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PubMed1999

New Homochiral Ligands Bearing Nonstereogenic Chirotopic Centers. Lithiated N,N'-Dialkylureas as Chiral Bases and Sterically Crowded Phosphines for Asymmetric Catalysis.

The synthesis of new homochiral pseudo-C(2)()-symmetrical ligands of type 1 bearing a nonstereogenic chirotopic center is reported. Two such structural units are combined in the ureas 2 and 10, which proved to be useful for enantioselective deprotonation and alkylation of ketones (up to 88% ee). The monophosphine 3 induced a high enantiomeric excess in the Pd-catalyzed allylation of dimethyl malonate (up to 73% ee). Furthermore, we have shown that the achiral sterically crowded alkyl diphosphine 23 efficiently stabilized Pd(0) at high temperatures.

Journal Article↗
PubMed2006

Diffusion and viscosity in a crowded environment: from nano- to macroscale.

Although water is the chief component of living cells, food, and personal care products, the supramolecular components make their viscosity larger than that of water by several orders of magnitude. Using fluorescence correlation spectroscopy (FCS), photon correlation spectroscopy (PCS), NMR, and rheology data, we show how the viscosity changes from the value for water at the molecular scale to the large macroviscosity. We determined the viscosity experienced by nanoprobes (of sizes from 0.28 to 190 nm) in aqueous micellar solution of hexaethylene-glycol-monododecyl-ether (in a range of concentration from 0.1% w/w to 35% w/w) and identified a clear crossover at the length scale of 17 +/- 2 nm (slightly larger than persistence length of micelles) at which viscosity acquires its macroscopic value. The sharp dependence of the viscosity coefficients on the size of the probe in the nanoregime has important consequences for diffusion-limited reactions in crowded environments (e.g., living cells).

Journal Article↗
PubMed2005

Looking for foes and friends: perceptual and emotional factors when finding a face in the crowd.

In a face-in-the-crowd setting, the authors examined visual search for photographically reproduced happy, angry, and fearful target faces among neutral distractor faces in 3 separate experiments. Contrary to the hypothesis, happy targets were consistently detected more quickly and accurately than angry and fearful targets, as were directed compared with averted targets. There was no consistent effect of social anxiety. A facial emotion recognition experiment suggested that the happy search advantage could be due to the ease of processing happy faces. In the final experiment with perceptually controlled schematic faces, the authors reported more effective detection of angry than happy faces. This angry advantage was most obvious for highly socially anxious individuals when their social fear was experimentally enhanced.

Adult↗
PubMed2004

Optimal traffic organization in ants under crowded conditions.

Efficient transportation, a hot topic in nonlinear science, is essential for modern societies and the survival of biological species. Biological evolution has generated a rich variety of successful solutions, which have inspired engineers to design optimized artificial systems. Foraging ants, for example, form attractive trails that support the exploitation of initially unknown food sources in almost the minimum possible time. However, can this strategy cope with bottleneck situations, when interactions cause delays that reduce the overall flow? Here, we present an experimental study of ants confronted with two alternative routes. We find that pheromone-based attraction generates one trail at low densities, whereas at a high level of crowding, another trail is established before traffic volume is affected, which guarantees that an optimal rate of food return is maintained. This bifurcation phenomenon is explained by a nonlinear modelling approach. Surprisingly, the underlying mechanism is based on inhibitory interactions. It points to capacity reserves, a limitation of the density-induced speed reduction, and a sufficient pheromone concentration for reliable trail perception. The balancing mechanism between cohesive and dispersive forces appears to be generic in natural, urban and transportation systems.

Animals↗
PubMed2006

Sterically crowded azulene-based dication salts as novel guests: synthesis and complexation studies with crown ethers and calixarenes in solution and in the gas phase.

