can account for an additional 10-fold difference in potency.

Aldehyde Reductase↗
PubMed2006

Design and synthesis of novel sulfonamide-containing bradykinin hB2 receptor antagonists. 1. Synthesis and SAR of alpha,alpha-dimethylglycine sulfonamides.

We recently published the extensive in vivo pharmacological characterization of MEN 16132 (J. Pharmacol. Exp. Ther. 2005, 616-623; Eur. J. Pharmacol. 2005, 528, 7), a member of the sulfonamide-containing human B(2) receptor (hB(2)R) antagonists. Here we report, in detail, how this family of compounds was designed, synthesized, and optimized to provide a group of products with subnanomolar affinity for the hB(2)R and high in vivo potency after topical administration to the respiratory tract. The series was designed on the basis of indications from the X-ray structures of the key structural motifs A and B present in known antagonists and is characterized by the presence of an alpha,alpha-dialkyl amino acid. The first lead (17) of the series was submitted to extensive chemical work to elucidate the structural requirements to increase hB(2) receptor affinity and antagonist potency in bioassays expressing the human B(2) receptor (hB(2)R). The following structural features were selected: a 2,4-dimethylquinoline moiety and a piperazine linker acylated with a basic amino acid. The representative lead compound 68 inhibited the specific binding of [(3)H]BK to hB(2)R with a pKi of 9.4 and antagonized the BK-induced inositolphosphate (IP) accumulation in recombinant cell systems expressing the hB(2)R with a pA(2) of 9.1. Moreover, compound 68 when administered (300 nmol/kg) intratracheally in the anesthetized guinea pig, was able to significantly inhibit BK-induced bronchoconstriction for up to 120 min after its administration, while having a lower and shorter lasting effect on hypotension.

Animals↗
PubMed2001

Cyclopropane-derived peptidomimetics. design, synthesis, and evaluation of novel Ras farnesyltransferase inhibitors.

Trisubstituted cyclopropanes have previously been established as rigid replacements of dipeptide arrays in several biological systems. Toward further evaluating the utility of these dipeptide mimics in the design of novel CA(1)A(2)X-based inhibitors of Ras farnesyltransferase (FTase), the conformationally constrained, diastereomeric pseudopeptides CAbuPsi[COcpCO]FM 7-9, the flexible analogue CAbuPsi[CHOHCH(2)]FM (10), and the tetrapeptide CAbuFM (6) were prepared. The orientations of the two peptide backbone substituents and the phenyl group on the cyclopropane rings in 7-9were specifically designed to probe selected topological features of the hydrophobic binding pocket of the A(2) subsite of FTase. The syntheses of the requisite trisubstituted cyclopropane carboxylic acid 22 and the diastereomeric cyclopropyl lactones 32a,b featured diastereoselective intramolecular cyclopropanations of chiral allylic diazoacetates and a new method for introducing side chains onto the C-terminal amino acid of cyclopropane-derived dipeptide replacements via the opening of an N-Boc-aziridine with an organocuprate. These cyclopropane intermediates were then converted into the targeted FTase inhibitors 7-9 by standard peptide coupling techniques. The pseudopeptides 7-9 were found to be competitive inhibitors of Ras FTase with IC(50)s of 1055 nM for 7, 760 nM for 8, and 7200 nM for 9. The flexible analogue 10 of these constrained inhibitors exhibited a IC(50) of 320 nM and hence was slightly more potent than 7 and 8. All of these pseudopeptides were less potent than the tetrapeptide parent CAbuFM (6), which had an IC(50) of 38 nM. Because 7 and 8 are approximately equipotent, it appears that the orientation of the peptide backbone substituents on the cyclopropane rings in 7 and 8 do not have any significant effect on binding affinity and that multiple binding modes are possible without significant changes in affinity. On the other hand, this flexibility does not extend to the orientation of the side chain of the A(2) residue as 7 and 8 were both nearly 1 order of magnitude more potent than 9. Comparison of the relative potencies of 6 and 10 suggests that the amide linkage between the A(1) and the A(2) residues of CA(1)A(2)X-derived FTase inhibitors is important.

Alkyl and Aryl Transferases↗
PubMed2003

Temporal stability of high-frequency brain oscillations in the human EEG.

