Suchergebnisse

Electronic excitations and ionisations produced by electron impact are key processes in the radiation-induced damage mechanisms in materials of biological relevance, underlying important medical and technological applications, including radiotherapy, radiation protection in manned space missions and nanodevice fabrication techniques. However, experimentally measuring all the necessary electronic interaction cross-sections for every relevant material is an arduous task, so it is necessary having predictive models, sufficiently accurate yet easily implementable. In this work we present a model, based on the dielectric formalism, to provide reliable ionisation and excitation cross-sections for electron-impact on complex biomolecular media, considering their condensed-phase nature. We account for the indistinguishability and exchange between the primary beam and excited electrons, for the molecular electronic structure effects in the electron binding, as well as for low-energy corrections to the first Born approximation. The resulting approach yields total ionisation cross-sections, energy distributions of secondary electrons, and total electronic excitation cross-sections for condensed-phase biomaterials, once the electronic excitation spectrum is known, either from experiments or from a predictive model. The results of this methodology are compared with the available experimental data in water and DNA/RNA molecular building blocks, showing a very good agreement and a great predictive power in a wide range of electron incident energies, from the large values characteristic of electron beams down to excitation threshold. The proposed model constitutes a very useful procedure for computing the electronic interaction cross-sections for arbitrary biological materials in a wide range of electron incident energies. ; This work has received funding from the European Union's Horizon 2020 Research and Innovation programme under the Marie Sklodowska-Curie grant agreement no. 840752, from the Spanish Ministerio de Economía y Competitividad and the European Regional Development Fund (Project no. PGC2018-096788-B-I00), from the Fundación Séneca (Project no. 19907/GERM/15) and from the Conselleria d'Educació, Investigació, Cultura i Esport de la Generalitat Valenciana (Project no. AICO/2019/070). PdV acknowledges further financial support provided by the Spanish Ministerio de Economía y Competitividad by means of a Juan de la Cierva postdoctoral fellowship (FJCI-2017-32233).

We present a simple method for obtaining reliable angular and energy distributions of electrons ejected from arbitrary condensed biomaterials by proton impact. Relying on a suitable description of the electronic excitation spectrum and a physically motivated relation between the ion and electron scattering angles, it yields cross sections in rather good agreement with experimental data in a broad range of ejection angles and energies, by only using as input the target composition and density. The versatility and simplicity of the method, which can be also extended to other charged particles, make it especially suited for obtaining ionization data for any complex biomaterial present in realistic cellular environments. ; The authors recognize the financial support from the Spanish Ministerio de Economía y Competitividad and the European Regional Development Fund (Project No. FIS2010–17225). PdV acknowledges financial support from the European Union's FP7-People Program (Marie Curie Actions) within the Initial Training Network No. 608163 "ARGENT". Support from the European COST Action MP1002 NanoIBCT is gratefully acknowledged.

We present a manageable approach to include, within the context of optical-data models of the dielectric response function, exchange and correlation (XC) effects in inelastic electron scattering, thus, going beyond the standard random-phase approximation (RPA). The many-body local-field correction in its static limit, G(q) , is employed to incorporate XC effects to all orders in q at both the level of "screening" and the level of "scattering" by computing the so-called test-charge–test-charge (t–t), electron–test-charge (e–t), and electron–electron (e–e) dielectric functions. Some of the most used analytic approximations for G(q) are examined, ranging from the early Hubbard-like expressions to more recent parameterized formulations that satisfy some of the known asymptotic limits. The effect of the different G(q) models upon the inelastic scattering of low-medium energy electrons in condensed matter is examined using solid (amorphous) carbon as an example. It is shown that when XC corrections at all levels are considered, a net reduction of the inelastic scattering cross section by up to 20%–30% from the corresponding RPA value is obtained. Interestingly, a screened Hubbard approximation to G(q) reproduces (to a few %) the results of more accurate representations. Based on the present results, the controversial high-q asymptotic behaviour of G(q) is inconsequential to inelastic electron scattering in the examined energy range. ; The work of D.E. and I.K. has been financially supported by the European Union FP7 (Marie Curie Actions) program "RADDEL" (REA Grant Agreement No. 290023). The work of R.G.M. and I.A. has been supported by the European Regional Development Fund and the Spanish Ministerio de Economía y Competitividad (Project No. FIS2010-17225).

