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1,710 result(s) for "Robinson, Joseph"
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Hundreds of Genes Experienced Convergent Shifts in Selective Pressure in Marine Mammals
Mammal species have made the transition to the marine environment several times, and their lineages represent one of the classical examples of convergent evolution in morphological and physiological traits. Nevertheless, the genetic mechanisms of their phenotypic transition are poorly understood, and investigations into convergence at the molecular level have been inconclusive. While past studies have searched for convergent changes at specific amino acid sites, we propose an alternative strategy to identify those genes that experienced convergent changes in their selective pressures, visible as changes in evolutionary rate specifically in the marine lineages. We present evidence of widespread convergence at the gene level by identifying parallel shifts in evolutionary rate during three independent episodes of mammalian adaptation to the marine environment. Hundreds of genes accelerated their evolutionary rates in all three marine mammal lineages during their transition to aquatic life. These marine-accelerated genes are highly enriched for pathways that control recognized functional adaptations in marine mammals, including muscle physiology, lipid-metabolism, sensory systems, and skin and connective tissue. The accelerations resulted from both adaptive evolution as seen in skin and lung genes, and loss of function as in gustatory and olfactory genes. In regard to sensory systems, this finding provides further evidence that reduced senses of taste and smell are ubiquitous in marine mammals. Our analysis demonstrates the feasibility of identifying genes underlying convergent organism-level characteristics on a genome-wide scale and without prior knowledge of adaptations, and provides a powerful approach for investigating the physiological functions of mammalian genes.
Liquid explosions induced by X-ray laser pulses
Explosions are spectacular and intriguing phenomena that expose the dynamics of matter under extreme conditions. We investigated, using time-resolved imaging, explosions induced by ultraintense X-ray laser pulses in water drops and jets. Our observations revealed an explosive vaporization followed by high-velocity interacting flows of liquid and vapour, and by the generation of shock trains in the liquid jets. These flows are different from those previously observed in laser ablation, owing to a simpler spatial pattern of X-ray absorption. We show that the explosion dynamics in our experiments is consistent with a redistribution of absorbed energy, mediated by a pressure or shock wave in the liquid, and we model the effects of explosions, including their adverse impact on X-ray laser experiments. X-ray laser explosions have predictable dynamics that may prove useful for controlling the state of pure liquids over broad energy scales and timescales, and for triggering pressure-sensitive molecular dynamics in solutions. X-ray-induced explosions in water drops, examined using time-resolved imaging, show interacting high-speed liquid and vapour flows. This type of X-ray absorption dynamics is predictable and may be used for inducing particular dynamical liquid states.
Ultrafast X-ray scattering reveals vibrational coherence following Rydberg excitation
The coherence and dephasing of vibrational motions of molecules constitute an integral part of chemical dynamics, influence material properties and underpin schemes to control chemical reactions. Considerable progress has been made in understanding vibrational coherence through spectroscopic measurements, but precise, direct measurement of the structure of a vibrating excited-state polyatomic organic molecule has remained unworkable. Here, we measure the time-evolving molecular structure of optically excited N -methylmorpholine through scattering with ultrashort X-ray pulses. The scattering signals are corrected for the differences in electron density in the excited electronic state of the molecule in comparison to the ground state. The experiment maps the evolution of the molecular geometry with femtosecond resolution, showing coherent motion that survives electronic relaxation and seems to persist for longer than previously seen using other methods. Quantum coherence and dephasing in molecular motions determine the behaviour of many chemical reactions and are the fundamental basis for the concept of coherent control. Now, ultrafast X-ray scattering combined with a detailed structural determination analysis precisely measures the coherent vibrational motions of a polyatomic organic molecule following photoexcitation.
