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Molecular dynamics simulations were performed to characterize the ablation process induced by a picosecond infrared laser (PIRL) operating in the regime of desorption by impulsive vibrational excitation (DIVE) of a model peptide (lysozyme)/counter-ion system in aqueous solution. The simulations were performed for ablation under typical experimental conditions found within a time-of-flight mass spectrometer (TOF-MS), that is in vacuum with an applied electric field (E = ± 107 V/m), for up to 2 ns post-ablation and compared to the standard PIRL-DIVE ablation condition (E = 0 V/m). Further, a simulation of ablation under an extreme field condition (E = 1010 V/m) was performed for comparison to extend the effective dynamic range of the effect of the field on charge separation. The results show that the plume dynamics were retained under a typical TOF-MS condition within the first 1 ns of ablation. Efficient desorption was observed with more than 90% of water molecules interacting with lysozyme stripped off within 1 ns post-ablation. The processes of ablation and desolvation of analytes were shown to be independent of the applied electric field and thus decoupled from the ion separation process. Unlike under the extreme field conditions, the electric field inside a typical TOF-MS was shown to modify the ions' motion over a longer time and in a soft manner with no enhancement to fragmentation observed as compared to the standard PIRL-DIVE. The study indicates that the PIRL-DIVE ablation mechanism could be used as a new, intrinsically versatile, and highly sensitive ion source for quantitative mass spectrometry. [ABSTRACT FROM AUTHOR]

Graphene crystals, containing arrays of disclination defects, are modeled and their energies are calculated exploring molecular dynamics (MD) simulation technique. Two cases are analyzed in details: (i) pseudo-graphenes, which contain the alternating sign disclination ensembles and (ii) graphene with periodic distribution of disclination quadrupoles. Electronic band structures of disclinated graphene crystals are calculated in the framework of density functional theory (DFT) approach. The evolution of the Dirac cone and magnitude of band gap in the band structure reveal a dependence on the density of disclination quadrupoles and alternating sign disclinations. The electronic properties of graphene with disclination ensembles are discussed. [ABSTRACT FROM AUTHOR]

A systematic approach to constructing intercrystallite boundaries (IBs) in graphene is developed based on the structural units (SUs) model of grain boundaries (GBs). The approach operates with SUs composed of carbon octagons, heptagons, pentagons and squares, which correspond to six-member carbon rings of an ideal hexagonal graphene lattice altered by wedge disclinations of different strength. A linear periodic arrangement of SUs containing disclination dipoles and quadrupoles is used to construct IBs in graphene. The energies of symmetric IBs are calculated in molecular dynamics simulations and are used for evaluation of the feasibility of experimental fabrication of the IBs in graphene. [ABSTRACT FROM AUTHOR]

The synthesis of metal nanoparticles by ultrafast laser ablation of nanometers-thick metal films has been studied experimentally and computationally. Near-threshold backside laser ablation of 2-20 nm-thick Pt films deposited on fused silica substrates was found to produce nanoparticles with size distributions that were bimodal for the thicker films, but collapsed into a single mode distribution for the thinnest film. Time-resolved imaging of blackbody emission from the Pt nanoparticles was used to reveal the nanoparticle propagation dynamics and estimate their temperatures. The observed nanoparticle plume was compact and highly forward-directed with a well-defined collective velocity that permitted multiple rebounds with substrates to be revealed. Large-scale molecular dynamics simulations were used to understand the evolution of compressive and tensile stresses in the thicker melted liquid films that lead to their breakup and ejection of two groups of nanoparticles with different velocity and size distributions. Ultrafast laser irradiation of ultrathin (few nm) metal films avoids the splitting of the film and appears to be a method wellsuited to cleanly synthesize and deposit nanoparticles from semitransparent thin film targets in highly directed beams. [ABSTRACT FROM AUTHOR]

The mechanisms of photomechanical spallation are investigated in a large-scale MD simulation of laser interaction with a molecular target performed in an irradiation regime of inertial stress confinement. The relaxation of laser-induced thermoelastic stresses is found to be responsible for the nucleation, growth, and coalescence of voids in a broad sub-surface region of the irradiated target. The depth of the region subjected to void evolution is defined by the competition between the evolving tensile stresses and thermal softening of the material due to the laser heating. The initial void volume distribution obtained in the simulation of laser spallation can be well described by a power law. A similar volume distribution is obtained in a series of simulations of uniaxial expansion of the same molecular system performed at a strain rate and temperature realized in the irradiated target. Spatial and time evolution of the laser-induced pressure predicted in the MD simulation of laser spallation is related to the results of an integration of a thermoelastic wave equation. The scope of applicability of the continuum calculations is discussed. [ABSTRACT FROM AUTHOR]