@article{3399, abstract = {Context-dependent adjustment of mating tactics can drastically increase the mating success of behaviourally flexible animals. We used the ant Cardiocondyla obscurior as a model system to study adaptive adjustment of male mating tactics. This species shows a male diphenism of wingless fighter males and peaceful winged males. Whereas the wingless males stay and exclusively mate in the maternal colony, the mating behaviour of winged males is plastic. They copulate with female sexuals in their natal nests early in life but later disperse in search for sexuals outside. In this study, we observed the nest-leaving behaviour of winged males under different conditions and found that they adaptively adjust the timing of their dispersal to the availability of mating partners, as well as the presence, and even the type of competitors in their natal nests. In colonies with virgin female queens winged males stayed longest when they were the only male in the nest. They left earlier when mating partners were not available or when other males were present. In the presence of wingless, locally mating fighter males, winged males dispersed earlier than in the presence of docile, winged competitors. This suggests that C. obscurior males are capable of estimating their local breeding chances and adaptively adjust their dispersal behaviour in both an opportunistic and a risk-sensitive way, thus showing hitherto unknown behavioural plasticity in social insect males.}, author = {Cremer, Sylvia and Schrempf, Alexandra and Heinze, Jürgen}, journal = {PLoS One}, number = {3}, publisher = {Public Library of Science}, title = {{Competition and opportunity shape the reproductive tactics of males in the ant Cardiocondyla obscurior}}, doi = {10.1371/journal.pone.0017323}, volume = {6}, year = {2011}, } @article{3401, abstract = {The Bicoid morphogen gradient directs the patterning of cell fates along the anterior-posterior axis of the syncytial Drosophila embryo and serves as a paradigm of morphogen-mediated patterning. The simplest models of gradient formation rely on constant protein synthesis and diffusion from anteriorly localized source mRNA, coupled with uniform protein degradation. However, currently such models cannot account for all known gradient characteristics. Recent work has proposed that bicoid mRNA spatial distribution is sufficient to produce the observed protein gradient, minimizing the role of protein transport. Here, we adapt a novel method of fluorescent in situ hybridization to quantify the global spatio-temporal dynamics of bicoid mRNA particles. We determine that >90% of all bicoid mRNA is continuously present within the anterior 20% of the embryo. bicoid mRNA distribution along the body axis remains nearly unchanged despite dynamic mRNA translocation from the embryo core to the cortex. To evaluate the impact of mRNA distribution on protein gradient dynamics, we provide detailed quantitative measurements of nuclear Bicoid levels during the formation of the protein gradient. We find that gradient establishment begins 45 minutes after fertilization and that the gradient requires about 50 minutes to reach peak levels. In numerical simulations of gradient formation, we find that incorporating the actual bicoid mRNA distribution yields a closer prediction of the observed protein dynamics compared to modeling protein production from a point source at the anterior pole. We conclude that the spatial distribution of bicoid mRNA contributes to, but cannot account for, protein gradient formation, and therefore that protein movement, either active or passive, is required for gradient formation.}, author = {Little, Shawn and Tkacik, Gasper and Kneeland, Thomas and Wieschaus, Eric and Gregor, Thomas}, journal = {PLoS Biology}, number = {3}, publisher = {Public Library of Science}, title = {{The formation of the Bicoid morphogen gradient requires protein movement from anteriorly localized source}}, doi = {10.1371/journal.pbio.1000596}, volume = {9}, year = {2011}, } @article{3405, abstract = {Glutamate is the major excitatory neurotransmitter in the mammalian central nervous system and gates non-selective cation channels. The origins of glutamate receptors are not well understood as they differ structurally and functionally from simple bacterial ligand-gated ion channels. Here we report the discovery of an ionotropic glutamate receptor that combines the typical eukaryotic domain architecture with the 'TXVGYG' signature sequence of the selectivity filter found in K+ channels. This receptor exhibits functional properties intermediate between bacterial and eukaryotic glutamate-gated ion channels, suggesting a link in the evolution of ionotropic glutamate receptors.