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We present results on ultrafast gas electron diffraction (UGED) experiments with femtosecond resolution using the MeV electron gun at SLAC National Accelerator Laboratory. UGED is a promising method to investigate molecular dynamics in the gas phase because electron pulses can probe the structure with a high spatial resolution. Until recently, however, it was not possible for UGED to reach the relevant timescale for the motion of the nuclei during a molecular reaction. Using MeV electron pulses has allowed us to overcome the main challenges in reaching femtosecond resolution, namely delivering short electron pulses on a gas target, overcoming the effect of velocity mismatch between pump laser pulses and the probe electron pulses, and maintaining a low timing jitter. At electron kinetic energies above 3 MeV, the velocity mismatch between laser and electron pulses becomes negligible. The relativistic electrons are also less susceptible to temporal broadening due to the Coulomb force. One of the challenges of diffraction with relativistic electrons is that the small de Broglie wavelength results in very small diffraction angles. In this paper we describe the new setup and its characterization, including capturing static diffraction patterns of molecules in the gas phase, finding time-zero with sub-picosecond accuracy and first time-resolved diffraction experiments. The new device can achieve a temporal resolution of 100 fs root-mean-square, and sub-angstrom spatial resolution. The collimation of the beam is sufficient to measure the diffraction pattern, and the transverse coherence is on the order of 2 nm. Currently, the temporal resolution is limited both by the pulse duration of the electron pulse on target and by the timing jitter, while the spatial resolution is limited by the average electron beam current and the signal-to-noise ratio of the detection system. We also discuss plans for improving both the temporal resolution and the spatial resolution.
This study examined the spoken narrative skills of a group of bilingual Mandarin–English speaking 3–6-year-olds (N = 25) in Australia, using a remote online story-retell task. Bilingual preschoolers are an understudied population, especially those who are speaking typologically distinct languages such as Mandarin and English which have fewer structural overlaps compared to language pairs that are typologically closer, reducing cross-linguistic positive transfer. We examined these preschoolers’ spoken narrative skills as measured by macrostructures (the global organization of a story) and microstructures (linguistic structures, e.g., total number of utterances, nouns, verbs, phrases, and modifiers) across and within each language, and how various factors such as age and language experiences contribute to individual variability. The results indicate that our bilingual preschoolers acquired spoken narrative skills similarly across their two languages, i.e., showing similar patterns of productivity for macrostructure and microstructure elements in both of their two languages. While chronological age was positively correlated with macrostructures in both languages (showing developmental effects), there were no significant correlations between measures of language experiences and the measures of spoken narrative skills (no effects for language input/output). The findings suggest that although these preschoolers acquire two typologically diverse languages in different learning environments, Mandarin at home with highly educated parents, and English at preschool, they displayed similar levels of oral narrative skills as far as these macro−/micro-structure measures are concerned. This study provides further evidence for the feasibility of remote online assessment of preschoolers’ narrative skills.
Inositol phosphates (IPs) and their turnover products have been implicated to play important roles in stress signaling in eukaryotic cells. In higher plants genes encoding inositol polyphosphate kinases have been identified previously, but their physiological functions have not been fully resolved. Here we expressed Arabidopsis inositol polyphosphate 6-/3-kinase (AtIpk2 beta) in two heterologous systems, i.e. the yeast Saccharomyces cerevisiae and in tobacco (Nicotiana tabacum), and tested the effect on abiotic stress tolerance. Expression of AtIpk2 beta rescued the salt-, osmotic- and temperature-sensitive growth defects of a yeast mutant strain (arg82 Delta) that lacks inositol polyphosphate multikinase activity encoded by the ARG82/IPK2 gene. Transgenic tobacco plants constitutively expressing AtIpk2 beta under the control of the Cauliflower Mosaic Virus 35S promoter were generated and found to exhibit improved tolerance to diverse abiotic stresses when compared to wild type plants. Expression patterns of various stress responsive genes were enhanced, and the activities of anti-oxidative enzymes were elevated in transgenic plants, suggesting a possible involvement of AtIpk2 beta in plant stress responses.
