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These predictions are shown to explain quantitatively the split modes observed in BPCB.The existence of ideal quantum measurements is one of the fundamental predictions of quantum mechanics. In theory, an ideal measurement projects a quantum state onto the eigenbasis of the measurement observable, while preserving coherences between eigenstates that have the same eigenvalue. The question arises whether there are processes in nature that correspond to such ideal quantum measurements and how such processes are dynamically implemented in nature. Here we address this question and present experimental results monitoring the dynamics of a naturally occurring measurement process the coupling of a trapped ion qutrit to the photon environment. By taking tomographic snapshots during the detection process, we show that the process develops in agreement with the model of an ideal quantum measurement with an average fidelity of 94%.Terrestrial experiments on active particles, such as Volvox, involve gravitational forces, torques and accompanying monopolar fluid flows. Taking these into account, we analyze the dynamics of a pair of self-propelling, self-spinning active particles between widely separated parallel planes. Neglecting flow reflected by the planes, the dynamics of orientation and horizontal separation is symplectic, with a Hamiltonian exactly determining limit cycle oscillations. Near the bottom plane, gravitational torque damps and reflected flow excites this oscillator, sustaining a second limit cycle that can be perturbatively related to the first. Our work provides a theory for dancing Volvox and highlights the importance of monopolar flow in active matter.We consider a model for driven particulate matter in which absorbing states can be reached both by particle isolation and by particle caging. The model predicts a nonequilibrium phase diagram in which analogs of hydrodynamic and elastic reversibility emerge at low and high volume fractions respectively, partially separated by a diffusive, nonabsorbing region. We thus find a single phase boundary that spans the onset of chaos in sheared suspensions to the onset of yielding in jammed packings. This boundary has the properties of a nonequilibrium second order phase transition, leading us to write a Manna-like mean field description that captures the model predictions. Dependent on contact details, jamming marks either a direct transition between the two absorbing states, or occurs within the diffusive region.To gain insight into the kinetics of colloidal gel evolution at low particle volume fractions ?, we utilize differential dynamic microscopy to investigate particle aggregation, geometric percolation, and the subsequent transition to nonergodic dynamics. We report the emergence of unexpectedly rich multiscale dynamics upon the onset of nonergodicity, which separates the wave vectors q into three different regimes. In the high-q domain, the gel exhibits ?-independent internal vibrations of fractal clusters. The intermediate-q domain is dominated by density fluctuations at the length scale of the clusters, as evidenced by the q independence of the relaxation time τ. In the low-q domain, the scaling of τ as q^-3 suggests that the network appears homogeneous. The transitions between these three regimes introduce two characteristic length scales, distinct from the cluster size.In this Letter we study an infinite extension of the Galilei symmetry group in any dimension that can be thought of as a nonrelativistic or post-Galilean expansion of the Poincaré symmetry. We find an infinite-dimensional vector space on which this generalized Galilei group acts and usual Minkowski space can be modeled by our construction. We also construct particle and string actions that are invariant under these transformations.The fundamental principles of electrodynamics allow an electron carrying both electric monopole (charge) and magnetic dipole (spin) but prohibit its magnetic counterpart. Recently, it was predicted that the magnetic "monopoles" carrying emergent magnetic charges in spin ice systems can induce electric dipoles. The inspiring prediction offers a novel way to study magnetic monopole excitations and magnetoelectric coupling. However, no clear example has been identified up to now. Here, we report the experimental evidence for electric dipoles induced by magnetic monopoles in spin frustrated Tb_2Ti_2O_7. The magnetic field applied to pyrochlore Tb_2Ti_2O_7 along the [111] direction, brings out a "3-in-1-out" magnetic monopole configuration, and then induces a subtle structural phase transition at H_c?2.3??T. The transition is made evident by the nonlinear phonon splitting under magnetic fields and the anomalous crystal-field excitations of Tb^3+ https://www.selleckchem.com/products/nec-1s-7-cl-o-nec1.html ions. The observations consistently point to the dispWe propose a scheme for global optimization with first-principles energy expressions of atomistic structure. While unfolding its search, the method actively learns a surrogate model of the potential energy landscape on which it performs a number of local relaxations (exploitation) and further structural searches (exploration). Assuming Gaussian processes, deploying two separate kernel widths to better capture rough features of the energy landscape while retaining a good resolution of local minima, an acquisition function is used to decide on which of the resulting structures is the more promising and should be treated at the first-principles level. The method is demonstrated to outperform by 2 orders of magnitude a well established first-principles based evolutionary algorithm in finding surface reconstructions. Finally, global optimization with first-principles energy expressions is utilized to identify initial stages of the edge oxidation and oxygen intercalation of graphene sheets on the Ir(111) surface.Quantum spin liquids (QSLs) form an extremely unusual magnetic state in which the spins are highly correlated and fluctuate coherently down to the lowest temperatures, but without symmetry breaking and without the formation of any static long-range-ordered magnetism. Such intriguing phenomena are not only of great fundamental relevance in themselves, but also hold promise for quantum computing and quantum information. Among different types of QSLs, the exactly solvable Kitaev model is attracting much attention, with most proposed candidate materials, e.g., RuCl_3 and Na_2IrO_3, having an effective S=1/2 spin value. Here, via extensive first-principles-based simulations, we report the investigation of the Kitaev physics and possible Kitaev QSL state in epitaxially strained Cr-based monolayers, such as CrSiTe_3, that rather possess a S=3/2 spin value. Our study thus extends the playground of Kitaev physics and QSLs to 3d transition metal compounds.The only known way to study quantum field theories in nonperturbative regimes is using numerical calculations regulated on discrete space-time lattices. Such computations, however, are often faced with exponential signal-to-noise challenges that render key physics studies untenable even with next generation classical computing. Here, a method is presented by which the output of small-scale quantum computations on noisy intermediate-scale quantum era hardware can be used to accelerate larger-scale classical field theory calculations through the construction of optimized interpolating operators. The method is implemented and studied in the context of the 1+1-dimensional Schwinger model, a simple field theory which shares key features with the standard model of nuclear and particle physics.We show theoretically that spin and orbital degrees of freedom in the pyrochlore oxide Y_2Mo_2O_7, which is free of quenched disorder, can exhibit a simultaneous glass transition, working as dynamical disorder for each other. The interplay of spins and orbitals is mediated by the Jahn-Teller lattice distortion that selects the choice of orbitals, which then generates variant spin exchange interactions ranging from ferromagnetic to antiferromagnetic ones. Our Monte Carlo simulations detect the power-law divergence of the relaxation times and the negative divergence of both the magnetic and dielectric nonlinear susceptibilities, resolving the long-standing puzzle on the origin of the disorder-free spin glass.Acceleration of particles from the interaction of ultraintense laser pulses up to 5×10^21??W?cm^-2 with thin foils is investigated experimentally. The electron beam parameters varied with decreasing spot size, not just laser intensity, resulting in reduced temperatures and divergence. In particular, the temperature saturated due to insufficient acceleration length in the tightly focused spot. These dependencies affected the sheath-accelerated protons, which showed poorer spot-size scaling than widely used scaling laws. It is therefore shown that maximizing laser intensity by using very small foci has reducing returns for some applications.Excitons, as bound electron-hole paired quasiparticle, play an essential role in the energy transport in the optical-electric properties of semiconductors. Their momentum-energy dispersion relation is a fundamental physical property of great significance to understand exciton dynamics. However, this dispersion is seldom explored especially in two-dimensional transition metal dichalcogenides with rich valleytronic properties. In this work, momentum resolved electron energy-loss spectroscopy was used to measure the dispersions of excitons in freestanding monolayer WSe_2. Besides the parabolically dispersed valley excitons, a subgap dispersive exciton was observed at nonzero momenta for the first time, which can be introduced by the prolific Se vacancies. Our work provides a paradigm to directly probe exciton dispersions in 2D semiconductors and could be generalized to many low-dimensional systems.Antiferromagnet Mn_3P with Neel temperature T_N=30??K is composed of Mn tetrahedrons and zigzag chains formed by three inequivalent Mn sites. Due to the nearly frustrated lattice with many short Mn-Mn bonds, competition of the exchange interactions is expected. We here investigate the magnetic structure and physical properties including pressure effect in single crystals of this material, and reveal a complex yet well-ordered helimagnetic