@article{11985, abstract = {Hydrocodone, a high value active pharmaceutical ingredient (API), is usually produced in a semisynthetic pathway from morphine, codeine or thebaine. The latter alkaloid is an attractive precursor as it is not used as a remedy itself. The key step in this production route is a selective olefin reduction forming 8,14-dihydrothebaine which can be subsequently hydrolyzed to yield hydrocodone. Unfortunately, standard hydrogenation procedures cannot be applied due to severe selectivity problems. A transfer hydrogenation using in situ generated diimide is the only known alternative to achieve a selective transformation. The most (atom) economic generation of this highly unstable reducing agent is by oxidizing hydrazine hydrate (N2H4·H2O) with O2. In the past, this route was “forbidden” on an industrial scale due to its enormous explosion potential in batch. A continuous high-temperature/high-pressure methodology allows an efficient, safe, and scalable processing of the hazardous reaction mixture. The industrially relevant reduction was achieved by using four consecutive liquid feeds (of N2H4·H2O) and residence time units, resulting in a highly selective reduction within less than 1 h.}, author = {Pieber, Bartholomäus and Cox, D. Phillip and Kappe, C. Oliver}, issn = {1520-586X}, journal = {Organic Process Research and Development}, number = {2}, pages = {376--385}, publisher = {American Chemical Society}, title = {{Selective olefin reduction in thebaine using hydrazine hydrate and O₂ under intensified continuous flow conditions}}, doi = {10.1021/acs.oprd.5b00370}, volume = {20}, year = {2016}, } @article{11988, abstract = {A continuous Bucherer–Bergs hydantoin synthesis utilizing intensified conditions is reported. The methodology is characterized by a two-feed flow approach to independently feed the organic substrate and the aqueous reagent solution. The increased interfacial area of the biphasic reaction mixture and the lack of headspace enabled almost quantitative conversions within ca. 30 minutes at 120 °C and 20 bar even for unpolar starting materials. In addition, a selective N(3)-monoalkylation of the resulting heterocycles under batch microwave conditions is reported yielding potential acetylcholinesterase inhibitors.}, author = {Kappe, C. and Monteiro, Julia and Pieber, Bartholomäus and Corrêa, Arlene}, issn = {1437-2096}, journal = {Synlett}, number = {01}, pages = {83--87}, publisher = {Georg Thieme Verlag}, title = {{Continuous synthesis of hydantoins: Intensifying the Bucherer–Bergs reaction}}, doi = {10.1055/s-0035-1560317}, volume = {27}, year = {2016}, } @article{1200, author = {Hilbe, Christian and Traulsen, Arne}, journal = {Physics of Life Reviews}, pages = {29 -- 31}, publisher = {Elsevier}, title = {{Only the combination of mathematics and agent based simulations can leverage the full potential of evolutionary modeling: Comment on “Evolutionary game theory using agent-based methods” by C. Adami, J. Schossau and A. Hintze}}, doi = {10.1016/j.plrev.2016.10.004}, volume = {19}, year = {2016}, } @article{1201, abstract = {In this issue of Cell, Skau et al. show that the formin FMN2 organizes a perinuclear actin cytoskeleton that protects the nucleus and its genomic content of migrating cells squeezing through small spaces.}, author = {Renkawitz, Jörg and Sixt, Michael K}, journal = {Cell}, number = {6}, pages = {1448 -- 1449}, publisher = {Cell Press}, title = {{Formin’ a nuclear protection}}, doi = {10.1016/j.cell.2016.11.024}, volume = {167}, year = {2016}, } @article{1202, author = {Milutinovic, Barbara and Peuß, Robert and Ferro, Kevin and Kurtz, Joachim}, journal = {Zoology }, number = {4}, pages = {254 -- 261}, publisher = {Elsevier}, title = {{Immune priming in arthropods: an update focusing on the red flour beetle}}, doi = {10.1016/j.zool.2016.03.006}, volume = {119}, year = {2016}, } @article{1203, abstract = {Haemophilus haemolyticus has been recently discovered to have the potential to cause invasive disease. It is closely related to nontypeable Haemophilus influenzae (NT H. influenzae). NT H. influenzae and H. haemolyticus are often misidentified because none of the existing tests targeting the known phenotypes of H. haemolyticus are able to specifically identify H. haemolyticus. Through comparative genomic analysis of H. haemolyticus and NT H. influenzae, we identified genes unique to H. haemolyticus that can be used as targets for the identification of H. haemolyticus. A real-time PCR targeting purT (encoding phosphoribosylglycinamide formyltransferase 2 in the purine synthesis pathway) was developed and evaluated. The lower limit of detection was 40 genomes/PCR; the sensitivity and specificity in detecting H. haemolyticus were 98.9% and 97%, respectively. To improve the discrimination of H. haemolyticus and NT H. influenzae, a testing scheme combining two targets (H. haemolyticus purT and H. influenzae hpd, encoding protein D lipoprotein) was also evaluated and showed 96.7% sensitivity and 98.2% specificity for the identification of H. haemolyticus and 92.8% sensitivity and 100% specificity for the identification of H. influenzae, respectively. The dual-target testing scheme can be used for the diagnosis and surveillance of infection and disease caused by H. haemolyticus and NT H. influenzae.