Temporal stability of a given measurement within individual participants is a desirable property of psychophysiological measures. The present study aims to examine the reliability of high-frequency oscillatory activity in the human electroencephalogram (EEG) across 4 sessions. Convolution of the EEG time series with Morlet wavelets yielded time-frequency representations of the signal for each session. Stability of both topography and time course of gamma-band activity (GBA) was determined for two participants performing a feature-based selective attention task in four separate sessions, spaced at weekly intervals. We found high temporal stability of non-phase-locked GBA typically occurring in time ranges between 200 and 500 ms following presentation of a stimulus, both in terms of topography and time course. Early phase-locked GBA (80-120 ms) showed higher variability with respect to topography, but was consistent in terms of time course. We conclude that measures of high-frequency oscillatory activity as used in the cognitive neurosciences meet stability requirements necessary for meaningful interpretation of this parameter of brain function.

Adult↗
PubMed1998

Structural relationships among dimensions of the DSM-IV anxiety and mood disorders and dimensions of negative affect, positive affect, and autonomic arousal.

Using outpatients with anxiety and mood disorders (N = 350), the authors tested several models of the structural relationships of dimensions of key features of selected emotional disorders and dimensions of the tripartite model of anxiety and depression. Results supported the discriminant validity of the 5 symptom domains examined (mood disorders: generalized anxiety disorder, GAD; panic disorder; obsessive-compulsive disorder; social phobia). Of various structural models evaluated, the best fitting involved a structure consistent with the tripartite model (e.g., the higher order factors, negative affect and positive affect, influenced emotional disorder factors in the expected manner). The latent factor, GAD, influenced the latent factor, autonomic arousal, in a direction consistent with recent laboratory findings (autonomic suppression). Findings are discussed in the context of the growing literature on higher order trait dimensions (e.g., negative affect) that may be of considerable importance to the understanding of the pathogenesis, course, and co-occurrence of emotional disorders.

Adolescent↗
PubMed1998

Selectivity in distraction by irrelevant featural singletons: evidence for two forms of attentional capture.

Four experiments addressed the degree of top-down control over attentional capture in visual search for featural singletons. In a modified spatial cuing paradigm, the spatial relationship and featural similarity of target and distractor singletons were systematically varied. Contrary to previous studies, all 4 experiments showed that when searching for a singleton target, an irrelevant featural singleton captures spatial attention only when defined by the same feature value as the target. Experiments 2, 3 and 4 provided a potential explanation for the discrepancy with previous studies by showing that irrelevant singletons can produce distraction effects that are dissociable from shifts of spatial attention. The results suggest the existence of 2 distinct forms of attentional capture.

Adolescent↗
PubMed2005

Building face composites can harm lineup identification performance.

Face composite programs permit eyewitnesses to build likenesses of target faces by selecting facial features and combining them into an intact face. Research has shown that these composites are generally poor likenesses of the target face. Two experiments tested the proposition that this composite-building process could harm the builder's memory for the face. In Experiment 1 (n = 150), the authors used 50 different faces and found that the building of a composite reduced the chances that the person could later identify the original face from a lineup when compared with no composite control conditions or with yoked composite-exposure control conditions. In Experiment 2 (n = 200), the authors found that this effect generalized to a simulated-crime video, but mistaken identifications from target-absent lineups were not inflated by composite building.

Adolescent↗
PubMed1996

Creation of genomic methylation patterns.

There are two biological properties of genomic methylation patterns that can be regarded as established. First, methylation of 5'-CpG-3' dinucleotides within promoters represses transcription, often to undetectable levels. Second, in most cases methylation patterns are subject to clonal inheritance. These properties suit methylation patterns for a number of biological roles, although none of the current hypotheses can be regarded as proved or disproved. One hypothesis suggests that the activity of parasitic sequence elements is repressed by selective methylation. Features of invasive sequences that might allow their identification and inactivation are discussed in terms of the genome defense hypothesis. Identification of the cues that direct de novo methylation may reveal the biological role (or roles) of genomic methylation patterns.

Alleles↗
PubMed1979

A study of some factors affecting generalization of language training.

Two related experiments examined generalization across contexts involving different sentence forms when selected grammatical features were trained within a single syntactic context. Results obtained within a single-subject multiple baseline design showed that training the verbal/auxiliary (contracted with pronoun he) was sufficient to induce its generalization across a variety of verbs, object noun phrases, and a different subjective case pronoun, but not across an objective case pronoun. Similar results were obtained for the uncontractible auxiliary in the past tense. Generalization of the uncontractible auxiliary in the present tense was noted across different verbs; so also was the generalization of contractible copula to different adjectives qualifying the subjective case pronouns he and she (but not in qualifying an objective case pronoun it). Finally, generalization of possessive s inflection across male, female, and animal categories was evident. Trained behavior generalized to home situation in one of the experiments. Some unexpected results also suggest that training on certain forms of either verbal auxiliary or copula may be sufficient to generate correct production of both of them.