}, author = {Janovjak, Harald L and Sandoz, Guillaume and Isacoff, Ehud}, journal = {Nature Communications}, number = {232}, pages = {1 -- 6}, publisher = {Nature Publishing Group}, title = {{Modern ionotropic glutamate receptor with a K+ selectivity signature sequence}}, doi = {10.1038/ncomms1231}, volume = {2}, year = {2011}, } @article{341, abstract = {An oriented attachment and growth mechanism allows an accurate control of the size and morphology of Cu2-xS nanocrystals, from spheres and disks to tetradecahedrons and dodecahedrons. The synthesis conditions and the growth mechanism are detailed here.}, author = {Li, Wenhua and Shavel, Alexey and Guzman, Roger and Rubio Garcia, Javier and Flox, Cristina and Fan, Jiandong and Cadavid, Doris and Ibáñez, Maria and Arbiol, Jordi and Morante, Joan and Cabot, Andreu}, journal = {Chemical Communications}, number = {37}, pages = {10332 -- 10334}, publisher = {Royal Society of Chemistry (RSC) }, title = {{Morphology evolution of Cu2−xS nanoparticles: from spheres to dodecahedrons}}, doi = {10.1039/c1cc13803k}, volume = {47}, year = {2011}, } @article{14305, abstract = {Understanding the mechanism of protein folding requires a detailed knowledge of the structural properties of the barriers separating unfolded from native conformations. The S-peptide from ribonuclease S forms its α-helical structure only upon binding to the folded S-protein. We characterized the transition state for this binding-induced folding reaction at high resolution by determining the effect of site-specific backbone thioxylation and side-chain modifications on the kinetics and thermodynamics of the reaction, which allows us to monitor formation of backbone hydrogen bonds and side-chain interactions in the transition state. The experiments reveal that α-helical structure in the S-peptide is absent in the transition state of binding. Recognition between the unfolded S-peptide and the S-protein is mediated by loosely packed hydrophobic side-chain interactions in two well defined regions on the S-peptide. Close packing and helix formation occurs rapidly after binding. Introducing hydrophobic residues at positions outside the recognition region can drastically slow down association.}, author = {Bachmann, Annett and Wildemann, Dirk and Praetorius, Florian M and Fischer, Gunter and Kiefhaber, Thomas}, issn = {1091-6490}, journal = {PNAS}, keywords = {Multidisciplinary}, number = {10}, pages = {3952--3957}, publisher = {Proceedings of the National Academy of Sciences}, title = {{Mapping backbone and side-chain interactions in the transition state of a coupled protein folding and binding reaction}}, doi = {10.1073/pnas.1012668108}, volume = {108}, year = {2011}, } @article{1467, abstract = {We propose a general conjecture for the mixed Hodge polynomial of the generic character varieties of representations of the fundamental group of a Riemann surface of genus g to GLn(C) with fixed generic semisimple conjugacy classes at k punctures. This conjecture generalizes the Cauchy identity for Macdonald polynomials and is a common generalization of two formulas that we prove in this paper. The first is a formula for the E-polynomial of these character varieties which we obtain using the character table of GLn(Fq). We use this formula to compute the Euler characteristic of character varieties. The second formula gives the Poincaré polynomial of certain associated quiver varieties which we obtain using the character table of gln(Fq). In the last main result we prove that the Poincaré polynomials of the quiver varieties equal certain multiplicities in the tensor product of irreducible characters of GLn(Fq). As a consequence we find a curious connection between Kac-Moody algebras associated with comet-shaped, and typically wild, quivers and the representation theory of GLn(Fq).}, author = {Tamas Hausel and Letellier, Emmanuel and Rodríguez Villegas, Fernando}, journal = {Duke Mathematical Journal}, number = {2}, pages = {323 -- 400}, publisher = {Duke University Press}, title = {{Arithmetic harmonic analysis on character and quiver varieties}}, doi = {10.1215/00127094-1444258}, volume = {160}, year = {2011}, } @article{1781, abstract = {Microwave cavities with high quality factors enable coherent coupling of distant quantum systems. Virtual photons lead to a transverse interaction between qubits when they are nonresonant with the cavity but resonant with each other. We experimentally investigate the inverse scaling of the interqubit coupling with the detuning from a cavity mode and its proportionality to the qubit-cavity interaction strength. We demonstrate that the enhanced coupling at higher frequencies is mediated by multiple higher-harmonic cavity modes. Moreover, we observe dark states of the coupled qubit-qubit system and analyze their relation to the symmetry of the applied driving field at different frequencies.