structure. The itinerant character of this materials is strong, and the ordered state with small magnetic moments is easily suppressed under pressure, exhibiting a quantum critical point at ?1.6??GPa. The remarkable mass renormalization, even in the ordered state, and an incoherent-coherent crossover in the low-temperature region, characterize an unusual electronic state in Mn_3P, which is most likely effected by the underlying frustration effect.A novel and efficient access to polyfunctionnalized chiral 1-tetralols, bearing two contiguous quaternary carbon stereocenters, has been developed from various and easily accessible alkynyl-1,3-diketones, through a cascade process including a regioselective alkyne insertion, a 1,4-Rh shift, and a nucleophilic addition step via the desymmetrization of the 1,3-diketone moiety thanks to an appropriate rhodium-chiral diene complex in the presence of arylboronic acids.(±)-Dispirocochlearoids A-C (1-3), meroterpenoids with a 6/6/5/6/6/6 ring system, were isolated from Ganoderma cochlear. 1-3 are selective COX-2 inhibitors with an IC50 value of (-)-2 at 386 nM. Site-directed mutagenesis identified His351 as a COX-2 active site. In vivo anti-inflammatory activities of (-)-2 were performed against acute lung injury in mice.The co-occurrence of contaminants in drinking water may pose enhanced risks to health beyond the effects of single contaminants. Here, we investigated the co-occurrence of four health-relevant redox-sensitive elements (U, As, V, and Cr) in 1494 groundwater wells across North Carolina. The highest concentrations of these elements were measured mostly in groundwater from fractured igneous and metamorphic formations throughout the Piedmont region. Arsenic occurred most frequently in suboxic to mixed redox character groundwater, whereas U, V, and Cr occurred mostly in oxic groundwater. Occurrences of As, and to a lesser extent U, increased with pH, likely reflecting desorption, while higher Cr and V levels were measured in near-neutral pH and oxic groundwater, reflecting greater sensitivity to redox conditions. Due to similar geochemistry, V and Cr co-occurred most frequently. Concentrations of V and Cr(VI) co-exceeded health recommendations from the NC Department of Health and Human Services in up to 84% of wellThe recurrence of malignant tumors is mostly caused by incompleted surgical resection. Especially, it is difficult for surgeons to detect and accurately remove metastatic tumors by predominantly using visual examination and palpation owing to the lack of effective means to specifically distinguish the boundary range between normal and tumor tissues. Thus, the development of activated fluorescent probe with superior tumor-to-normal (T/N) tissue ratios is particularly urgent in clinics. In view of CD13/aminopeptidase N (APN) regarded as a cancer-specific biomarker, mediating with progression, invasion, and migration of malignant tumor, herein, we reported an APN-responsive fluorescent probe YH-APN and demonstrated its application to distinguish cancer cells. Through in situ spraying manner, fluorescent superior tumor-to-normal (T/N) tissue ratios (subcutaneous transplantation tumor, 13.86; hepatic metastasis, 4.42 and 6.25; splenic metastasis, 4.99) were achieved. More importantly, we have demonstrated the abilDiarrheal illnesses from enteric pathogens are a leading cause of death in children under five in low- and middle-income countries (LMICs). Sanitation is one way to reduce the spread of enteric pathogens in the environment; however, few studies have investigated the effectiveness of sanitation in rural LMICs in reducing pathogens in the environment. In this study, we measured the impact of a sanitation intervention (dual-pit latrines, sani-scoops, child potties delivered as part of a randomized control trial, WASH Benefits) in rural Bangladeshi household compounds by assessing prevalence ratios, differences, and changes in the concentration of pathogen genes and host-specific fecal markers. We found no difference in the prevalence of pathogenic Escherichia coli, norovirus, or Giardia genes in the domestic environment in the sanitation and control arms. The prevalence of the human fecal marker was lower on child hands and the concentration of animal fecal marker was lower on mother hands in the sanitation arm Cellulose nanofibrils (CNFs) prepared from wood biomass are promising candidates to replace oil-based materials in, for example, packaging applications. However, CNFs' affinity for water combined with their small size leads to very slow and energy-demanding processes for handling and removal of water. To a large extent, this is the major roadblock that prevents a feasible production of dry CNF-based materials on an industrial scale. In this work, self-fibrillating fibers (SFFs) from wood, where the fibrils can be liberated by external stimuli, were prepared via sequential TEMPO and periodate oxidation reactions. Papers made from these modified fibers using conventional laboratory papermaking methods were then in situ nanofibrillated via a modest pH increase. With a dewatering time of less than 10 s for a 3 g/L dispersion, SFFs represent a major improvement