Molecularly imprinted polymers (MIPs) have the potential to complement antibodies in bioanalysis, are more stable under harsh conditions, and are potentially cheaper to produce. However, the affinity and especially the selectivity of MIPs are in general lower than those of their biological pendants. Enzymes are useful tools for the preparation of MIPs for both low and high-molecular weight targets: As a green alternative to the well-established methods of chemical polymerization, enzyme-initiated polymerization has been introduced and the removal of protein templates by proteases has been successfully applied. Furthermore, MIPs have been coupled with enzymes in order to enhance the analytical performance of biomimetic sensors: Enzymes have been used in MIP-sensors as tracers for the generation and amplification of the measuring signal. In addition, enzymatic pretreatment of an analyte can extend the analyte spectrum and eliminate interferences.
Electrochemical methods offer the simple characterization of the synthesis of molecularly imprinted polymers (MIPs) and the readouts of target binding. The binding of electroinactive analytes can be detected indirectly by their modulating effect on the diffusional permeability of a redox marker through thin MIP films. However, this process generates an overall signal, which may include nonspecific interactions with the nonimprinted surface and adsorption at the electrode surface in addition to (specific) binding to the cavities. Redox-active low-molecular-weight targets and metalloproteins enable a more specific direct quantification of their binding to MIPs by measuring the faradaic current. The in situ characterization of enzymes, MIP-based mimics of redox enzymes or enzyme-labeled targets, is based on the indication of an electroactive product. This approach allows the determination of both the activity of the bio(mimetic) catalyst and of the substrate concentration.
We present an electrochemical MIP sensor for tamoxifen (TAM)-a nonsteroidal anti-estrogen-which is based on the electropolymerisation of an O-phenylenediamine. resorcinol mixture directly on the electrode surface in the presence of the template molecule. Up to now only. bulk. MIPs for TAM have been described in literature, which are applied for separation in chromatography columns. Electro-polymerisation of the monomers in the presence of TAM generated a film which completely suppressed the reduction of ferricyanide. Removal of the template gave a markedly increased ferricyanide signal, which was again suppressed after rebinding as expected for filling of the cavities by target binding. The decrease of the ferricyanide peak of the MIP electrode depended linearly on the TAM concentration between 1 and 100 nM. The TAM-imprinted electrode showed a 2.3 times higher recognition of the template molecule itself as compared to its metabolite 4-hydroxytamoxifen and no cross-reactivity with the anticancer drug doxorubucin was found. Measurements at + 1.1 V caused a fouling of the electrode surface, whilst pretreatment of TAM with peroxide in presence of HRP generated an oxidation product which was reducible at 0 mV, thus circumventing the polymer formation and electrochemical interferences.
Inverted perovskite solar cells still suffer from significant non-radiative recombination losses at the perovskite surface and across the perovskite/C₆₀ interface, limiting the future development of perovskite-based single- and multi-junction photovoltaics. Therefore, more effective inter- or transport layers are urgently required. To tackle these recombination losses, we introduce ortho-carborane as an interlayer material that has a spherical molecular structure and a three-dimensional aromaticity. Based on a variety of experimental techniques, we show that ortho-carborane decorated with phenylamino groups effectively passivates the perovskite surface and essentially eliminates the non-radiative recombination loss across the perovskite/C₆₀ interface with high thermal stability. We further demonstrate the potential of carborane as an electron transport material, facilitating electron extraction while blocking holes from the interface. The resulting inverted perovskite solar cells deliver a power conversion efficiency of over 23% with a low non-radiative voltage loss of 110 mV, and retain >97% of the initial efficiency after 400 h of maximum power point tracking. Overall, the designed carborane based interlayer simultaneously enables passivation, electron-transport and hole-blocking and paves the way toward more efficient and stable perovskite solar cells.
Almost half of the political life has been experienced under the
state of emergency and state of siege policies in the Turkish
Republic. In spite of such a striking number and continuity in the
deployment of legal emergency powers, there are just a few legal
and political studies examining the reasons for such permanency
in governing practices. To fill this gap, this paper aims to discuss
one of the most important sources of the ‘permanent’ political
crisis in the country: the historical evolution of legal emergency
power. In order to highlight how these policies have intensified
the highly fragile citizenship regime by weakening the separation
of power, repressing the use of political rights and increasing the
discretionary power of both the executive and judiciary authori-
ties, the paper sheds light on the emergence and production of
a specific form of legality based on the idea of emergency and the
principle of executive prerogative. In that context, it aims to
provide a genealogical explanation of the evolution of the excep-
tional form of the nation-state, which is based on the way political
society, representation, and legitimacy have been instituted and
accompanying failure of the ruling classes in building hegemony
in the country.