}, author = {Filipp, Stefan and Göppl, M and Johannes Fink and Baur, Matthias P and Bianchetti, R and Steffen, L. Kraig and Wallraff, Andreas}, journal = {Physical Review A - Atomic, Molecular, and Optical Physics}, number = {6}, publisher = {American Physical Society}, title = {{Multimode mediated qubit-qubit coupling and dark-state symmetries in circuit quantum electrodynamics}}, doi = {10.1103/PhysRevA.83.063827}, volume = {83}, year = {2011}, } @article{18012, abstract = {We report the first concurrent determination of conductance (G) and thermopower (S) of single-molecule junctions via direct measurement of electrical and thermoelectric currents using a scanning tunneling microscope-based break-junction technique. We explore several amine-Au and pyridine-Au linked molecules that are predicted to conduct through either the highest occupied molecular orbital (HOMO) or the lowest unoccupied molecular orbital (LUMO), respectively. We find that the Seebeck coefficient is negative for pyridine-Au linked LUMO-conducting junctions and positive for amine-Au linked HOMO-conducting junctions. Within the accessible temperature gradients (<30 K), we do not observe a strong dependence of the junction Seebeck coefficient on temperature. From histograms of thousands of junctions, we use the most probable Seebeck coefficient to determine a power factor, GS2, for each junction studied, and find that GS2 increases with G. Finally, we find that conductance and Seebeck coefficient values are in good quantitative agreement with our self-energy corrected density functional theory calculations.}, author = {Widawsky, Jonathan R. and Darancet, Pierre and Neaton, Jeffrey B. and Venkataraman, Latha}, issn = {1530-6992}, journal = {Nano Letters}, number = {1}, pages = {354--358}, publisher = {American Chemical Society}, title = {{Simultaneous determination of conductance and thermopower of single molecule junctions}}, doi = {10.1021/nl203634m}, volume = {12}, year = {2011}, } @article{18014, abstract = {We measure electronic conductance through single conjugated molecules bonded to Au metal electrodes with direct Au–C covalent bonds using the scanning tunneling microscope based break-junction technique. We start with molecules terminated with trimethyltin end groups that cleave off in situ, resulting in formation of a direct covalent σ bond between the carbon backbone and the gold metal electrodes. The molecular carbon backbone used in this study consist of a conjugated π system that has one terminal methylene group on each end, which bonds to the electrodes, achieving large electronic coupling of the electrodes to the π system. The junctions formed with the prototypical example of 1,4-dimethylenebenzene show a conductance approaching one conductance quantum (G0 = 2e2/h). Junctions formed with methylene-terminated oligophenyls with two to four phenyl units show a 100-fold increase in conductance compared with junctions formed with amine-linked oligophenyls. The conduction mechanism for these longer oligophenyls is tunneling, as they exhibit an exponential dependence of conductance on oligomer length. In addition, density functional theory based calculations for the Au–xylylene–Au junction show near-resonant transmission, with a crossover to tunneling for the longer oligomers.}, author = {Chen, Wenbo and Widawsky, Jonathan R. and Vázquez, Héctor and Schneebeli, Severin T. and Hybertsen, Mark S. and Breslow, Ronald and Venkataraman, Latha}, issn = {1520-5126}, journal = {Journal of the American Chemical Society}, number = {43}, pages = {17160--17163}, publisher = {American Chemical Society}, title = {{Highly conducting π-conjugated molecular junctions covalently bonded to gold electrodes}}, doi = {10.1021/ja208020j}, volume = {133}, year = {2011}, } @article{18015, abstract = {We investigate the binding and energy level alignment of 2,3,5,6-tetramethyl-1,4-benzenediamine (TMBDA) on Au(111) through a combination of helium atom scattering (HAS), X-ray photoemission (XPS), and scanning tunneling microscopy (STM). We show that TMBDA binds to step edges and to flat Au (111) terraces in a nearly flat-lying configuration. Through combination of HAS and STM data, we determine that the molecules are bound on step edges with an adsorption energy of about 1.2 eV, which is about 0.2 eV stronger than the adsorption energy we measure on flat surface. Preferential bonding to the under-coordinated Au atoms on step edges suggests that the molecules bind to Au through the nitrogen lone pair. Finally, STM measurements on TMBDA in these two different adsorption configurations show that the highest-occupied molecular orbital is deeper relative to Fermi for the more strongly bound molecules on step edges, confirming that the nitrogen bonds through charge donation to the Au.