over conventional CNF nanopapers that take approximately 6 h to dewater. Moreover, 100 g/m2 nanopapers obtained through in situ fibrillation exhibited compIn this work, a cleancap-regulated aggregation-induced emission (AIE) strategy based on copper nanoclusters (CuNCs) was developed with stepwise recognition for highly specific analysis of the enzyme. The dissolved CuNCs with AIE characteristics in alkaline solution were prepared by using p-mercaptophenylboronic acid as the reducing agent and the stabilizing ligand. The prepared CuNCs can specifically conjugate with glucose (Glu) to connect with each other via the rapid boronate esters formation between boronic acids of CuNCs and a pair of cis-diols on Glu. The cleancap-regulated AIE strategy was further identified by modification of CuNCs with d-glucose 6-phosphate (P-Glu) as the capper and substrate. Introduction of alkaline phosphatase to the P-Glu/CuNCs complex can induce the cleavage of phosphate group to activate the 5,6-diol of Glu on the CuNCs. The decapped complexes could be aggregated through further conjugation between 5,6-diol and boronic acid of two CuNCs, resulting in strong red AIE luminescence.Supramolecular systems are intrinsically dynamic and sensitive to changes in molecular structure and external conditions. Because of these unique properties, strategies to control polymer length, composition, comonomer sequence, and morphology have to be developed for sufficient control over supramolecular copolymerizations. We designed photoresponsive, mono acyl hydrazone functionalized benzene-1,3,5-tricarboxamide (m-BTA) monomers that play a dual role in the coassembly with achiral alkyl BTAs (a-BTA). In the E isomer form, the chiral m-BTA monomers intercalate into stacks of a-BTA and dictate the chirality of the helices. Photoisomerization to the Z isomer transforms the intercalator into a chain capper, allowing dynamic shortening of chain length in the supramolecular aggregates. We combine optical spectroscopy and light-scattering experiments with theoretical modeling to show the reversible decrease in length when switching from the E to Z isomer of m-BTA in the copolymer with inert a-BTA. With a mass-baWhile 17O NMR is increasingly being used for elucidating the structure and reactivity of complex molecular and materials systems, much effort is still required for it to become a routine analytical technique. One of the main difficulties for its development comes from the very low natural abundance of 17O (0.04%), which implies that isotopic labeling is generally needed prior to NMR analyses. However, 17O-enrichment protocols are often unattractive in terms of cost, safety, and/or practicality, even for compounds as simple as metal oxides. Here, we demonstrate how mechanochemistry can be used in a highly efficient way for the direct 17O isotopic labeling of a variety of s-, p-, and d-block oxides, which are of major interest for the preparation of functional ceramics and glasses Li2O, CaO, Al2O3, SiO2, TiO2, and ZrO2. For each oxide, the enrichment step was performed under ambient conditions in less than 1 h and at low cost, which makes these synthetic approaches highly appealing in comparison to the existingFluoxetine has been recognized as one of the most toxic pharmaceuticals in the aquatic environment. Since there is growing evidence that the toxic potential of fluoxetine in surface waters is markedly influenced by its own metabolism in aquatic species, this study investigated the biotransformation of fluoxetine in the zebrafish embryo - an aquatic model organism of intermediate complexity. Zebrafish embryos were exposed to 0.1, 1.0, 10, 50, and 5000 μg/L of fluoxetine from 48 to 120 h post-fertilization (hpf), and the accumulation of fluoxetine and its metabolites was analyzed over time. Additionally, depuration of fluoxetine and its metabolites from 96 to 120 hpf was investigated, and autoinhibitory effects of fluoxetine on phase I biotransformation were analyzed. Exposure to 5000 μg/L fluoxetine resulted in elevated 7-ethoxyresorufin-O-deethylase (EROD) activity of cytochrome P450 enzymes and continuous accumulation of fluoxetine and 11 fluoxetine metabolites. Embryos exposed to 10 and 50 μg/L fluoxetine wA new type of ammonium vanadium bronze, (NH4)2V7O16, was synthesized by the hydrothermal method. The triclinic crystal structure (P1?) is successfully identified by the single-crystal X-ray diffraction method. The layered structure is similar to that of other vanadium bronzes but with an unprecedented stoichiometry and crystal structure. The structure is composed of a stack of V7O16 layers along the c axis, and two NH4+ ions occupy the interlayer space per formula unit. Each ammonium ion is hydrogen-bonded to four lattice oxygen atoms, resulting in a stable structure with a large interlayer space, thus enabling the intercalation of various guest ions. Lithium ions are electrochemically intercalated into (NH4)2V7O16, with an initial discharge capacity of 232 mAh g-1 and an average discharge voltage of 2 V (vs Li/Li+). Upon the first discharge, lithium ions are inserted, whereas ammonium ions are extracted. Upon charging, a reverse reaction takes