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Ion-matter interaction: the three dimensional version of the thermal spike model. Application to nanoparticle irradiation with swift heavy ions

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 Added by Christian Dufour
 Publication date 2011
  fields Physics
and research's language is English




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In the framework of swift heavy ion - matter interaction, the thermal spike has proved its worth since nearly two decades. This paper deals with the necessary refinement of the computation due to the kind of materials involved i.e. nanomaterials such as multilayered systems or composite films constitued of nanocylinders or nanospheres embedded in matrix. The three dimensional computation of the thermal spike model is applied for the first time in layers containing spherical nanoparticles embedded in a silica matrix. The temperature profile calculated at each point (x,y,z) of the target for times up to $10^{-10}$s allows a possible explanation of the particle shape change under irradiation with swift heavy ions having an energy of several MeV/u.m.a. The comparison made with the former 2D version of the code applied to cylindrical gold nanoparticles confirms the validity of the present 3D version.



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Thermal spike model (TSM) is presently a widely accepted mechanism of swift heavy ion (SHI) - matter interaction. It provides explanation to various SHI induced effects including mixing across interfaces. The model involves electron-phonon (e-p) coupling to predict the evolution of lattice temperature with time. SHI mixing is considered to be a result of diffusion in transient molten state thus achieved. In this work, we assess this conception primarily via tuning the e-p coupling strength by taking a series Pd$_{1-x}$Ni$_x$ of a completely solid soluble binary, and then observing 100 MeV Au ion induced mixing across Pd$_{1-x}$Ni$_x$/Si interfaces. The extent of mixing has been parametrised by the irradiation induced change $Delta sigma^2$ in variances of Pd and Ni depth profiles derived from X-ray photoelectron spectroscopy. The $x$-dependence of $Delta sigma^2$ follows a curve that is concave upward with a prominent minimum. Theoretically, e-p coupling strength determined using density functional theory has been used to solve the equations appropriate to TSM, and then an equivalent quantity L$^2$ proportional to $Delta sigma^2$ has been calculated. L$^2$, however, increases monotonically with $x$ without any minimum, bringing out a convincing disparity between experiment and theory. Perhaps some mechanisms more than the TSM plus the transient molten state diffusion are operative, which can not be foreseen at this point of time.
In this paper we show how single layer graphene can be utilized to study swift heavy ion (SHI) modifications on various substrates. The samples were prepared by mechanical exfoliation of bulk graphite onto SrTiO$_3$, NaCl and Si(111), respectively. SHI irradiations were performed under glancing angles of incidence and the samples were analysed by means of atomic force microscopy in ambient conditions. We show that graphene can be used to check whether the irradiation was successful or not, to determine the nominal ion fluence and to locally mark SHI impacts. In case of samples prepared in situ, graphene is shown to be able to catch material which would otherwise escape from the surface.
High electronic excitations in radiation of metallic targets with swift heavy ion beams at the coulomb barrier play a dominant role in the damaging processes of some metals. The inelastic thermal spike model was developed to describe tracks in materials and is applied in this paper to some systems beams/targets employed recently in some nuclear physics experiments. Taking into account the experimental conditions and the approved electron-phonon coupling factors, the results of the calculation enable to interpret the observation of the fast deformation of some targets.
We experimentally discovered that Al2O3 and MgO exhibit well-pronounced nanometric modifications on the surfaces when irradiated under grazing incidence with 23 MeV I beam, in contrast to normal incidence irradiation with the same ion beam when no damage was found. Moreover, ions in these two materials produce notably different structures: grooves surrounded with nanohillocks on MgO surfaces vs. smoother, roll-like discontinuous structures on the surfaces of Al2O3. To explain these results, detailed numerical simulations were performed. We identified that a presence of the surface inhibits recrystallization process, thereby preventing transient tracks from recovery, and thus forming observable nanopatterns. Furthermore, a difference in the viscosities in molten states in Al2O3 vs. MgO explains the differences in the created nanostructures. Our results thus provide a deeper understanding of the fundamental processes of surface nanostructuring, potentially allowing for controlled production of periodic surface nanopatterns.
In this brief review we discuss the transient processes in solids under irradiation with femtosecond X-ray free-electron-laser (FEL) pulses and swift-heavy ions (SHI). Both kinds of irradiation produce highly excited electrons in a target on extremely short timescales. Transfer of the excess electronic energy into the lattice may lead to observable target modifications such as phase transitions and damage formation. Transient kinetics of material excitation and relaxation under FEL or SHI irradiation are comparatively discussed. The same origin for the electronic and atomic relaxation in both cases is demonstrated. Differences in these kinetics introduced by the geometrical effects ({mu}m-size of a laser spot vs nm-size of an ion track) and initial irradiation (photoabsorption vs an ion impact) are analyzed. The basic mechanisms of electron transport and electron-lattice coupling are addressed. Appropriate models and their limitations are presented. Possibilities of thermal and nonthermal melting of materials under FEL and SHI irradiation are discussed.
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