}, author = {Kamenetska, M. and Dell’Angela, M. and Widawsky, J.R. and Kladnik, G. and Verdini, A. and Cossaro, A. and Cvetko, D. and Morgante, A. and Venkataraman, Latha}, issn = {1932-7455}, journal = {The Journal of Physical Chemistry C}, number = {25}, pages = {12625--12630}, publisher = {American Chemical Society}, title = {{Structure and energy level alignment of tetramethyl benzenediamine on Au(111)}}, doi = {10.1021/jp202555d}, volume = {115}, year = {2011}, } @article{18016, abstract = {Understanding the electrical properties of semiconducting quantum dot devices have been limited due to the variability of their size/composition and the chemistry of ligand/electrode binding. Furthermore, to probe their electrical conduction properties and its dependence on ligand/electrode binding, measurements must be carried out at the single dot/cluster level. Herein we report scanning tunneling microscope based break junction measurements of cobalt chalcogenide clusters with Te, Se and S to probe the conductance properties. Our measured conductance trends show that the Co–Te based clusters have the highest conductance while the Co-S clusters the lowest. These trends are in very good agreement with cyclic voltammetry measurements of the first oxidation potentials and with density functional theory calculations of their HOMO–LUMO gaps.}, author = {Boardman, Brycelyn M. and Widawsky, Jonathan R. and Park, Young S. and Schenck, Christine L. and Venkataraman, Latha and Steigerwald, Michael L. and Nuckolls, Colin}, issn = {1520-5126}, journal = {Journal of the American Chemical Society}, number = {22}, pages = {8455--8457}, publisher = {American Chemical Society}, title = {{Conductance of single cobalt chalcogenide cluster junctions}}, doi = {10.1021/ja201334s}, volume = {133}, year = {2011}, } @article{18017, abstract = {The conductance of individual 1,4-benzenediamine (BDA)–Au molecular junctions is measured in different solvent environments using a scanning tunneling microscope based point-contact technique. Solvents are found to increase the conductance of these molecular junctions by as much as 50%. Using first principles calculations, we explain this increase by showing that a shift in the Au contact work function is induced by solvents binding to undercoordinated Au sites around the junction. Increasing the Au contact work function reduces the separation between the Au Fermi energy and the highest occupied molecular orbital of BDA in the junction, increasing the measured conductance. We demonstrate that the solvent-induced shift in conductance depends on the affinity of the solvent to Au binding sites and also on the induced dipole (relative to BDA) upon adsorption. Via this mechanism, molecular junction level alignment and transport properties can be statistically altered by solvent molecule binding to the contact surface.}, author = {Fatemi, V. and Kamenetska, M. and Neaton, J. B. and Venkataraman, Latha}, issn = {1530-6992}, journal = {Nano Letters}, number = {5}, pages = {1988--1992}, publisher = {American Chemical Society}, title = {{Environmental control of single-molecule junction transport}}, doi = {10.1021/nl200324e}, volume = {11}, year = {2011}, } @article{18018, abstract = {Controlling electron transport through a single-molecule device is key to the realization of nanoscale electronic components. A design requirement for single molecule electrical devices is that the molecule must be both structurally and electrically connected to the metallic electrodes. Typically, the mechanical and electrical contacts are achieved by the same chemical moiety. In this study, we demonstrate that the structural role may be played by one group (for example, a sulfide) while the electrical role may be played by another (a conjugated chain of C═C π-bonds). We can specify the electrical conductance through the molecule by modulating to which particular site on the oligoene chain the electrode binds. The result is a device that functions as a potentiometer at the single-molecule level.