פרסומים

Single-molecule, protein-induced fluorescence enhancement (PIFE) serves as a molecular ruler at molecular distances inaccessible to other spectroscopic rulers such as Förster-type resonance energy transfer (FRET) or photoinduced electron transfer. In order to provide two simultaneous measurements of two distances on different molecular length scales for the analysis of macromolecular complexes, we and others recently combined measurements of PIFE and FRET (PIFE-FRET) on the single molecule level. PIFE relies on steric hindrance of the fluorophore Cy3, which is covalently attached to a biomolecule of interest, to rotate out of an excited-state trans isomer to the cis isomer through a 90° intermediate. In this work, we provide a theoretical framework that accounts for relevant photophysical and kinetic parameters of PIFE-FRET, show how this framework allows the extraction of the fold-decrease in isomerization mobility from experimental data, and show how these results provide information on changes in the accessible volume of Cy3. The utility of this model is then demonstrated for experimental results on PIFE-FRET measurement of different protein-DNA interactions. The proposed model and extracted parameters could serve as a benchmark to allow quantitative comparison of PIFE effects in different biological systems.

Various engine types are thermodynamically equivalent in the quantum limit of small “engine action”. Our previous derivation of the equivalence is restricted to Markovian heat baths and to implicit classical work repository (e.g., laser light in the semi-classical approximation). In this paper, all the components, baths, batteries, and engines, are explicitly taken into account. To neatly treat non-Markovian dynamics, we use mediating particles that function as a heat exchanger. We find that, on top of the previously observed equivalence, there is a higher degree of equivalence that cannot be achieved in the Markovian regime. Next, we focus on the quality of the battery charging process. A condition for positive energy increase and zero entropy increase (work) is given. Moreover, it is shown that, in the strong coupling regime, it is possible to super-charge a battery. With super-charging, the energy of the battery is increased while its entropy is being reduced at the same time.

We experimentally demonstrate the protection of a room-temperature hybrid spin register against environmental decoherence by performing repeated quantum error correction whilst maintaining sensitivity to signal fields. We use a long-lived nuclear spin to correct multiple phase errors on a sensitive electron spin in diamond and realize magnetic field sensing beyond the time scales set by natural decoherence. The universal extension of sensing time, robust to noise at any frequency, demonstrates the definitive advantage entangled multiqubit systems provide for quantum sensing and offers an important complement to quantum control techniques.

The quantum wave packet dynamics following a coherent electronic excitation of LiH by an ultrashort, polarized, strong one cycle infrared optical pulse is computed on several electronic states using a grid method. The coupling to the strong field of the pump and the probe pulses is included in the Hamiltonian used to solve the time-dependent Schrodinger equation. The polarization of the pump pulse allows us to control the localization in time and in space of the nonequilibrium coherent electronic motion and the subsequent nuclear dynamics. We show that transient absorption, resulting from the interaction of the total molecular dipole with the electric fields of the pump and the probe, is a very versatile probe of the different time scales of the vibronic dynamics. It allows probing both the ultrashort, femtosecond time scale of the electronic coherences as well as the longer dozens of femtoseconds time scales of the nuclear motion on the excited electronic states. The ultrafast beatings of the electronic coherences in space and in time are shown to be modulated by the different periods of the nuclear motion.

Quasi-block copolymers (q-BCPs) are block copolymers consisting of conventional and supramolecular blocks, in which the conventional block is end-terminated by a functionality that interacts with the supramolecular monomer (a ‘‘chain stopper’’ functionality). A new design of q-BCPs based on a general polymeric chain stopper, which consists of polystyrene end-terminated with a sulfonate group (PS-SO3Li), is described. Through viscosity measurements and a detailed diffusion-ordered NMR spectroscopy study, it is shown that PS-SO3Li can effectively cap two types of model supramolecular monomers to form q-BCPs in solution. Furthermore, differential scanning calorimetry data and structural characterization of thin films by scanning force microscopy suggests the existence of the q-BCP architecture in the melt. The new design considerably simplifies the synthesis of polymeric chain stoppers; thus promoting the utilization of q-BCPs as smart, nanostructured materials.