Bright high-repetition-rate source of narrowband extreme-ultraviolet harmonics beyond 22 eV
Novel table-top sources of extreme-ultraviolet light based on high-harmonic generation yield unique insight into the fundamental properties of molecules, nanomaterials or correlated solids, and enable advanced applications in imaging or metrology. Extending high-harmonic generation to high repetition rates portends great experimental benefits, yet efficient extreme-ultraviolet conversion of correspondingly weak driving pulses is challenging. Here, we demonstrate a highly-efficient source of femtosecond extreme-ultraviolet pulses at 50-kHz repetition rate, utilizing the ultraviolet second-harmonic focused tightly into Kr gas. In this cascaded scheme, a photon flux beyond ≈3 × 10 13  s −1 is generated at 22.3 eV, with 5 × 10 −5 conversion efficiency that surpasses similar harmonics directly driven by the fundamental by two orders-of-magnitude. The enhancement arises from both wavelength scaling of the atomic dipole and improved spatio-temporal phase matching, confirmed by simulations. Spectral isolation of a single 72-meV-wide harmonic renders this bright, 50-kHz extreme-ultraviolet source a powerful tool for ultrafast photoemission, nanoscale imaging and other applications. Table-top extreme-ultraviolet (XUV) light sources with high repetition rates are sought for fundamental studies, metrology and imaging. Here, Wang et al . demonstrate the efficient generation of bright XUV harmonics at 50-kHz repetition rate, with very high photon flux and spectral definition.
Inequities in Educational and Psychological Outcomes Between LGBTQ and Straight Students in Middle and High School
This study finds that, compared with straight-identified youth, youth who identify as lesbian, gay, bisexual, transgender, or questioning (LGBTQ) are at greater risk of suicidal thoughts, suicide attempts, victimization by peers, and elevated levels of unexcused absences from school. Results disaggregated by LGBTQ subgroups reveal heterogeneity within the broad LGBTQ group, with bisexual youth appearing to be particularly at risk. Also, although the risk gaps in school belongingness and unexcused absences are significant in high school, we find that these gaps are significantly greater in middle school, suggesting heightened early risk for LGBTQ-identified students.By raising awareness of educational inequities related to LGBTQ identification, this study lays the descriptive groundwork for interventions aimed at improving psychological and educational outcomes for these students.
Tracking excited-state charge and spin dynamics in iron coordination complexes
Femtosecond resolution X-ray fluorescence spectroscopy is shown to track the charge and spin dynamics triggered when an iron coordination complex is excited by light, and establishes the critical role of intermediate spin states in the de-excitation process. Tracking 3 d excitations in transition metal compounds The absorption and dissipation of light energy by 3 d transition metal complexes has a crucial role in photosynthesis and many artificial systems that harvest solar energy, but understanding this complex phenomenon in detail remains challenging. Wenkai Zhang and colleagues now show that femtosecond resolution X-ray fluorescence spectroscopy can overcome the limitations of existing methods for probing the excited-state dynamics involved. This is illustrated for a prototypical iron complex, where tracking of the charge and spin dynamics triggered upon light-excitation establishes the critical role of intermediate spin states in the de-excitation process. The authors anticipate that their method will finally enable the detailed mapping — and hence understanding — of the fundamental processes that underpin many useful light-triggered molecular phenomena involving 3 d transition metal complexes. Crucial to many light-driven processes in transition metal complexes is the absorption and dissipation of energy by 3 d electrons 1 , 2 , 3 , 4 . But a detailed understanding of such non-equilibrium excited-state dynamics and their interplay with structural changes is challenging: a multitude of excited states and possible transitions result in phenomena too complex to unravel when faced with the indirect sensitivity of optical spectroscopy to spin dynamics 5 and the flux limitations of ultrafast X-ray sources 6 , 7 . Such a situation exists for archetypal polypyridyl iron complexes, such as [Fe(2,2′-bipyridine) 3 ] 2+ , where the excited-state charge and spin dynamics involved in the transition from a low- to a high-spin state (spin crossover) have long been a source of interest and controversy 6 , 7 , 8 , 9 , 10 , 11 , 12 , 13 , 14 , 15 . Here we demonstrate that femtosecond resolution X-ray fluorescence spectroscopy, with its sensitivity to spin state, can elucidate the spin crossover dynamics of [Fe(2,2′-bipyridine) 3 ] 2+ on photoinduced metal-to-ligand charge transfer excitation. We are able to track the charge and spin dynamics, and establish the critical role of intermediate spin states in the crossover mechanism. We anticipate that these capabilities will make our method a valuable tool for mapping in unprecedented detail the fundamental electronic excited-state dynamics that underpin many useful light-triggered molecular phenomena involving 3 d transition metal complexes.