The 1,4-bis(3-guaiazulenylmethylium)benzene and 1,4-bis[1-(4,6,8-trimethylazulenylmethylium)]benzene dication salts were synthesized via an acid-catalyzed condensation/dehydration protocol with guaiazulene-terephthalaldehyde (2 : 1 ratio), and 4,6,8-trimethylazulene-terephthalaldehyde (2 : 1 ratio) respectively in one-pot processes. A similar condensation reaction with the parent azulene led to an insoluble oligomer that was shown by MALDI-TOF-MS to contain 1,4-bis[(diazulenyl)methylium]benzene as a repeating unit. Dication salts and were fully characterized by 2D NMR and NOE techniques and by electrospray-MS (ES-MS) and MALDI-TOF-MS. NMR studies confirm that the dications are best represented as bis-tropylium species. A delicate balance of electronic (inductive stabilization) and steric influence of the alkyl groups on the seven-membered ring seems to influence the chemo-/regioselectivity of the co-condensation process. NMR titration and T(1) measurements established that, despite its highly crowded structure, dication forms host-guest HG complexes with dibenzo-30-crown-10 (DB30C10) and dibenzo-24-crown-8 (DB24C8) in solution, but fails to complex with the smaller dibenzo-18-crown-6 (DB18C6). The corresponding HG cation-molecule cluster ions were also detected in the gas phase by ES-MS, showing the formation of both dication-crown 1 : 1 and 1 : 2 complexes. Similar complexation of dication salt with DB30C10 was observed via NMR titration and T(1) measurements in solution and by ES-MS in the gas phase. Although solution complexation studies (NMR titration) did not indicate stable complex formation between and p-tert-butyl-methoxycalix[8]arene, their [HG](2+) and [H(2)G](2+) clusters were detectable by ES-MS. Solution decomplexation experiments (HG(2+) --> H + G(2+)) were performed on -crown complex by addition of DMSO, acetone, silver tosylate, and tropylium cation salt. Complexation of with DB30C10 was also studied by microcalorimetric titration.

Calixarenes↗
PubMed1986

Late lower arch crowding. The role of facial morphology.

A study of the relationship between dental crowding and facial morphology in 51 individuals studied over the first five years of the permanent dentition, finding some relationships but no strong or consistent pattern.

Adolescent↗
PubMed1995

Reliability of the Bolton tooth-size analysis when applied to crowded dentitions.

The Bolton tooth-size analysis is widely taught and used in orthodontics. However, its reliability has not been documented. The purpose of this study was to evaluate the reliability of the analysis when performed with needle-pointed dividers and a Boley gauge. Four clinicians measured the teeth on 15 sets of casts with two instruments at two sessions. The measurements were used to calculate tooth-size excess. To evaluate the measurement error, the difference between the two analyses made by the same investigator on the same set of casts was calculated. More of the same-investigator analyses were significantly correlated when the Boley gauge was used than when the needle-pointed dividers were used. Between-investigator analyses revealed significant correlations for each measurement session with both instruments. Every investigator was found to have at least one measurement error for each analysis and with each instrument that was as large as a clinically significant result of a Bolton analysis. The results of this study demonstrate that clinically significant measurement errors can occur when the Bolton tooth-size analysis is performed on casts with at least 3 mm of crowding. The Boley gauge demonstrated a higher frequency of significantly correlated repeated measures and thus may be somewhat more reliable for this analysis than the needle-pointed dividers.

Cuspid↗
PubMed1998

Early versus late treatment of crowded first premolar extraction cases: postretention evaluation of stability and relapse.

The purpose of this study was to evaluate the differences in the long-term stability of orthodontically induced changes in arch form between patients who receive early orthodontic treatment (Hellman's dental age III B, mixed dentition, n = 36) and those who are treated later (Hellman's dental age III C or after, permanent dentition, n = 47). Dental casts were evaluated before treatment, after treatment, and at a minimum of 10 years after retention. All patients had received routine edgewise orthodontic treatment that included maxillary and mandibular first premolar extraction. There were no significant differences between these groups at pretreatment and posttreatment. In the majority of cases, some degree of mandibular crowding occurred during the postretention period. There was a significant difference in the mandibular irregularity index at postretention between these groups. Regarding the deviation of the midline of the central incisors, there were no significant differences between these groups at pretreatment and posttreatment, but there was a significant difference at postretention. At the postretention stage, the late treatment group had greater mandibular anterior irregularity and deviation of the midline.

Adolescent↗
PubMed2005

Diffusion of spheres in crowded suspensions of rods.

