X-ray free-electron lasers enable the investigation of the structure and dynamics of diverse systems, including atoms, molecules, nanocrystals and single bioparticles, under extreme conditions. Many ...imaging applications that target biological systems and complex materials use hard X-ray pulses with extremely high peak intensities (exceeding 10
watts per square centimetre). However, fundamental investigations have focused mainly on the individual response of atoms and small molecules using soft X-rays with much lower intensities. Studies with intense X-ray pulses have shown that irradiated atoms reach a very high degree of ionization, owing to multiphoton absorption, which in a heteronuclear molecular system occurs predominantly locally on a heavy atom (provided that the absorption cross-section of the heavy atom is considerably larger than those of its neighbours) and is followed by efficient redistribution of the induced charge. In serial femtosecond crystallography of biological objects-an application of X-ray free-electron lasers that greatly enhances our ability to determine protein structure-the ionization of heavy atoms increases the local radiation damage that is seen in the diffraction patterns of these objects and has been suggested as a way of phasing the diffraction data. On the basis of experiments using either soft or less-intense hard X-rays, it is thought that the induced charge and associated radiation damage of atoms in polyatomic molecules can be inferred from the charge that is induced in an isolated atom under otherwise comparable irradiation conditions. Here we show that the femtosecond response of small polyatomic molecules that contain one heavy atom to ultra-intense (with intensities approaching 10
watts per square centimetre), hard (with photon energies of 8.3 kiloelectronvolts) X-ray pulses is qualitatively different: our experimental and modelling results establish that, under these conditions, the ionization of a molecule is considerably enhanced compared to that of an individual heavy atom with the same absorption cross-section. This enhancement is driven by ultrafast charge transfer within the molecule, which refills the core holes that are created in the heavy atom, providing further targets for inner-shell ionization and resulting in the emission of more than 50 electrons during the X-ray pulse. Our results demonstrate that efficient modelling of X-ray-driven processes in complex systems at ultrahigh intensities is feasible.
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IJS, KISLJ, NUK, SBMB, UL, UM, UPUK
ABSTRACT We report the first hard X-ray observations with NuSTAR of the BL Lac-type blazar PKS 2155-304, augmented with soft X-ray data from XMM-Newton and γ-ray data from the Fermi Large Area ...Telescope, obtained in 2013 April when the source was in a very low flux state. A joint NuSTAR and XMM spectrum, covering the energy range 0.5-60 keV, is best described by a model consisting of a log-parabola component with curvature and a (local) photon index 3.04 0.15 at photon energy of 2 keV, and a hard power-law tail with photon index 2.2 0.4. The hard X-ray tail can be smoothly joined to the quasi-simultaneous γ-ray spectrum by a synchrotron self-Compton component produced by an electron distribution with index p = 2.2. Assuming that the power-law electron distribution extends down to γmin = 1 and that there is one proton per electron, an unrealistically high total jet power of Lp ∼ 1047 erg s−1 is inferred. This can be reduced by two orders of magnitude either by considering a significant presence of electron-positron pairs with lepton-to-proton ratio , or by introducing an additional, low-energy break in the electron energy distribution at the electron Lorentz factor γbr1 ∼ 100. In either case, the jet composition is expected to be strongly matter-dominated.
The hemoprotein myoglobin is a model system for the study of protein dynamics. We used time-resolved serial femtosecond crystallography at an x-ray free-electron laser to resolve the ultrafast ...structural changes in the carbonmonoxy myoglobin complex upon photolysis of the Fe-CO bond. Structural changes appear throughout the protein within 500 femtoseconds, with the C, F, and H helices moving away from the heme cofactor and the E and A helices moving toward it. These collective movements are predicted by hybrid quantum mechanics/molecular mechanics simulations. Together with the observed oscillations of residues contacting the heme, our calculations support the prediction that an immediate collective response of the protein occurs upon ligand dissociation, as a result of heme vibrational modes coupling to global modes of the protein.
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The interaction of intense femtosecond x-ray pulses with molecules sensitively depends on the interplay between multiple photoabsorptions, Auger decay, charge rearrangement, and nuclear motion. Here, ...we report on a combined experimental and theoretical study of the ionization and fragmentation of iodomethane (CH3I) by ultraintense (∼ 1019 W/cm2) x-ray pulses at 8.3 keV, demonstrating how these dynamics depend on the x-ray pulse energy and duration. We show that the timing of multiple ionization steps leading to a particular reaction product and, thus, the product's final kinetic energy, is determined by the pulse duration rather than the pulse energy or intensity. While the overall degree of ionization is mainly defined by the pulse energy, our measurement reveals that the yield of the fragments with the highest charge states is enhanced for short pulse durations, in contrast to earlier observations for atoms and small molecules in the soft x-ray domain. We attribute this effect to a decreased charge transfer efficiency at larger internuclear separations, which are reached during longer pulses.