NMY-2, TOE-2 and PIG-1 regulate Caenorhabditis elegans asymmetric cell divisions
Asymmetric cell division is an important mechanism that generates cellular diversity during development. Not only do asymmetric cell divisions produce daughter cells of different fates, but many can also produce daughters of different sizes, which we refer to as Daughter Cell Size Asymmetry (DCSA). In Caenorhabditis elegans , apoptotic cells are frequently produced by asymmetric divisions that exhibit DCSA, where the smaller daughter dies. We focus here on the divisions of the Q.a and Q.p neuroblasts, which produce larger surviving cells and smaller apoptotic cells and divide with opposite polarity using both distinct and overlapping mechanisms. Several proteins regulate DCSA in these divisions. Previous studies showed that the PIG-1/MELK and TOE-2 proteins regulate DCSA in both the Q.a and Q.p divisions, and the non-muscle myosin NMY-2 regulates DCSA in the Q.a division but not the Q.p division. In this study, we examined endogenously tagged NMY-2, TOE-2, and PIG-1 reporters and characterized their distribution at the cortex during the Q.a and Q.p divisions. In both divisions, TOE-2 localized toward the side of the dividing cell that produced the smaller daughter, whereas PIG-1 localized toward the side that produced the larger daughter. As previously reported, NMY-2 localized to the side of Q.a that produced the smaller daughter and did not localize asymmetrically in Q.p. We used temperature-sensitive nmy-2 mutants to determine the role of nmy-2 in these divisions and were surprised to find that these mutants only displayed DCSA defects in the Q.p division. We generated double mutant combinations between the nmy-2 mutations and mutations in toe-2 and pig-1 . Because previous studies indicate that DCSA defects result in the transformation of cells fated to die into their sister cells, the finding that the nmy-2 mutations did not significantly alter the Q.a and Q.p DCSA defects of toe-2 and pig-1 mutants but did alter the number of daughter cells produced by Q.a and Q.p suggests that nmy-2 plays a role in specifying the fates of the Q.a and Q.p that is independent of its role in DCSA.
Ultrafast X-ray scattering offers a structural view of excited-state charge transfer
Intramolecular charge transfer and the associated changes in molecular structure in N,N′-dimethylpiperazine are tracked using femtosecond gas-phase X-ray scattering. The molecules are optically excited to the 3p state at 200 nm. Following rapid relaxation to the 3s state, distinct charge-localized and charge-delocalized species related by charge transfer are observed. The experiment determines the molecular structure of the two species, with the redistribution of electron density accounted for by a scattering correction factor. The initially dominant charge-localized state has a weakened carbon–carbon bond and reorients one methyl group compared with the ground state. Subsequent charge transfer to the charge-delocalized state elongates the carbon–carbon bond further, creating an extended 1.634 Å bond, and also reorients the second methyl group. At the same time, the bond lengths between the nitrogen and the ring-carbon atoms contract from an average of 1.505 to 1.465 Å. The experiment determines the overall charge transfer time constant for approaching the equilibrium between charge-localized and charge-delocalized species to 3.0 ps.
Observation of the molecular response to light upon photoexcitation
When a molecule interacts with light, its electrons can absorb energy from the electromagnetic field by rapidly rearranging their positions. This constitutes the first step of photochemical and photophysical processes that include primary events in human vision and photosynthesis. Here, we report the direct measurement of the initial redistribution of electron density when the molecule 1,3-cyclohexadiene (CHD) is optically excited. Our experiments exploit the intense, ultrashort hard x-ray pulses of the Linac Coherent Light Source (LCLS) to map the change in electron density using ultrafast x-ray scattering. The nature of the excited electronic state is identified with excellent spatial resolution and in good agreement with theoretical predictions. The excited state electron density distributions are thus amenable to direct experimental observation. Photoabsorption is a fundamental process that leads to changes in the electron density in matter. Here, the authors show a direct measurement of the distribution of electron density when a cyclohexadine molecule is excited by pulsed UV radiation and probed by a time delayed X-ray pulse generated at LCLS.