The use of proton beams in several modern technologies to probe or modify the properties of materials, such as proton beam lithography or ion beam cancer therapy, requires us to accurately know the extent to which the energy lost by the swift projectiles in the medium is redistributed radially around their tracks, since this determines several endpoints, such as the resolution of imaging or manufacturing techniques, or even the biological outcomes of radiotherapy. In this paper, the radial distribution of the energy deposited around swift-proton tracks in polymethylmethacrylate (PMMA) by the transport of secondary electrons is obtained by means of a detailed Monte Carlo simulation. The initial energy and angular distributions of the secondary electrons generated by proton impact, as well as the electronic cross sections for the ejection of these electrons, are reliably calculated in the framework of the dielectric formalism, where a realistic electronic excitation spectrum of PMMA is accounted for. The cascade of all secondary electrons generated in PMMA is simulated taking into account the main interactions that occur between these electrons and the condensed phase target. After analyzing the influence that several angular distributions of the electrons generated by the proton beam have on the resulting radial profiles of deposited energy, we conclude that the widely used Rudd and Kim formula should be replaced by the simpler isotropic angular distribution, which leads to radial energy distributions comparable to the ones obtained from more realistic angular distributions. By studying the dependence of the radial dose on the proton energy we recommend lower proton energies than previously published for reducing proximity effects around a proton track. The obtained results are of relevance for assessing the resolution limits of proton beam based imaging and manufacturing techniques. ; Financial support was provided by the Spanish Ministerio de Economía y Competitividad and the European Regional Development Fund (Project No. FIS2014-58849-P), as well as by the Fundación Séneca (Project No. 19907/GERM/15). P.d.V. acknowledges financial support from the European Union's FP7 People: Marie-Curie Actions program within the Initial Training Network No. 608163 "ARGENT", Advanced Radiotherapy, Generated by Exploiting Nanoprocesses and Technologies.

We have studied the radial dependence of the energy deposition of the secondary electron generated by swift proton beams incident with energies T = 50 keV–5 MeV on poly(methylmethacrylate) (PMMA). Two different approaches have been used to model the electronic excitation spectrum of PMMA through its energy loss function (ELF), namely the extended-Drude ELF and the Mermin ELF. The singly differential cross section and the total cross section for ionization, as well as the average energy of the generated secondary electrons, show sizeable differences at T ⩽ 0.1 MeV when evaluated with these two ELF models. In order to know the radial distribution around the proton track of the energy deposited by the cascade of secondary electrons, a simulation has been performed that follows the motion of the electrons through the target taking into account both the inelastic interactions (via electronic ionizations and excitations as well as electron-phonon and electron trapping by polaron creation) and the elastic interactions. The radial distribution of the energy deposited by the secondary electrons around the proton track shows notable differences between the simulations performed with the extended-Drude ELF or the Mermin ELF, being the former more spread out (and, therefore, less peaked) than the latter. The highest intensity and sharpness of the deposited energy distributions takes place for proton beams incident with T ~ 0.1–1 MeV. We have also studied the influence in the radial distribution of deposited energy of using a full energy distribution of secondary electrons generated by proton impact or using a single value (namely, the average value of the distribution); our results show that differences between both simulations become important for proton energies larger than ~0.1 MeV. The results presented in this work have potential applications in materials science, as well as hadron therapy (due to the use of PMMA as a tissue phantom) in order to properly consider the generation of electrons by proton beams and their subsequent transport and energy deposition through the target in nanometric scales. ; This work has been supported by the Spanish Ministerio de Economía y Competitividad (Project FIS2014-58849-P) and by the Istituto Nazionale di Fisica Nucleare (INFN) through the Supercalcolo agreement with FBK. PdV acknowledges financial support from the European Union's FP7-People Program (Marie Curie Actions) within the Initial Training Network No. 608163 "ARGENT".

The energy dissipation pattern of low-energy electron beams (0.3–30 keV) in multi-walled carbon nanotube (MWCNT) materials is studied by Monte Carlo simulation taking into account secondary-electron cascade generation. A quasi first-principles discrete-energy-loss model deduced from a dielectric response function description of electronic excitations in MWCNTs is employed whereby both single-particle and plasmon excitations are included in a unified and self-consistent manner. Our simulations provide practical analytical functions for computing depth-dose curves and charged-carrier generation volumes in MWCNT materials under low-energy electron beam irradiation. ; Financial support for D.E., I.K., and K.K. by the European Union FP7 ANTICARB (HEALTH-F2-2008-201587) and for R.G.M. and I.A. by the Spanish Ministerio de Ciencia e Innovación (project FIS2010-17225).

The effect of bulk and surface excitations to inelastic scattering in low-energy electron beam irradiation of multi-walled carbon nanotubes (MWNTs) is studied using the dielectric formalism. Calculations are based on a semiempirical dielectric response function for MWCNTs determined by means of a many-pole plasmon model with parameters adjusted to available experimental spectroscopic data under theoretical sum-rule constrains. Finite-size effects are considered in the context of electron gas theory via a boundary correction term in the plasmon dispersion relations, thus, allowing a more realistic extrapolation of the electronic excitation spectrum over the whole energy-momentum plane. Energy-loss differential and total inelastic scattering cross sections as a function of electron energy and distance from the surface, valid over the energy range ∼50–30,000 eV, are calculated with the individual contribution of bulk and surface excitations separated and analyzed for the case of normally incident and escaping electrons. The sensitivity of the results to the various approximations for the spatial dispersion of the electronic excitations is quantified. Surface excitations are shown to have a strong influence upon the shape and intensity of the energy-loss differential cross section in the near surface region whereas the general notion of a spatially invariant inelastic mean free path inside the material is found to be of good approximation. ; Financial support of D.E., I.K., and K.K. by the European Union FP7 ANTICARB (Grant No. HEALTH-F2-2008-201587) and of I.A. and RGM by the Spanish Ministerio de Ciencia e Innovación (Project FIS2010-17225).