X-ray free-electron lasers (XFELs) and table-top sources of x-rays based upon high harmonic generation (HHG) have revolutionized the field of ultrafast x-ray atomic and molecular physics, largely due to an explosive growth in capabilities in the past decade. XFELs now provide unprecedented intensity (1020 W cm−2) of x-rays at wavelengths down to ~1 Ångstrom, and HHG provides unprecedented time resolution (~50 attoseconds) and a correspondingly large coherent bandwidth at longer wavelengths. For context, timescales can be referenced to the Bohr orbital period in hydrogen atom of 150 attoseconds and the hydrogen-molecule vibrational period of 8 femtoseconds; wavelength scales can be referenced to the chemically significant carbon K-edge at a photon energy of ~280 eV (44 Ångstroms) and the bond length in methane of ~1 Ångstrom. With these modern x-ray sources one now has the ability to focus on individual atoms, even when embedded in a complex molecule, and view electronic and nuclear motion on their intrinsic scales (attoseconds and Ångstroms). These sources have enabled coherent diffractive imaging, where one can image non-crystalline objects in three dimensions on ultrafast timescales, potentially with atomic resolution. The unprecedented intensity available with XFELs has opened new fields of multiphoton and nonlinear x-ray physics where behavior of matter under extreme conditions can be explored. The unprecedented time resolution and pulse synchronization provided by HHG sources has kindled fundamental investigations of time delays in photoionization, charge migration in molecules, and dynamics near conical intersections that are foundational to AMO physics and chemistry. This roadmap coincides with the year when three new XFEL facilities, operating at Ångstrom wavelengths, opened for users (European XFEL, Swiss-FEL and PAL-FEL in Korea) almost doubling the present worldwide number of XFELs, and documents the remarkable progress in HHG capabilities since its discovery roughly 30 years ago, showcasing experiments in AMO physics and other applications. Here we capture the perspectives of 17 leading groups and organize the contributions into four categories: ultrafast molecular dynamics, multidimensional x-ray spectroscopies; high-intensity x-ray phenomena; attosecond x-ray science.
Metal-containing ionic liquids (ILs) are of interest for a variety of technical applications, e.g., particle synthesis and materials with magnetic or thermochromic properties. In this paper we report the synthesis of, and two structures for, some new tetrabromidocuprates(II) with several “onium” cations in comparison to the results of electron paramagnetic resonance (EPR) spectroscopic analyses. The sterically demanding cations were used to separate the paramagnetic Cu(II) ions for EPR measurements. The EPR hyperfine structure in the spectra of these new compounds is not resolved, due to the line broadening resulting from magnetic exchange between the still-incomplete separated paramagnetic Cu(II) centres. For the majority of compounds, the principal g values (g|| and gK) of the tensors could be determined and information on the structural changes in the [CuBr4]2- anions can be obtained. The complexes have high potential, e.g., as ionic liquids, as precursors for the synthesis of copper bromide particles, as catalytically active or paramagnetic ionic liquids.
We consider synchronization properties of arrays of spin-torque nano-oscillators coupled via an RC load. We show that while the fully synchronized state of identical oscillators may be locally stable in some parameter range, this synchrony is not globally attracting. Instead, regimes of different levels of compositional complexity are observed. These include chimera states (a part of the array forms a cluster while other units are desynchronized), clustered chimeras (several clusters plus desynchronized oscillators), cluster state (all oscillators form several clusters), and partial synchronization (no clusters but a nonvanishing mean field). Dynamically, these states are also complex, demonstrating irregular and close to quasiperiodic modulation. Remarkably, when heterogeneity of spin-torque oscillators is taken into account, dynamical complexity even increases: close to the onset of a macroscopic mean field, the dynamics of this field is rather irregular.
Records from ocean bottom seismometers (OBSs) are highly contaminated by noise, which is much stronger
compared to data from most land stations, especially on the horizontal components. As a consequence, the high energy of the oceanic noise at frequencies below 1 Hz considerably complicates the analysis of the teleseismic earthquake signals recorded by OBSs.