}, author = {Hu, Fang and Rishishwar, Lavanya and Sivadas, Ambily and Mitchell, Gabriel and King, Jordan and Murphy, Timothy and Gilsdorf, Janet and Mayer, Leonard and Wang, Xin}, journal = {Journal of Clinical Microbiology}, number = {12}, pages = {3010 -- 3017}, publisher = {American Society for Microbiology}, title = {{Comparative genomic analysis of Haemophilus haemolyticus and nontypeable Haemophilus influenzae and a new testing scheme for their discrimination}}, doi = {10.1128/JCM.01511-16}, volume = {54}, year = {2016}, } @article{1204, abstract = {In science, as in life, "surprises" can be adequately appreciated only in the presence of a null model, what we expect a priori. In physics, theories sometimes express the values of dimensionless physical constants as combinations of mathematical constants like π or e. The inverse problem also arises, whereby the measured value of a physical constant admits a "surprisingly" simple approximation in terms of well-known mathematical constants. Can we estimate the probability for this to be a mere coincidence, rather than an inkling of some theory? We answer the question in the most naive form.}, author = {Amir, Ariel and Lemeshko, Mikhail and Tokieda, Tadashi}, journal = {American Mathematical Monthly}, number = {6}, pages = {609 -- 612}, publisher = {Mathematical Association of America}, title = {{Surprises in numerical expressions of physical constants}}, doi = {10.4169/amer.math.monthly.123.6.609}, volume = {123}, year = {2016}, } @inproceedings{1205, abstract = {In this paper, we present a formal model-driven engineering approach to establishing a safety-assured implementation of Multifunction vehicle bus controller (MVBC) based on the generic reference models and requirements described in the International Electrotechnical Commission (IEC) standard IEC-61375. First, the generic models described in IEC-61375 are translated into a network of timed automata, and some safety requirements tested in IEC-61375 are formalized as timed computation tree logic (TCTL) formulas. With the help of Uppaal, we check and debug whether the timed automata satisfy the formulas or not. Within this step, several logic inconsistencies in the original standard are detected and corrected. Then, we apply the tool Times to generate C code from the verified model, which was later synthesized into a real MVBC chip. Finally, the runtime verification tool RMOR is applied to verify some safety requirements at the implementation level. We set up a real platform with worldwide mostly used MVBC D113, and verify the correctness and the scalability of the synthesized MVBC chip more comprehensively. The errors in the standard has been confirmed and the resulted MVBC has been deployed in real train communication network.}, author = {Jiang, Yu and Liu, Han and Song, Houbing and Kong, Hui and Gu, Ming and Sun, Jiaguang and Sha, Lui}, location = {Limassol, Cyprus}, pages = {757 -- 763}, publisher = {Springer}, title = {{Safety assured formal model driven design of the multifunction vehicle bus controller}}, doi = {10.1007/978-3-319-48989-6_47}, volume = {9995}, year = {2016}, } @article{1206, abstract = {We study a polar molecule immersed in a superfluid environment, such as a helium nanodroplet or a Bose–Einstein condensate, in the presence of a strong electrostatic field. We show that coupling of the molecular pendular motion, induced by the field, to the fluctuating bath leads to formation of pendulons—spherical harmonic librators dressed by a field of many-particle excitations. We study the behavior of the pendulon in a broad range of molecule–bath and molecule–field interaction strengths, and reveal that its spectrum features a series of instabilities which are absent in the field-free case of the angulon quasiparticle. Furthermore, we show that an external field allows to fine-tune the positions of these instabilities in the molecular rotational spectrum. This opens the door to detailed experimental studies of redistribution of orbital angular momentum in many-particle systems. © 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim}, author = {Redchenko, Elena and Lemeshko, Mikhail}, journal = {ChemPhysChem}, number = {22}, pages = {3649 -- 3654}, publisher = {Wiley-Blackwell}, title = {{Libration of strongly oriented polar molecules inside a superfluid}}, doi = {10.1002/cphc.201601042}, volume = {17}, year = {2016}, } @article{1209, abstract = {NADH-ubiquinone oxidoreductase (complex I) is the largest (∼1 MDa) and the least characterized complex of the mitochondrial electron transport chain. Because of the ease of sample availability, previous work has focused almost exclusively on bovine complex I. However, only medium resolution structural analyses of this complex have been reported. Working with other mammalian complex I homologues is a potential approach for overcoming these limitations. Due to the inherent difficulty of expressing large membrane protein complexes, screening of complex I homologues is limited to large mammals reared for human consumption. The high sequence identity among these available sources may preclude the benefits of screening. Here, we report the characterization of complex I purified from Ovis aries (ovine) heart mitochondria. All 44 unique subunits of the intact complex were identified by mass spectrometry. We identified differences in the subunit composition of subcomplexes of ovine complex I as compared with bovine, suggesting differential stability of inter-subunit interactions within the complex. Furthermore, the 42-kDa subunit, which is easily lost from the bovine enzyme, remains tightly bound to ovine complex I. Additionally, we developed a novel purification protocol for highly active and stable mitochondrial complex I using the branched-chain detergent lauryl maltose neopentyl glycol. Our data demonstrate that, although closely related, significant differences exist between the biochemical properties of complex I prepared from ovine and bovine mitochondria and that ovine complex I represents a suitable alternative target for further structural studies. }, author = {Letts, James A and Degliesposti, Gianluca and Fiedorczuk, Karol and Skehel, Mark and Sazanov, Leonid A}, journal = {Journal of Biological Chemistry}, number = {47}, pages = {24657 -- 24675}, publisher = {American Society for Biochemistry and Molecular Biology}, title = {{Purification of ovine respiratory complex i results in a highly active and stable preparation}}, doi = {10.1074/jbc.M116.735142}, volume = {291}, year = {2016}, } @inbook{1210, abstract = {Mechanisms for cell protection are essential for survival of multicellular organisms. In plants, the apical hook, which is transiently formed in darkness when the germinating seedling penetrates towards the soil surface, plays such protective role and shields the vitally important shoot apical meristem and cotyledons from damage. The apical hook is formed by bending of the upper hypocotyl soon after germination, and it is maintained in a closed stage while the hypocotyl continues to penetrate through the soil and rapidly opens when exposed to light in proximity of the soil surface. To uncover the complex molecular network orchestrating this spatiotemporally tightly coordinated process, monitoring of the apical hook development in real time is indispensable. Here we describe an imaging platform that enables high-resolution kinetic analysis of this dynamic developmental process. © Springer Science+Business Media New York 2017.}, author = {Zhu, Qiang and Žádníková, Petra and Smet, Dajo and Van Der Straeten, Dominique and Benková, Eva}, booktitle = {Plant Hormones}, pages = {1 -- 8}, publisher = {Humana Press}, title = {{Real time analysis of the apical hook development}}, doi = {10.1007/978-1-4939-6469-7_1}, volume = {1497}, year = {2016}, } @article{1212, abstract = {Plants adjust their growth according to gravity. Gravitropism involves gravity perception, signal transduction, and asymmetric growth response, with organ bending as a consequence [1]. Asymmetric growth results from the asymmetric distribution of the plant-specific signaling molecule auxin [2] that is generated by lateral transport, mediated in the hypocotyl predominantly by the auxin transporter PIN-FORMED3 (PIN3) [3–5]. Gravity stimulation polarizes PIN3 to the bottom sides of endodermal cells, correlating with increased auxin accumulation in adjacent tissues at the lower side of the stimulated organ, where auxin induces cell elongation and, hence, organ bending. A curvature response allows the hypocotyl to resume straight growth at a defined angle [6], implying that at some point auxin symmetry is restored to prevent overbending. Here, we present initial insights into cellular and molecular mechanisms that lead to the termination of the tropic response. We identified an auxin feedback on PIN3 polarization as underlying mechanism that restores symmetry of the PIN3-dependent auxin flow. Thus, two mechanistically distinct PIN3 polarization events redirect auxin fluxes at different time points of the gravity response: first, gravity-mediated redirection of PIN3-mediated auxin flow toward the lower hypocotyl side, where auxin gradually accumulates and promotes growth, and later PIN3 polarization to the opposite cell side, depleting this