Synchronising ultra-short (~fs) and focussed laser pulses is a particularly difficult task, as this timescale lies orders of magnitude below the typical range of fast electronic devices. Here we present an optical technique that allows for femtosecon
d-scale synchronisation of the focal planes of two focussed laser pulses. This technique is virtually applicable to any focussing geometry and relative intensity of the two lasers. Experimental implementation of this technique provides excellent quantitative agreement with theoretical expectations. The proposed technique will prove highly beneficial for the next generation of multiple, petawatt class laser systems.
Laser-wakefield acceleration is a promising technique for the next generation of ultra-compact, high-energy particle accelerators. However, for a meaningful use of laser-driven particle beams it is necessary that they present a high degree of pointin
g stability in order to be injected into transport lines and further acceleration stages. Here we show a comprehensive experimental study of the main factors limiting the pointing stability of laser-wakefield accelerated electron beams. It is shown that gas-cells provide a much more stable electron generation axis, if compared to gas-jet targets, virtually regardless of the gas density used. A sub-mrad shot-to-shot fluctuation in pointing is measured and a consistent non-zero offset of the electron axis in respect to the laser propagation axis is found to be solely related to a residual angular dispersion introduced by the laser compression system and can be used as a precise diagnostic tool for compression oprtimisation in chirped pulse amplified lasers.
We carry out a first-principles atomistic study of the electronic mechanisms of ligand binding and discrimination in the myoglobin protein. Electronic correlation effects are taken into account using one of the most advanced methods currently availab
le, namely a linear-scaling density functional theory (DFT) approach wherein the treatment of localized iron 3d electrons is further refined using dynamical mean-field theory (DMFT). This combination of methods explicitly accounts for dynamical and multi-reference quantum physics, such as valence and spin fluctuations, of the 3d electrons, whilst treating a significant proportion of the protein (more than 1000 atoms) with density functional theory. The computed electronic structure of the myoglobin complexes and the nature of the Fe-O2 bonding are validated against experimental spectroscopic observables. We elucidate and solve a long standing problem related to the quantum-mechanical description of the respiration process, namely that DFT calculations predict a strong imbalance between O2 and CO binding, favoring the latter to an unphysically large extent. We show that the explicit inclusion of many body-effects induced by the Hunds coupling mechanism results in the correct prediction of similar binding energies for oxy- and carbonmonoxymyoglobin.
We report on the laser-driven generation of purely neutral, relativistic electron-positron pair plasmas. The overall charge neutrality, high average Lorentz factor ($gamma_{e/p} approx 15$), small divergence ($theta_{e/p} approx 10 - 20$ mrad), and h
igh density ($n_{e/p}simeq 10^{15}$cm$^{-3}$) of these plasmas open the pathway for the experimental study of the dynamics of this exotic state of matter, in regimes that are of relevance to electron-positron astrophysical plasmas.
We have extended our study of the competition between the drive and stabilization of plasma microinstabilities by sheared flow to include electromagnetic effects at low plasma $beta$ (the ratio of plasma to magnetic pressure). The extended system of
characteristic equations is formulated, for a dissipative fluid model developed from the gyrokinetic equation, using a twisting mode representation in sheared slab geometry and focusing on the ion temperature gradient mode. Perpendicular flow shear convects perturbations along the field at the speed we denote as $Mc_s$ (where $c_s$ is the sound speed). $M > 1/ sqrt{beta}$ is required to make the system characteristics unidirectional and inhibit eigenmode formation, leaving only transitory perturbations in the system. This typically represents a much larger flow shear than in the electrostatic case, which only needs $M>1$. Numerical investigation of the region $M < 1/sqrt{beta}$ shows the driving terms can conflict, as in the electrostatic case, giving low growth rates over a range of parameters. Also, at modest drive strengths and low $beta$ values typical of experiments, including electromagnetic effects does not significantly alter the growth rates. For stronger flow shear and higher $beta$, geometry characteristic of the spherical tokamak mitigates the effect of an instability of the shear Alfv{e}n wave, driven by the parallel flow shear.
Myoglobin modulates the binding of diatomic molecules to its heme group via hydrogen-bonding and steric interactions with neighboring residues, and is an important benchmark for computational studies of biomolecules. We have performed calculations on
the heme binding site and a significant proportion of the protein environment (more than 1000 atoms) using linear-scaling density functional theory and the DFT+U method to correct for self-interaction errors associated with localized 3d states. We confirm both the hydrogen-bonding nature of the discrimination effect (3.6 kcal/mol) and assumptions that the relative strain energy stored in the protein is low (less than 1 kcal/mol). Our calculations significantly widen the scope for tackling problems in drug design and enzymology, especially in cases where electron localization, allostery or long-ranged polarization influence ligand binding and reaction.
We have studied the segregation of P and B impurities during oxidation of the Si(100) surface by means of combined static and dynamical first-principles simulations based on density functional theory. In the bare surface, dopants segregate to chemica
lly stable surface sites or to locally compressed subsurface sites. Surface oxidation is accompanied by development of tensile surface stress up to 2.9 N/m at a coverage of 1.5 monolayers of oxygen and by formation of oxidised Si species with charges increasing approximately linearly with the number of neighbouring oxygen atoms. Substitutional P and B defects are energetically unstable within the native oxide layer, and are preferentially located at or beneath the Si/SiOx interface. Consistently, first-principles molecular dynamics simulations of native oxide formation on doped surfaces reveal that dopants avoid the formation of P-O and B-O bonds, suggesting a surface oxidation mechanism whereby impurities remain trapped at the Si/SiOx interface. This seems to preclude a direct influence of impurities on the surface electrostatics and, hence, on the interactions with an external environment.
We have developed a classical two- and three-body interaction potential to simulate the hydroxylated, natively oxidised Si surface in contact with water solutions, based on the combination and extension of the Stillinger-Weber potential and of a pote
ntial originally developed to simulate SiO2 polymorphs. The potential parameters are chosen to reproduce the structure, charge distribution, tensile surface stress and interactions with single water molecules of a natively oxidised Si surface model previously obtained by means of accurate density functional theory simulations. We have applied the potential to the case of hydrophilic silicon wafer bonding at room temperature, revealing maximum room temperature work of adhesion values for natively oxidised and amorphous silica surfaces of 97 mJ/m2 and 90mJ/m2, respectively, at a water adsorption coverage of approximately 1 monolayer. The difference arises from the stronger interaction of the natively oxidised surface with liquid water, resulting in a higher heat of immersion (203 mJ/m2 vs. 166 mJ/m2), and may be explained in terms of the more pronounced water structuring close to the surface in alternating layers of larger and smaller density with respect to the liquid bulk. The computed force-displacement bonding curves may be a useful input for cohesive zone models where both the topographic details of the surfaces and the dependence of the attractive force on the initial surface separation and wetting can be taken into account.