place. However, only a fraction of the extracted ammonium ions arFatty acyl coenzyme A esters (FA-CoAs?) are important crossroad intermediates in lipid catabolism and anabolism, and the structures are complicated. Several mass spectrometric approaches have been previously described to elucidate their structures. However, a direct mass spectrometric approach toward a complete identification of the molecule, including the location of unsaturated bond(s) in the fatty acid chain has not been reported. In this study we applied a simple MALDI/TOF mass spectrometric method to a near complete characterization of long-chain FA-CoAs?, including the location(s) of the double-bond in the fatty acyl chain, and the common structural features that recognize FA-CoAs?. Negative ion mass spectra of saturated, monounsaturated, and polyunsaturated FA-CoAs? were acquired with MALDI/TOF mass spectrometer using 2,5-dihydroxybenzoic acid as the matrix and ionized with a laser fluence two folds of the threshold to induce the in-source fragmentation (ISF) of the analytes. The resulting ISF spectra contHousehold drinking water storage is commonly practiced in rural India. Fecal contamination may be introduced at the water source, during collection, storage, or access. Within a trial of a community-level water supply intervention, we conducted five quarterly household-level surveys to collect information about water, sanitation, and hygiene practices in rural India. In a random subsample of households, we tested stored drinking water samples for Escherichia coli, concurrently observing storage and access practices. We conducted 9961 surveys and collected 3296 stored water samples. Stored water samples were frequently contaminated with E. coli (69%), and E. coli levels were the highest during the wet season. Most households contributing two or more drinking water samples had detectable E. coli in some (47%) or all (44%) samples. Predictors of stored water contamination with E. coli included consumption of river water and open defecation; consumption of reverse osmosis-treated water and safe water access practTo reach their site of action, it is essential for antibiotic molecules to cross the bacterial outer membrane. The progress of enhanced sampling techniques in molecular dynamics simulations enables us to understand these translocations at an atomic level. To this end, calculations of free energy surfaces for these permeation processes are of key importance. Herein, we investigate the translocation of a variety of anionic solutes through the outer membrane pore OprO of the Gram-negative bacterium Pseudomonas aeruginosa using the metadynamics and umbrella sampling techniques at the all-atom level. Free energy calculations have been performed employing these two distinct methods in order to illustrate the difference in computed free energies, if any. The investigated solutes range from a single atomic chloride ion over a multiatomic monophosphate ion to a more bulky fosmidomycin antibiotic. The role of complexity of the permeating solutes in estimating accurate free energy profiles is demonstrated by performing (Amino)cyclotriphosphazenes have been used as new scaffolds for the synthesis of silver(I) metallomesogens. Two cyclotriphosphazenes, [N3P3(NHCy)6] (phos-1) and nongem-trans-[N3P3(NHCy)3(NMe2)3] (phos-2), were reacted with the silver complex having a pro-mesogenic ligand, [Ag(OTf)L] (L = CNC6H4OC(O)C6H2(3,4,5-(OC10H21)3)-4; OTf = OSO2CF3), in different molar ratios, 11, 12, or 13, to give two series of cationic metallophosphazenes, [N3P3(NHCy)6AgLn?](TfO)n (phos-1.n) and nongem-trans-[N3P3(NHCy)3(NMe2)3AgLn?](TfO)n (phos-2.n) with n = 1, 2, or 3. The chemical structure of these compounds, deduced from spectroscopic techniques, was in accordance with coordination of the silver fragments "AgL" to nitrogen atoms of the phosphazene ring, whereby their number n depends on the molar ratio used. Despite the presence of the bulky substituents on the core N atoms, cyclotriphosphazenes coordinated to three "AgL" units exhibited mesomorphism at room temperature. The mesophase was characterized as columnar hexagonal Uranium (U) in situ bioremediation has been investigated as a cost-effective strategy to tackle U contamination in the subsurface. While uraninite was believed to be the only product of bioreduction, numerous studies have revealed that noncrystalline U(IV) species (NCU(IV)) are dominant. This finding brings into question the effectiveness of bioremediation because NCU(IV) species are expected to be labile and susceptible to oxidation. Thus, understanding the stability of NCU(IV) in the environment is of crucial importance. Fe(II) minerals (such as FeS) are often associated with U(IV) in bioremediated or naturally reduced sediments. Their impact on the stability of NCU(IV) is not well understood. Here, we show that, at high dissolved oxygen concentrations, FeS accelerates NCU(IV) reoxidation. We hypothesize that either highly reactive ferric minerals or radical S species produced by the oxidation of FeS drive this rapid reoxidation of NCU(IV). Furthermore, we found evidence for the contribution of reactive oxygen species to NCU(IV) reoxidation.