auxin maximum to end the bending. Accordingly, genetic or pharmacological interference with the late PIN3 polarization prevents termination of the response and leads to hypocotyl overbending. This observation reveals a role of auxin feedback on PIN polarity in the termination of the tropic response. © 2016 Elsevier Ltd}, author = {Rakusová, Hana and Abbas, Mohamad and Han, Huibin and Song, Siyuan and Robert, Hélène and Friml, Jirí}, journal = {Current Biology}, number = {22}, pages = {3026 -- 3032}, publisher = {Cell Press}, title = {{Termination of shoot gravitropic responses by auxin feedback on PIN3 polarity}}, doi = {10.1016/j.cub.2016.08.067}, volume = {26}, year = {2016}, } @inproceedings{1214, abstract = {With the accelerated development of robot technologies, optimal control becomes one of the central themes of research. In traditional approaches, the controller, by its internal functionality, finds appropriate actions on the basis of the history of sensor values, guided by the goals, intentions, objectives, learning schemes, and so forth. While very successful with classical robots, these methods run into severe difficulties when applied to soft robots, a new field of robotics with large interest for human-robot interaction. We claim that a novel controller paradigm opens new perspective for this field. This paper applies a recently developed neuro controller with differential extrinsic synaptic plasticity to a muscle-tendon driven arm-shoulder system from the Myorobotics toolkit. In the experiments, we observe a vast variety of self-organized behavior patterns: when left alone, the arm realizes pseudo-random sequences of different poses. By applying physical forces, the system can be entrained into definite motion patterns like wiping a table. Most interestingly, after attaching an object, the controller gets in a functional resonance with the object's internal dynamics, starting to shake spontaneously bottles half-filled with water or sensitively driving an attached pendulum into a circular mode. When attached to the crank of a wheel the neural system independently develops to rotate it. In this way, the robot discovers affordances of objects its body is interacting with.}, author = {Martius, Georg S and Hostettler, Raphael and Knoll, Alois and Der, Ralf}, location = {Daejeon, Korea}, publisher = {IEEE}, title = {{Compliant control for soft robots: Emergent behavior of a tendon driven anthropomorphic arm}}, doi = {10.1109/IROS.2016.7759138}, volume = {2016-November}, year = {2016}, } @article{261, abstract = {Let G = SL(2, R) ⋉R2 and Γ = SL(2, Z) ⋉Z2. Building on recent work of Strömbergsson, we prove a rate of equidistribution for the orbits of a certain one-dimensional unipotent flow of Γ\G, which projects to a closed horocycle in the unit tangent bundle to the modular surface. We use this to answer a question of Elkies and McMullen by making effective the convergence of the gap distribution of √n mod 1.}, author = {Timothy Browning and Vinogradov, Ilya}, journal = {Journal of the London Mathematical Society}, number = {1}, pages = {61 -- 84}, publisher = {John Wiley and Sons Ltd}, title = {{Effective ratner theorem for SL (2, R) ⋉R2 and gaps in √n modulo 1}}, doi = {10.1112/jlms/jdw025}, volume = {94}, year = {2016}, } @article{262, abstract = {For any number field we calculate the exact proportion of rational numbers which are everywhere locally a norm but not globally a norm from the number field.}, author = {Timothy Browning and Newton, Rachel}, journal = {Mathematika}, number = {2}, pages = {337 -- 347}, publisher = {Cambridge University Press}, title = {{The proportion of failures of the Hasse norm principle}}, doi = {10.1112/S0025579315000261}, volume = {62}, year = {2016}, } @article{263, abstract = {We count rational points of bounded height on the Cayley ruled cubic surface and interpret the result in the context of general conjectures due to Batyrev and Tschinkel.}, author = {de la Bretèche, Régis and Timothy Browning and Salberger, Per}, journal = {European Journal of Mathematics}, number = {1}, pages = {55 -- 72}, publisher = {Springer Nature}, title = {{Counting rational points on the Cayley ruled cubic}}, doi = {10.1007/s40879-015-0049-1}, volume = {2}, year = {2016}, } @article{264, abstract = {Given a family of varieties over a number field, we determine conditions under which there is a Brauer-Manin obstruction to weak approximation for 100% of the fibres which are everywhere locally soluble.