Translational tracer diffusion of spherical macromolecules in crowded suspensions of rodlike colloids is investigated. Experiments are done using several kinds of spherical tracers in fd-virus suspensions. A wide range of size ratios L/2a of the length L of the rods and the diameter 2a of the tracer sphere is covered by combining several experimental methods: fluorescence correlation spectroscopy for small tracer spheres, dynamic light scattering for intermediate sized spheres, and video microscopy for large spheres. Fluorescence correlation spectroscopy is shown to measure long-time diffusion only for relatively small tracer spheres. Scaling of diffusion coefficients with a/xi, predicted for static networks, is not found for our dynamical network of rods (with xi the mesh size of the network). Self-diffusion of tracer spheres in the dynamical network of freely suspended rods is thus fundamentally different as compared to cross-linked networks. A theory is developed for the rod-concentration dependence of the translational diffusion coefficient at low rod concentrations for freely suspended rods. The proposed theory is based on a variational solution of the appropriate Smoluchowski equation without hydrodynamic interactions. The theory can, in principle, be further developed to describe diffusion through dynamical networks at higher rod concentrations with the inclusion of hydrodynamic interactions. Quantitative agreement with the experiments is found for large tracer spheres, and qualitative agreement for smaller spheres. This is probably due to the increasing importance of hydrodynamic interactions as compared to direct interactions as the size of the tracer sphere decreases.

Journal Article↗
PubMed2002

Evaluation of the relationship between the anterior component of occlusal force and postretention crowding.

The aim of this study was to investigate whether a relationship exists between the anterior component of occlusal force (ACF) and postretention crowding in the mandibular incisor area. The study group comprised 32 adults who had undergone fixed orthodontic treatment in the department clinic at Marmara University in Istanbul, Turkey. In 13 subjects, the mandibular arch was treated without extractions; in 19, it was treated with bilateral first premolar extractions. The average postretention period was 3.5 years. The ACF created in the left side of the mandibular dentition was determined by measuring interdental frictional forces at each contact point mesial to the first molar and distal to the canine. Anatomic contact point displacements between the left mandibular anterior teeth (lateral incisor-canine, central incisor-lateral incisor, and central incisor-central incisor) were measured on plaster casts and summed to provide the irregularity index for these teeth. Correlation analysis was used to assess the relationship between the ACF values at each contact and the irregularity index. In the nonextraction group, statistically significant positive correlations were observed between the ACF and the irregularity index at the 3 contact points that were measured. The strongest correlation was found at the canine-first premolar contact (r = 0.65). In the extraction group, a positive correlation was found between the ACF and the irregularity index (r = 0.49, P <.05) at the second premolar-first molar contact, but no correlation was found at the canine-second premolar contact.

Adolescent↗
PubMed2002

Treatment of a patient with a crowded Class I malocclusion and a congenitally missing mandibular incisor.

This case report describes the management of maxillary and mandibular crowding in a patient with facial esthetic concerns and a tooth-size discrepancy due to a missing mandibular central incisor. The treatment included extracting the remaining mandibular central incisor and the 2 maxillary first premolars. The mandibular canines were repositioned to substitute for lateral incisors, and the mandibular premolars were used as canines.

Adolescent↗
PubMed1996

It takes a confounded face to pop out of a crowd.

It is widely reported that a picture of an angry face seems to figuratively pop out of an array of happy faces, although all of these reports are based on a single experiment by Hansen and Hansen. Pop out, when it occurs, indicates that an observer has located the target by means of a preattentive, parallel search. Hansen and Hansen concluded that it was the affect displayed by the face which caused it to pop out from its surrounding distracters. However, Hansen and Hansen's angry faces contained extraneous dark areas which were introduced when they transformed Ekman and Friesen's photographs of angry and happy faces into black-on-white sketches. When the original artifact-free gray-scaled versions of angry and happy faces were used no evidence for pop out was found. All target faces were found during a serial, self-terminating search regardless of their expression. The angry face in Hansen and Hansen's experiments may have popped out from a crowd of happy faces because of a contrast artifact inadvertently introduced when they created their stimuli.

Artifacts↗
PubMed1983

Macromolecular crowding allows blunt-end ligation by DNA ligases from rat liver or Escherichia coli.