Previous studies suggested different approaches to remove low-frequency noises from OBS recordings but mainly focused on the vertical component. The records of horizontal components, which are crucial for the application of many methods in passive seismological analysis of body and surface waves, could not be much improved in the teleseismic frequency band. Here we introduce a noise reduction method, which is derived from the harmonic–percussive separation algorithms used in Zali et al. (2021), in order to separate long-lasting narrowband signals from broadband transients in the OBS signal. This leads to significant noise reduction of OBS records on both the vertical and horizontal components and increases the earthquake signal-to-noise ratio (SNR) without distortion of the broadband earthquake waveforms. This is demonstrated through tests with synthetic data. Both SNR and cross-correlation coefficients showed significant improvements for different realistic noise realizations. The application of denoised signals in surface wave analysis and receiver functions is discussed through tests with synthetic and real data.
Picosecond X-ray absorption spectroscopy (XAS) is used to investigate the electronic and structural dynamics initiated by plasmon excitation of 1.8 nm diameter Au nanoparticles (NPs) functionalised with 1-hexanethiol. We show that 100 ps after photoexcitation the transient XAS spectrum is consistent with an 8% expansion of the Au–Au bond length and a large increase in disorder associated with melting of the NPs. Recovery of the ground state occurs with a time constant of ∼1.8 ns, arising from thermalisation with the environment. Simulations reveal that the transient spectrum exhibits no signature of charge separation at 100 ps and allows us to estimate an upper limit for the quantum yield (QY) of this process to be <0.1.
Venomous snakes often display extensive variation in venom composition both between and within species. However, the mechanisms underlying the distribution of different toxins and venom types among populations and taxa remain insufficiently known. Rattlesnakes (Crotalus, Sistrurus) display extreme inter-and intraspecific variation in venom composition, centered particularly on the presence or absence of presynaptically neurotoxic phospholipases A2 such as Mojave toxin (MTX). Interspecific hybridization has been invoked as a mechanism to explain the distribution of these toxins across rattlesnakes, with the implicit assumption that they are adaptively advantageous. Here, we test the potential of adaptive hybridization as a mechanism for venom evolution by assessing the distribution of genes encoding the acidic and basic subunits of Mojave toxin across a hybrid zone between MTX-positive Crotalus scutulatus and MTX-negative C. viridis in southwestern New Mexico, USA. Analyses of morphology, mitochondrial and single copy-nuclear genes document extensive admixture within a narrow hybrid zone. The genes encoding the two MTX subunits are strictly linked, and found in most hybrids and backcrossed individuals, but not in C. viridis away from the hybrid zone. Presence of the genes is invariably associated with presence of the corresponding toxin in the venom. We conclude that introgression of highly lethal neurotoxins through hybridization is not necessarily favored by natural selection in rattlesnakes, and that even extensive hybridization may not lead to introgression of these genes into another species.
The dynamics of external contributions to the geomagnetic field is investigated by applying time-frequency methods to magnetic observatory data. Fractal models and multiscale analysis enable obtaining maximum quantitative information related to the short-term dynamics of the geomagnetic field activity. The stochastic properties of the horizontal component of the transient external field are determined by searching for scaling laws in the power spectra. The spectrum fits a power law with a scaling exponent β, a typical characteristic of self-affine time-series. Local variations in the power-law exponent are investigated by applying wavelet analysis to the same time-series. These analyses highlight the self-affine properties of geomagnetic perturbations and their persistence. Moreover, they show that the main phases of sudden storm disturbances are uniquely characterized by a scaling exponent varying between 1 and 3, possibly related to the energy contained in the external field. These new findings suggest the existence of a long-range dependence, the scaling exponent being an efficient indicator of geomagnetic activity and singularity detection. These results show that by using magnetogram regularity to reflect the magnetosphere activity, a theoretical analysis of the external geomagnetic field based on local power-law exponents is possible.
Marked along-strike changes in stratigraphy, mountain belt morphology, basement exhumation, and deformation styles characterize the Andean retroarc; these changes have previously been related to spatiotemporal variations in the subduction angle. We modeled new apatite fission track and apatite (U-Th-Sm)/He data from nine ranges located between 26 degrees S and 28 degrees S. Using new and previously published data, we constructed a Cretaceous to Pliocene paleogeographic model that delineates a four-stage tectonic evolution: extensional tectonics during the Cretaceous (120-75 Ma), the formation of a broken foreland basin between 55 and 30 Ma, reheating due to burial beneath sedimentary rocks (18-13 Ma), and deformation, exhumation, and surface uplift during the Late Miocene and the Pliocene (13-3 Ma). Our model highlights how preexisting upper plate structures control the deformation patterns of broken foreland basins. Because retroarc deformation predates flat-slab subduction, we propose that slab anchoring may have been the precursor of Eocene-Oligocene compression in the Andean retroarc. Our model challenges models which consider broken foreland basins and retroarc deformation in the NW Argentinian Andes to be directly related to Miocene flat subduction.