Religious experiences have long been documented in patients with epilepsy, though their exact underlying neural mechanisms are still unclear. Here, we had the rare opportunity to record a delusional religious conversion in real time in a patient with right temporal lobe epilepsy undergoing continuous video-EEG. In this patient, a messianic revelation experience occurred several hours after a complex partial seizure of temporal origin, compatible with postictal psychosis (PIP). We analyzed the recorded resting-state EEG epochs separately for each of the conventional frequency bands. Topographical analysis of the bandpass filtered EEG epochs revealed increased activity in the low-gamma range (30-40Hz) during religious conversion compared with activity during the patient's habitual state. The brain generator underlying this activity was localized to the left prefrontal cortex. This suggests that religious conversion in PIP is related to control mechanisms in the prefrontal lobe-related processes rather than medial temporal lobe-related processes.

Interest in male mosquitoes has been motivated by the potential to develop novel vector control strategies, exploiting the fact that males do not feed on blood or transmit diseases, such as malaria. However, genetic studies of male Anopheles mosquitoes have been impeded by the lack of molecular characterization of the Y chromosome. Here we show that the Anopheles gambiae Y chromosome contains a very small repertoire of genes, with massively amplified tandem arrays of a small number of satellites and transposable elements constituting the vast majority of the sequence. These genes and repeats evolve rapidly, bringing about remodeling of the Y, even among closely related species. Our study provides a long-awaited foundation for studying mosquito Y chromosome biology and evolution.Y chromosomes control essential male functions in many species, including sex determination and fertility. However, because of obstacles posed by repeat-rich heterochromatin, knowledge of Y chromosome sequences is limited to a handful of model organisms, constraining our understanding of Y biology across the tree of life. Here, we leverage long single-molecule sequencing to determine the content and structure of the nonrecombining Y chromosome of the primary African malaria mosquito, Anopheles gambiae. We find that the An. gambiae Y consists almost entirely of a few massively amplified, tandemly arrayed repeats, some of which can recombine with similar repeats on the X chromosome. Sex-specific genome resequencing in a recent species radiation, the An. gambiae complex, revealed rapid sequence turnover within An. gambiae and among species. Exploiting 52 sex-specific An. gambiae RNA-Seq datasets representing all developmental stages, we identified a small repertoire of Y-linked genes that lack X gametologs and are not Y-linked in any other species except An. gambiae, with the notable exception of YG2, a candidate male-determining gene. YG2 is the only gene conserved and exclusive to the Y in all species examined, yet sequence similarity to YG2 is not detectable in the genome of a more distant mosquito relative, suggesting rapid evolution of Y chromosome genes in this highly dynamic genus of malaria vectors. The extensive characterization of the An. gambiae Y provides a long-awaited foundation for studying male mosquito biology, and will inform novel mosquito control strategies based on the manipulation of Y chromosomes.

RAS is a molecular switch that regulates a large number of pathways through interactions with many effector proteins. Most RAS/effector complexes are short-lived, demonstrating fast association and fast dissociation rate and Kds ranging from 10(-8)-10(-5) M, compatible with the signaling function of these interactions in the cell. RAS effectors share little sequence homology but all contain an RAS binding domain that exhibits ubiquitin fold. All effectors bind to the same epitope on RAS by forming an intermolecular beta sheet and creating a number of favorable hydrogen bonds and salt bridges across the binding interface. Several hot-spots on both RAS and effector molecules constitute a general recognition mode. RAS/effector interactions occur only when RAS is found in the active, GTP-bound state, and are disrupted upon GTP hydrolysis, most probably due to increased flexibility of the RAS molecule. Recent NMR studies demonstrate how in the presence of multiple binding partners, RAS prefers certain effectors to others. The hierarchy of these interactions could be altered for RAS oncogenic mutants, thus perturbing the network of the downstream signaling. Insights obtained through biophysical and structural studies of effectors interacting with RAS and its mutants establish the basic principles that could be used for designing drugs in RAS-associated diseases.

Archaeologists generally agree that high-power computer technology constitutes the most efficient venue for addressing many issues in archaeological research. Digital techniques have become indispensable components of archaeological surveys, fieldwork, lab work, and communication between researchers. One of the greatest advantages of the digital approach is its ability to examine large assemblages of items using advanced statistical methods. Digital documentation has reached the point of no return in archaeological research, and reverting to traditional methods is highly improbable. However, digital data may also contain additional information that has yet to be extracted by computer analysis. In this arena, new computer algorithms can be triggered by research questions that cannot be addressed without digital models.