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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 threshold laser fluence for the onset of surface melting is calculated for Ni films of different thicknesses and for a bulk Ni target using a combined atomistic-continuum computational model. The model combines the classical molecular dynamics (MD) method for simulation of non-equilibrium processes of lattice superheating and fast phase transformations with a continuum description of the laser excitation and subsequent relaxation of the conduction band electrons based on the two-temperature model (TTM). In the hybrid TTM-MD method, MD substitutes the TTM equation for the lattice temperature, and the diffusion equation for the electron temperature is solved simultaneously with MD integration of the equations of motion of atoms. The dependence of the threshold fluence on the film thickness predicted in TTM-MD simulations qualitatively agrees with TTM calculations, while the values of the thresholds for thick films and bulk targets are ∼10% higher in TTM-MD. The quantitative differences between the predictions of TTM and TTM-MD demonstrate that the kinetics of laser melting as well as the energy partitioning between the thermal energy of atomic vibrations and energy of the collective atomic motion driven by the relaxation of the laser-induced pressure should be taken into account in interpretation of experimental results on surface melting. [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]

The mechanisms of disintegration of submicrometer particles irradiated by short laser pulses are studied by a molecular dynamics simulation technique. Simulations at different laser fluences are performed for particles with homogeneous composition and particles with transparent inclusions. Spatially nonuniform deposition of laser energy is found to play a major role in defining the character and the extent of disintegration. The processes that contribute to the disintegration include overheating and explosive decomposition of the illuminated side of the particle, spallation of the backside of large particles, and disruption of the transparent inclusion caused by the relaxation of the laser-induced pressure. The observed mechanisms are related to the nature of the disintegration products and implications of the simulation results for aerosol time-of-flight mass spectrometry are discussed. Application of multiple laser pulses is predicted to be advantageous for efficient mass spectrometry sampling of aerosols with a large size to laser penetration depth ratio.