}, author = {Meisner, Jeffrey S. and Kamenetska, Masha and Krikorian, Markrete and Steigerwald, Michael L. and Venkataraman, Latha and Nuckolls, Colin}, issn = {1530-6992}, journal = {Nano Letters}, number = {4}, pages = {1575--1579}, publisher = {American Chemical Society}, title = {{A single-molecule potentiometer}}, doi = {10.1021/nl104411f}, volume = {11}, year = {2011}, } @article{18019, abstract = {We simultaneously measure conductance and force across nanoscale junctions. A new, two-dimensional histogram technique is introduced to statistically extract bond rupture forces from a large data set of individual junction elongation traces. For the case of Au point contacts, we find a rupture force of 1.4 ± 0.2 nN, which is in good agreement with previous measurements. We then study systematic trends for single gold metal−molecule−metal junctions for a series of molecules terminated with amine and pyridine linkers. For all molecules studied, single molecule junctions rupture at the Au−N bond. Selective binding of the linker group allows us to correlate the N−Au bond-rupture force to the molecular backbone. We find that the rupture force ranges from 0.8 nN for 4,4′ bipyridine to 0.5 nN in 1,4 diaminobenzene. These experimental results are in excellent quantitative agreement with density functional theory based adiabatic molecular junction elongation and rupture calculations.}, author = {Frei, Michael and Aradhya, Sriharsha V. and Koentopp, Max and Hybertsen, Mark S. and Venkataraman, Latha}, issn = {1530-6992}, journal = {Nano Letters}, number = {4}, pages = {1518--1523}, publisher = {American Chemical Society}, title = {{Mechanics and chemistry: Single molecule bond rupture forces correlate with molecular backbone structure}}, doi = {10.1021/nl1042903}, volume = {11}, year = {2011}, } @article{18020, abstract = {Understanding electron transport across π−π-stacked systems will help to answer fundamental questions about biochemical redox processes and benefit the design of new materials and molecular devices. Herein we employed the STM break-junction technique to measure the single-molecule conductance of multiple π−π-stacked aromatic rings. We studied electron transport through up to four stacked benzene rings held together in an eclipsed fashion via a paracyclophane scaffold. We found that the strained hydrocarbons studied herein couple directly to gold electrodes during the measurements; hence, we did not require any heteroatom binding groups as electrical contacts. Density functional theory-based calculations suggest that the gold atoms of the electrodes bind to two neighboring carbon atoms of the outermost cyclophane benzene rings in η2 fashion. Our measurements show an exponential decay of the conductance with an increasing number of stacked benzene rings, indicating a nonresonant tunneling mechanism. Furthermore, STM tip−substrate displacement data provide additional evidence that the electrodes bind to the outermost benzene rings of the π−π-stacked molecular wires.}, author = {Schneebeli, Severin T. and Kamenetska, Maria and Cheng, Zhanling and Skouta, Rachid and Friesner, Richard A. and Venkataraman, Latha and Breslow, Ronald}, issn = {1520-5126}, journal = {Journal of the American Chemical Society}, number = {7}, pages = {2136--2139}, publisher = {American Chemical Society}, title = {{Single-molecule conductance through multiple π−π-stacked benzene rings determined with direct electrode-to-benzene ring connections}}, doi = {10.1021/ja111320n}, volume = {133}, year = {2011}, } @article{18021, abstract = {Charge transport across metal–molecule interfaces has an important role in organic electronics1. Typically, chemical link groups such as thiols2 or amines3 are used to bind organic molecules to metal electrodes in single-molecule circuits, with these groups controlling both the physical structure and the electronic coupling at the interface. Direct metal–carbon coupling has been shown through C60, benzene and π-stacked benzene4,5,6,7, but ideally the carbon backbone of the molecule should be covalently bonded to the electrode without intervening link groups. Here, we demonstrate a method to create junctions with such contacts. Trimethyl tin (SnMe3)-terminated polymethylene chains are used to form single-molecule junctions with a break-junction technique2,3. Gold atoms at the electrode displace the SnMe3 linkers, leading to the formation of direct Au–C bonded single-molecule junctions with a conductance that is ∼100 times larger than analogous alkanes with most other terminations. The conductance of these Au–C bonded alkanes decreases exponentially with molecular length, with a decay constant of 0.97 per methylene, consistent with a non-resonant transport mechanism. Control experiments and ab initio calculations show that high conductances are achieved because a covalent Au–C sigma (σ) bond is formed. This offers a new method for making reproducible and highly conducting metal–organic contacts.}, author = {Cheng, Z.