Behavior Therapy↗
PubMed1999

Acoustical-perceptual correlates of "whisper pitch" in synthetically generated vowels.

The purpose of this investigation was to clarify acoustical-perceptual relationships in identification of "pitch" during whispered vowel production. The experimenters systematically varied selected acoustic features of synthetically generated "whispered" vowels to control which formant frequencies were shifted (F1, F2, or F1&F2), the direction of formant frequency shifts (up or down), and the magnitude of formant frequency shifts (20 Hz, 40 Hz, 60 Hz). Two sets of stimuli were produced to simulate the resonance characteristics of the vowel /a/: one set for male talkers and one for female talkers. Ninety-four pairs of synthesized vowel tokens were randomly presented to 17 listeners who judged if the "pitch" of the second member of the pair was the same, higher, or lower than the "pitch" of the first member. The results showed an inverse relationship between the magnitude of formant frequency changes presented to the judges and the number of perceptual mismatches in "whisper pitch." Also, fewer mismatches in the identification of whisper pitch occurred when both F1 and F2 were changed simultaneously than when either F1 or F2 was changed individually. No differences were found between the perceptual responses to "male" and "female" vowel simulations. The primary implication of this study is that whisper pitch is more influenced by simultaneous changes in F1 and F2 than by changes in only one of the formants.

Adult↗
PubMed1998

Surgical treatment and outcome in patients with a hepatocellular carcinoma greater than 10 cm in diameter.

BACKGROUND: Hepatocellular carcinoma (HCC) over 10 cm in diameter at the time of diagnosis continues to account for a number of patients undergoing hepatic resection. This study evaluated the clinicopathological features and outcome following surgery for large HCC. METHODS: Forty patients with a large HCC (greater than 10 cm) (group 1) resected between 1991 and 1996 were studied retrospectively. They were compared with 245 patients who had smaller HCCs (10 cm or less) (group 2). RESULTS: No patient in group 1 had hepatitis C infection compared with 22.9 per cent in group 2 (P=0.001). Patients in group 1 were significantly younger, had higher alpha-fetoprotein levels (16750 versus 1864 ng/ml; P < 0.001), better liver function, a higher incidence of multiple tumours (27 of 40 versus 42.0 per cent; P=0.003) and venous invasion (35 of 40 versus 52.2 per cent; P < 0.001), and underwent more major resections (37 of 40 versus 26.5 per cent; P < 0.001) than those in group 2. Morbidity and mortality rates and hospital stay were comparable in the two groups. For group 1, the 1-, 3- and 5-year disease-free survival rates were 42, 30 and 28 per cent respectively. Multiple tumours, venous invasion and impaired liver function were factors associated with recurrence. CONCLUSION: Large HCC had specific clinicopathological features. In selected patients, resection is safe and offers the chance of long-term disease-free survival.

Adult↗
PubMed2001

Segregation of effector mechanisms in a tumour-specific CD8+ T-cell clone correlates with CD30 expression.

In this study we have analyzed CD30-antigen expression in three melanoma-directed cytotoxic T lymphocyte (CTL) clones with a T helper 0 (Th0)-like cytokine secretion profile (i.e. interleukin (IL)-4, IL-5, and interferon (IFN)-gamma). We show that all CTL clones expressed high levels of CD30 upon contact with the autologous tumour cells. One CTL clone, termed A2 with a monoclonal feature was selected for further analyses and found its CD30 expression dependent on the presence of IL-4. Functionally, a CD30-expressing A2 CTL was capable of producing higher amounts of IFN-gamma (up to 1.5-fold) and IL-4 (up to two-fold) than its CD30- counterpart. Furthermore, CD30-positive A2 CTL displayed an at least three-fold greater proliferative response to the tumour cell stimulation, contrasting with CD30- CTL. However, the antitumour cytotoxic activity of A2 CTL was not modulated by the CD30 expression. These results suggest that CD30 antigen can be inducible on a subset of tumour-directed CD8+ CTL, and that this subset of cells may have profound effector functions, such as cytokine secretion, proliferation, and cytotoxicity.

Cell Line, Transformed↗