The article starts with an overview of modernization theories, its history of ups and downs as well as its present status. This first part is followed by an analysis of basic social structure distributions and trends in human development in selected countries. One major focal point of the paper is the Non-Western world and the Arab countries, in particular. The author looks at modernization and modernity in that region and comes to the conclusion that the Western world can no longer expect to be able to simply export its own values and its way of life to the rest of the world.
Ecosystems with highly pulsed water supply must be better understood as climate change may increase frequency and severity of intense storms, droughts and floods. Here we collected data over 3 years (2016-2018) in the episodic wetland outflow channel (Aluize), Banhine National Park, in which the system state changed from dry to wet to dry. Field sampling included vegetation records, small-scale vegetation zoning, the seed bank and water and soil quality. The same main plant species were found in both dry and wet conditions across the riverbed of the outflow channel. We found only very few diaspores of plants in the soil after prolonged drought. In the subsequent flooded state, we examined very dense vegetation on the water surface, which was dominated by the gramineous species Paspalidium obtusifolium. This species formed a compact floating mat that was rooted to the riverbed. The Cyperaceae Bolboschoenus glaucus showed high clonal growth in the form of root tubers, which likely serve as important food reservoir during drought. Soil and water analyses do not indicate a limitation by nutrients. We outline how resident people may change the plant community structure with an increasing practice of setting fire to the meadows in the dried-up riverbed to facilitate plant regrowth as food for their livestock.
When it comes to teacher attitudes towards teaching and learning, research relies heavily on explicit measures (e.g., questionnaires). These attitudes are generally conceptualized as constructivist and transmissive views on teaching and learning with constructivism often considered to be more desirable. In explicit measures, this can have drawbacks like socially desirable responding. It is for this reason that, in this study, we investigated implicit attitudes as well as explicit attitudes towards constructivism and transmission. N = 100 preservice teachers worked on a questionnaire and two Single-Target Implicit Association Tests (ST-IAT constructivism and ST-IAT transmission) before (T1) and after (T2) a single master’s semester. One group (n = 50) did student teaching while a second group (n = 50) took master’s courses. We evaluated preservice teachers’ views on teaching at the end of their masters’ studies. Participants agreed with transmission and constructivism (T1) on both an explicit and implicit level. Implicit measures seem to exceed explicit measures in differentially assessing constructivist and transmissive views on teaching and learning. After student teaching (T2), there was no overall effect of attitude development but changes in rank indicate that participants’ implicit attitudes towards constructivism and transmission developed differently for each individual.
(1) Background: People with HIV (PWH) may perform more than one type of exercise cumulatively. The objective of this study is to investigate recreational exercise and its association with health-related quality of life (HRQOL) and comorbidities in relation to potential covariates. (2) Methods: The HIBES study (HIV-Begleiterkrankungen-Sport) is a cross-sectional study for people with HIV. The differences between non-exercisers versus exercisers (cumulated vs. single type of exercises) were investigated using regression models based on 454 participants. (3) Results: Exercisers showed a higher HRQOL score compared to non-exercisers (Wilcox r = 0.2 to 0.239). Psychological disorders were identified as the main covariate. Participants performing exercise cumulatively showed higher scores in duration, frequency, and intensity when compared to participants performing only one type of exercise. The mental health summary score was higher for the cumulated and single type of exercise if a psychological disorder existed. Duration and intensity were associated with an increase of HRQOL, whilst a stronger association between psychological disorders and exercise variables were evident. Exercise duration (minutes) showed a significant effect on QOL (standardized beta = 0.1) and for participants with psychological disorders (standardized beta = 0.3), respectively. (4) Conclusions: Psychological disorders and other covariates have a prominent effect on HRQOL and its association with exercise. For PWH with a psychological disorder, a stronger relationship between HRQOL with exercise duration and intensity emerged. However, differentiation of high-HRQOL individuals warrants further investigation by considering additional factors.