-L. and Skouta, R. and Vazquez, H. and Widawsky, J. R. and Schneebeli, S. and Chen, W. and Hybertsen, M. S. and Breslow, R. and Venkataraman, Latha}, issn = {1748-3395}, journal = {Nature Nanotechnology}, number = {6}, pages = {353--357}, publisher = {Springer Nature}, title = {{In situ formation of highly conducting covalent Au–C contacts for single-molecule junctions}}, doi = {10.1038/nnano.2011.66}, volume = {6}, year = {2011}, } @article{1815, abstract = {Many membrane channels and receptors exhibit adaptive, or desensitized, response to a strong sustained input stimulus, often supported by protein activity-dependent inactivation. Adaptive response is thought to be related to various cellular functions such as homeostasis and enlargement of dynamic range by background compensation. Here we study the quantitative relation between adaptive response and background compensation within a modeling framework. We show that any particular type of adaptive response is neither sufficient nor necessary for adaptive enlargement of dynamic range. In particular a precise adaptive response, where system activity is maintained at a constant level at steady state, does not ensure a large dynamic range neither in input signal nor in system output. A general mechanism for input dynamic range enlargement can come about from the activity-dependent modulation of protein responsiveness by multiple biochemical modification, regardless of the type of adaptive response it induces. Therefore hierarchical biochemical processes such as methylation and phosphorylation are natural candidates to induce this property in signaling systems.}, author = {Tamar Friedlander and Brenner, Naama}, journal = {Mathematical Biosciences and Engineering}, number = {2}, pages = {515 -- 526}, publisher = {Arizona State University}, title = {{Adaptive response and enlargement of dynamic range}}, doi = {10.3934/mbe.2011.8.515}, volume = {8}, year = {2011}, } @article{18362, abstract = {Maximally stable component detection is a very popular method for feature analysis in images, mainly due to its low computation cost and high repeatability. With the recent advance of feature-based methods in geometric shape analysis, there is significant interest in finding analogous approaches in the 3D world. In this paper, we formulate a diffusion-geometric framework for stable component detection in non-rigid 3D shapes, which can be used for geometric feature detection and description. A quantitative evaluation of our method on the SHREC’10 feature detection benchmark shows its potential as a source of high-quality features.}, author = {Litman, Roee and Bronstein, Alexander and Bronstein, Michael M.}, issn = {0097-8493}, journal = {Computers & Graphics}, number = {3}, pages = {549--560}, publisher = {Elsevier}, title = {{Diffusion-geometric maximally stable component detection in deformable shapes}}, doi = {10.1016/j.cag.2011.03.011}, volume = {35}, year = {2011}, } @article{18363, abstract = {Natural objects can be subject to various transformations yet still preserve properties that we refer to as invariants. Here, we use definitions of affine-invariant arclength for surfaces in in order to extend the set of existing non-rigid shape analysis tools. We show that by re-defining the surface metric as its equi-affine version, the surface with its modified metric tensor can be treated as a canonical Euclidean object on which most classical Euclidean processing and analysis tools can be applied. The new definition of a metric is used to extend the fast marching method technique for computing geodesic distances on surfaces, where now, the distances are defined with respect to an affine-invariant arclength. Applications of the proposed framework demonstrate its invariance, efficiency, and accuracy in shape analysis.}, author = {Raviv, Dan and Bronstein, Alexander and Bronstein, Michael M. and Kimmel, Ron and Sochen, Nir}, issn = {0097-8493}, journal = {Computers & Graphics}, number = {3}, pages = {692--697}, publisher = {Elsevier}, title = {{Affine-invariant geodesic geometry of deformable 3D shapes}}, doi = {10.1016/j.cag.2011.03.030}, volume = {35}, year = {2011}, } @inproceedings{18377, abstract = {We introduce an (equi-)affine invariant diffusion geometry by which surfaces that go through squeeze and shear transformations can still be properly analyzed. The definition of an affine invariant metric enables us to construct an invariant Laplacian from which local and global geometric structures are extracted. Applications of the proposed framework demonstrate its power in generalizing and enriching the existing set of tools for shape analysis.}, author = {Raviv, Dan and Bronstein, Michael M. and Bronstein, Alexander and Kimmel, Ron and Sochen, Nir}, booktitle = {CVPR 2011}, isbn = {9781457703942}, issn = {1063-6919}, location = {Colorado Springs, CO, United States}, publisher = {IEEE}, title = {{Affine-invariant diffusion geometry for the analysis of deformable 3D shapes}}, doi = {10.1109/cvpr.2011.5995486}, year = {2011}, }