}, author = {Bright, Maritn J and Timothy Browning and Loughran, Daniel}, journal = {Compositio Mathematica}, number = {7}, pages = {1435 -- 1475}, publisher = {Cambridge University Press}, title = {{Failures of weak approximation in families}}, doi = {10.1112/S0010437X16007405}, volume = {152}, year = {2016}, } @article{363, abstract = {Lead halide perovskite materials have attracted significant attention in the context of photovoltaics and other optoelectronic applications, and recently, research efforts have been directed to nanostructured lead halide perovskites. Collodial nanocrystals (NCs) of cesium lead halides (CsPbX3, X = Cl, Br, I) exhibit bright photoluminescence, with emission tunable over the entire visible spectral region. However, previous studies on CsPbX3 NCs did not address key aspects of their chemistry and photophysics such as surface chemistry and quantitative light absorption. Here, we elaborate on the synthesis of CsPbBr3 NCs and their surface chemistry. In addition, the intrinsic absorption coefficient was determined experimentally by combining elemental analysis with accurate optical absorption measurements. 1H solution nuclear magnetic resonance spectroscopy was used to characterize sample purity, elucidate the surface chemistry, and evaluate the influence of purification methods on the surface composition. We find that ligand binding to the NC surface is highly dynamic, and therefore, ligands are easily lost during the isolation and purification procedures. However, when a small amount of both oleic acid and oleylamine is added, the NCs can be purified, maintaining optical, colloidal, and material integrity. In addition, we find that a high amine content in the ligand shell increases the quantum yield due to the improved binding of the carboxylic acid.}, author = {De Roo, Jonathan and Ibáñez, Maria and Geiregat, Pieter and Nedelcu, Georgian and Walravens, Willem and Maes, Jorick and Martins, Jose and Van Driessche, Isabel and Kovalenko, Maksym and Hens, Zeger}, journal = {ACS Nano}, number = {2}, pages = {2071 -- 2081}, publisher = {American Chemical Society}, title = {{Highly dynamic ligand binding and light absorption coefficient of cesium lead bromide perovskite nanocrystals}}, doi = {10.1021/acsnano.5b06295}, volume = {10}, year = {2016}, } @article{364, abstract = {The development of highly active, low cost and stable electrocatalysts for direct alcohol fuel cells remains a critical challenge. While Pd2Sn has been reported as an excellent catalyst for the ethanol oxidation reaction (EOR), here we present DFT analysis results showing the (100) and (001) facets of orthorhombic Pd2Sn to be more favourable for the EOR than (010). Accordingly, using tri-n-octylphosphine, oleylamine (OLA) and methylamine hydrochloride as size and shape directing agents, we produced colloidal Pd2Sn nanorods (NRs) grown in the [010] direction. Such Pd2Sn NRs, supported on graphitic carbon, showed excellent performance and stability as an anode electrocatalyst for the EOR in alkaline media, exhibiting 3 times and 10 times higher EOR current densities than that of Pd2Sn and Pd nanospheres, respectively. We associate this improved performance with the favourable faceting of the NRs.}, author = {Luo, Zhishan and Lu, Jianmin and Flox, Cristina and Nafria, Raquel and Genç, Aziz and Arbiol, Jordi and Llorca, Jordi and Ibanez Sabate, Maria and Morante, Joan and Cabot, Andreu}, journal = {Journal of Materials Chemistry A}, number = {42}, pages = {16706 -- 16713}, publisher = {Royal Society of Chemistry}, title = {{Pd2Sn [010] nanorods as a highly active and stable ethanol oxidation catalyst}}, doi = {10.1039/c6ta06430b}, volume = {4}, year = {2016}, } @article{366, abstract = {Cesium lead halide (CsPbX3, X = Cl, Br, I) nanocrystals (NCs) offer exceptional optical properties for several potential applications but their implementation is hindered by a low chemical and structural stability and limited processability. In the present work, we developed a new method to efficiently coat CsPbX3 NCs, which resulted in their increased chemical and optical stability as well as processability. The method is based on the incorporation of poly(maleic anhydride-alt-1-octadecene) (PMA) into the synthesis of the perovskite NCs. The presence of PMA in the ligand shell stabilizes the NCs by tightening the ligand binding, limiting in this way the NC surface interaction with the surrounding media. We further show that these NCs can be embedded in self-standing silicone/glass plates as down-conversion filters for the fabrication of monochromatic green and white light emitting diodes (LEDs) with narrow bandwidths and appealing color characteristics.}, author = {Meyn, Michaela and Perálvarez, Mariano and Heuer Jungemann, Amelie and Hertog, Wim and Ibanez Sabate, Maria and Nafria, Raquel and Genç, Aziz and Arbiol, Jordi and Kovalenko, Maksym and Carreras, Josep and Cabot, Andreu and Kanaras, Antonios}, journal = {ACS Applied Materials and Interfaces}, number = {30}, pages = {19579 -- 19586}, publisher = {American Chemical Society}, title = {{Polymer enhanced stability of inorganic perovskite nanocrystals and their application in color conversion LEDs}}, doi = {10.1021/acsami.6b02529}, volume = {8}, year = {2016}, }