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Register a new userOn the feasibility of nanocrystal imaging using intense and ultrashort 1.5 {AA} X-ray pulses
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Structural studies of biological macromolecules are severely limited by radiation damage. Traditional crystallography curbs the effects of damage by spreading damage over many copies of the molecule of interest. X-ray lasers, such as the recently built LINAC Coherent Light Source (LCLS), offer an additional opportunity for limiting damage by out-running damage processes with ultrashort and very intense X-ray pulses. Such pulses may allow the imaging of single molecules, clusters or nanoparticles, but coherent flash imaging will also open up new avenues for structural studies on nano- and micro-crystalline substances. This paper addresses the theoretical potentials and limitations of nanocrystallography with extremely intense coherent X-ray pulses. We use urea nanocrystals as a model for generic biological substances and simulate primary and secondary ionization dynamics in the crystalline sample. Our results establish conditions for ultrafast nanocrystallography diffraction experiments as a function of fluence and pulse duration.
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The spectrum of laser-plasma generated X-rays is very important, it characterizes electron dynamics in plasma and is basic for applications. However, the accuracies and efficiencies of existing methods to diagnose the spectrum of laser-plasma based X-ray pulse are not very high, especially in the range of several hundred keV. In this study, a new method based on electron tracks detection to measure the spectrum of laser-plasma produced X-ray pulses is proposed and demonstrated. Laser-plasma generated X-rays are scattered in a multi-pixel silicon tracker. Energies and scattering directions of Compton electrons can be extracted from the response of the detector, and then the spectrum of X-rays can be reconstructed. Simulations indicate that the energy resolution of this method is approximately 20% for X-rays from 200 to 550 keV for a silicon-on-insulator pixel detector with 12 $rm mu$m pixel pitch and 500 $rm mu$m depletion region thickness. The results of a proof-of-principle experiment based on a Timepix3 detector are also shown.
The interaction of 32.5 and 6 nm ultrashort X-ray pulses with the solid materials B4C, SiC and Si is simulated with a non-local thermodynamic equilibrium (NLTE) radiation transfer code. We study the ionization dynamics as function of depth in the material, modifications of the opacity during irradiation and estimate crater depth. Furthermore, we compare the estimated crater depth with experimental data, for fluences up to 2.2 J/cm2. Our results show that at 32.5 nm irradiation, the opacity changes with less than a factor of 2 for B4C and Si and a factor of 3 for SiC, for fluences up to 200 J/cm2. At a laser wavelength of 6 nm, the model predicts a dramatic decrease in opacity due to the weak inverse bremsstrahlung, increasing the crater depth for high fluences.
We present the results of an experiment where amorphous carbon was irradiated by femtosecond x-ray free electron laser pulses. The 830 eV laser pulses induce a phase transition in the material which is characterized ex-situ. The phase transition energy threshold is determined by measuring the surface of each irradiated area using an optical Nomarski microscope. The threshold fluence is found to be 282 +/- 11 mJ/cm^2, corresponding to an absorbed dose at the surface of 131 +/-5 meV/atom. Atomic force microscopy measurements show volume expansion of the irradiated sample area, suggesting a solid to solid phase transition. Deeper insight into the phase transition is gained by using scanning photoelectron microscopy and micro-Raman spectroscopy. Photoelectron microscopy shows graphitization, i.e. modification from sp3 to sp2 hybridization, of the irradiated material. The micro-Raman spectra show the appearance of local order, i.e. formation of graphite nanocrystals. Finally, the nature of the phase transition is discussed, taking into account previous theory and experimental results.
A theoretical comparison of the electronic excitation and ionisation behaviour of molecular hydrogen oriented either parallel or perpendicular to a linear polarised laser pulse is performed. The investigation is based on a non-perturbative treatment that solves the full time-dependent Schrodinger equation of both correlated electrons within the fixed-nuclei approximation and the dipole. Results are shown for two different laser pulse lengths and intensities as well as for a large variety of photon frequencies starting in the 1- and reaching into the 6-photon regime. In order to investigate the influence of the intrinsic diatomic two-center problem even further, two values of the internuclear separation and a newly developed atomic model are considered.
The laser-induced fragmentation dynamics of this most fundamental polar molecule HeH$^+$ are measured using an ion beam of helium hydride and an isotopologue at various wavelengths and intensities. In contrast to the prevailing interpretation of strong-field fragmentation, in which stretching of the molecule results primarily from laser-induced electronic excitation, experiment and theory for nonionizing dissociation, single ionization and double ionization both show that the direct vibrational excitation plays the decisive role here. We are able to reconstruct fragmentation pathways and determine the times at which each ionization step occurs as well as the bond length evolution before the electron removal. The dynamics of this extremely asymmetric molecule contrast the well-known symmetric systems leading to a more general picture of strong-field molecular dynamics and facilitating interpolation to systems between the two extreme cases.
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