In the presence of high concentrations of any of several types of macromolecules, DNA ligase preparations from rat liver nuclei or from Escherichia coli actively catalyze the blunt-end ligation of DNA. This is in contrast to the lack of activity on such substrates by these enzymes under conventional assay conditions. In addition, the previously established activity of T4 DNA ligase on blunt-ended molecules is greatly increased in the presence of high concentrations of macromolecules. Because such crowded solutions may well be a more adequate model for intracellular conditions than assays in dilute solutions, we suggest that blunt-end ligation may be a widely occurring reaction in vivo.

Animals↗
PubMed1992

Model for the role of macromolecular crowding in regulation of cellular volume.

A simple model is proposed to account for large increases in transporter-mediated ion flux across cell membranes that are elicited by small fractional changes of cell volume. The model is based upon the concept that, as a result of large excluded volume effects in cytoplasm (macromolecular crowding), the tendency of soluble macromolecules to associate with membrane proteins is much more sensitive to changes in cell water content than expected on the basis of simple considerations of mass action. The model postulates that an ion transporter may exist in either an active dephosphorylated state or an inactive phosphorylated state and that the steady-state activity of the transporter reflects a balance between the rates of phosphatase-catalyzed activation and kinase-catalyzed inactivation. Cell swelling results in the inhibition of kinase relative to phosphatase activity, thereby increasing the steady-state concentration of the active form of the transporter. Calculated volume-dependent stimulation of ion flux is comparable to that observed experimentally.

Animals↗
PubMed1997

The effect of macromolecular crowding on chaperonin-mediated protein folding.

The cylindrical chaperonin GroEL and its cofactor GroES mediate ATP-dependent protein folding in Escherichia coli. Recent studies in vitro demonstrated that GroES binding to GroEL causes the displacement of unfolded polypeptide into the central volume of the GroEL cavity for folding in a sequestrated environment. Resulting native protein leaves GroEL upon GroES release, whereas incompletely folded polypeptide can be recaptured for structural rearrangement followed by another folding trial. Additionally, each cycle of GroES binding and dissociation is associated with the release of nonnative polypeptide into the bulk solution. Here we show that this loss of substrate from GroEL is prevented when the folding reaction is carried out in the presence of macromolecular crowding agents, such as Ficoll and dextran, or in a dense cytosolic solution. Thus, the release of nonnative polypeptide is not an essential feature of the productive chaperonin mechanism. Our results argue that conditions of excluded volume, thought to prevail in the bacterial cytosol, increase the capacity of the chaperonin to retain nonnative polypeptide throughout successive reaction cycles. We propose that the leakiness of the chaperonin system under physiological conditions is adjusted such that E. coli proteins are likely to complete folding without partitioning between different GroEL complexes. Polypeptides that are unable to fold on GroEL eventually will be transferred to other chaperones or the degradation machinery.

Chaperonin 10↗
PubMed2000

Osmotic stress, crowding, preferential hydration, and binding: A comparison of perspectives.

There has been much confusion recently about the relative merits of different approaches, osmotic stress, preferential interaction, and crowding, to describe the indirect effect of solutes on macromolecular conformations and reactions. To strengthen all interpretations of measurements and to forestall further unnecessary conceptual or linguistic confusion, we show here how the different perspectives all can be reconciled. Our approach is through the Gibbs-Duhem relation, the universal constraint on the number of ways it is possible to change the temperature, pressure, and chemical potentials of the several components in any thermodynamically defined system. From this general Gibbs-Duhem equation, it is possible to see the equivalence of the different perspectives and even to show the precise identity of the more specialized equations that the different approaches use.

Binding Sites↗
PubMed1994

Crowding-induced organization of cytoskeletal elements: II. Dissolution of spontaneously formed filament bundles by capping proteins.

Through calculations of molecular packing constraints in crowded solutions, we have previously shown that dispersions of filament forming proteins and soluble proteins can be unstable at physiological concentrations, such that tight bundles of filaments are formed spontaneously, in the absence of any accessory binding proteins. Here we consider the modulation of this phenomenon by capping proteins. The theory predicts that, by shortening the average filament length, capping alleviates the packing problem. As a result, the dispersed isotropic solution is stable over an expanded range of compositions.

Actin Depolymerizing Factors↗