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CMK, CTK, FMFMET, IJS, NUK, PNG, UL, UM
X-ray crystallography of G protein-coupled receptors and other membrane proteins is hampered by difficulties associated with growing sufficiently large crystals that withstand radiation damage and ...yield high-resolution data at synchrotron sources. We used an x-ray free-electron laser (XFEL) with individual 50-femtosecond-duration x-ray pulses to minimize radiation damage and obtained a high-resolution room-temperature structure of a human serotonin receptor using sub-10-micrometer microcrystals grown in a membrane mimetic matrix known as lipidie cubic phase. Compared with the structure solved by using traditional microcrystallography from cryo-cooled crystals of about two orders of magnitude larger volume, the room-temperature XFEL structure displays a distinct distribution of thermal motions and conformations of residues that likely more accurately represent the receptor structure and dynamics in a cellular environment.
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Serial femtosecond crystallography (SFX) using X-ray free-electron laser sources is an emerging method with considerable potential for time-resolved pump-probe experiments. Here we present a lipidic ...cubic phase SFX structure of the light-driven proton pump bacteriorhodopsin (bR) to 2.3 Å resolution and a method to investigate protein dynamics with modest sample requirement. Time-resolved SFX (TR-SFX) with a pump-probe delay of 1 ms yields difference Fourier maps compatible with the dark to M state transition of bR. Importantly, the method is very sample efficient and reduces sample consumption to about 1 mg per collected time point. Accumulation of M intermediate within the crystal lattice is confirmed by time-resolved visible absorption spectroscopy. This study provides an important step towards characterizing the complete photocycle dynamics of retinal proteins and demonstrates the feasibility of a sample efficient viscous medium jet for TR-SFX.
The flight of the GAPS prototype experiment von Doetinchem, P.; Aramaki, T.; Bando, N. ...
Astroparticle physics,
February 2014, 2014-02-00, 20140201, Volume:
54
Journal Article
Peer reviewed
Open access
The General AntiParticle Spectrometer experiment (GAPS) is foreseen to carry out a dark matter search using low-energy cosmic ray antideuterons at stratospheric altitudes with a novel detection ...approach. A prototype flight from Taiki, Japan was carried out in June 2012 to prove the performance of the GAPS instrument subsystems (Lithium-drifted Silicon tracker and time-of-flight) and the thermal cooling concept as well as to measure background levels. The flight was a success and the stable flight operation of the GAPS detector concept was proven. During the flight about 106 charged particle triggers were recorded, extensive X-ray calibrations of the individual tracker modules were performed by using an onboard X-ray tube, and the background level of atmospheric and cosmic X-rays was measured. The behavior of the tracker performance as a function of temperature was investigated. The tracks of charged particle events were reconstructed and used to study the tracking resolution, the detection efficiency of the tracker, and coherent X-ray backgrounds. A timing calibration of the time-of-flight subsystem was performed to measure the particle velocity. The flux as a function of flight altitude and as a function of velocity was extracted taking into account systematic instrumental effects. The developed analysis techniques will form the basis for future flights.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK
In core-collapse supernovae, titanium-44 (44Ti) is produced in the innermost ejecta, in the layer of material directly on top of the newly formed compact object. As such, it provides a direct probe ...of the supernova engine. Observations of supernova 1987A (SN1987A) have resolved the 67.87- and 78.32–kilo–electron volt emission lines from decay of 44Ti produced in the supernova explosion. These lines are narrow and redshifted with a Doppler velocity of ∼700 kilometers per second, direct evidence of large-scale asymmetry in the explosion.
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ABSTRACT The distribution of elements produced in the innermost layers of a supernova explosion is a key diagnostic for studying the collapse of massive stars. Here we present the results of a 2.4 Ms ...NuSTAR observing campaign aimed at studying the supernova remnant Cassiopeia A (Cas A). We perform spatially resolved spectroscopic analyses of the 44Ti ejecta, which we use to determine the Doppler shift and thus the three-dimensional (3D) velocities of the 44Ti ejecta. We find an initial 44Ti mass of (1.54 0.21) × 10−4 M , which has a present-day average momentum direction of 340° 15° projected onto the plane of the sky (measured clockwise from celestial north) and is tilted by 58° 20° into the plane of the sky away from the observer, roughly opposite to the inferred direction of motion of the central compact object. We find some 44Ti ejecta that are clearly interior to the reverse shock and some that are clearly exterior to it. Where we observe 44Ti ejecta exterior to the reverse shock we also see shock-heated iron; however, there are regions where we see iron but do not observe 44Ti. This suggests that the local conditions of the supernova shock during explosive nucleosynthesis varied enough to suppress the production of 44Ti by at least a factor of two in some regions, even in regions that are assumed to be the result of processes like -rich freezeout that should produce both iron and titanium.
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