We use a simulation code, based on Molecular Dynamics and Monte Carlo, to investigate the depth-dose profile and lateral radial spreading of swift proton beams in liquid water. The stochastic nature of the projectile-target interaction is accounted for in a detailed manner by including in a consistent way fluctuations in both the energy loss due to inelastic collisions and the angular deflection from multiple elastic scattering. Depth-variation of the projectile charge-state as it slows down into the target, due to electron capture and loss processes, is also considered. By selectively switching on/off these stochastic processes in the simulation, we evaluate the contribution of each one of them to the Bragg curve. Our simulations show that the inclusion of the energy-loss straggling sizeably affects the width of the Bragg peak, whose position is mainly determined by the stopping power. The lateral spread of the beam as a function of the depth in the target is also examined. ; This work has been financially supported by the the Spanish Ministerio de Ciencia e Innovación (Project FIS2010-17225) and the European Union FP7 ANTICARB (HEALTH-F2-2008-201587). PdV thanks the Conselleria d'Educació, Formació i Ocupació de la Generalitat Valenciana for its support under the VALi+d program. We acknowledge support provided by the COST Action MP 1002, Nanoscale Insights into Ion Beam Cancer Therapy.

Energetic carbon ions are promising projectiles used for cancer radiotherapy. A thorough knowledge of how the energy of these ions is deposited in biological media (mainly composed of liquid water) is required. This can be attained by means of detailed computer simulations, both macroscopically (relevant for appropriately delivering the dose) and at the nanoscale (important for determining the inflicted radiobiological damage). The energy lost per unit path length (i.e., the so-called stopping power) of carbon ions is here theoretically calculated within the dielectric formalism from the excitation spectrum of liquid water obtained from two complementary approaches (one relying on an optical-data model and the other exclusively on ab initio calculations). In addition, the energy carried at the nanometre scale by the generated secondary electrons around the ion's path is simulated by means of a detailed Monte Carlo code. For this purpose, we use the ion and electron cross sections calculated by means of state-of-the art approaches suited to take into account the condensed-phase nature of the liquid water target. As a result of these simulations, the radial dose around the ion's path is obtained, as well as the distributions of clustered events in nanometric volumes similar to the dimensions of DNA convolutions, contributing to the biological damage for carbon ions in a wide energy range, covering from the plateau to the maximum of the Bragg peak. ; This research was funded by European Union's Horizon 2020 Research and Innovation programme grant number 840752, by the Spanish Ministerio de Economía y Competitividad grant number PGC2018-096788-B-I00 funded by MCIN/AEI/10.13039/501100011033 and by FEDER "A way to make Europe", and by the Fundación Séneca grant number 19907/GERM/15. The APC was funded by the Spanish Ministerio de Economía y Competitividad and the European Regional Development Fund grant number PGC2018-096788-B-I00.

The effective use of swift ion beams in cancer treatment (known as hadrontherapy) as well as appropriate protection in manned space missions rely on the accurate understanding of the energy delivery to cells that damages their genetic information. The key ingredient characterizing the response of a medium to the perturbation induced by charged particles is its electronic excitation spectrum. By using linear-response time-dependent density functional theory, we obtained the energy and momentum transfer excitation spectrum (the energy-loss function, ELF) of liquid water (the main constituent of biological tissues), which was in excellent agreement with experimental data. The inelastic scattering cross sections obtained from this ELF, together with the elastic scattering cross sections derived by considering the condensed phase nature of the medium, were used to perform accurate Monte Carlo simulations of the energy deposited by swift carbon ions in liquid water and carried away by the generated secondary electrons, producing inelastic events such as ionization, excitation, and dissociative electron attachment (DEA). The latter are strongly correlated with cellular death, which is scored in sensitive volumes with the size of two DNA convolutions. The sizes of the clusters of damaging events for a wide range of carbon-ion energies, from those relevant to hadrontherapy up to those for cosmic radiation, predict with unprecedented statistical accuracy the nature and relative magnitude of the main inelastic processes contributing to radiation biodamage, confirming that ionization accounts for the vast majority of complex damage. DEA, typically regarded as a very relevant biodamage mechanism, surprisingly plays a minor role in carbon-ion induced clusters of harmful events. ; This project received funding from the European Union's Horizon 2020 Research and Innovation programme under the Marie Sklodowska-Curie grant agreement no. 840752. P.d.V. received additional support by the Spanish Ministerio de Ciencia e Innovación by means of a Juan de la Cierva fellowship (no. FJCI-2017-32233). This work was also supported by the Spanish Ministerio de Ciencia e Innovación and the European Regional Development Fund (Project PGC2018-096788−B−I00); the Fundación Séneca−Agencia de Ciencia y Tecnología de la Región de Murcia (Project 19907/GERM/15); and the Conselleria d'Educació, Investigació, Cultura i Esport de la Generalitat Valenciana (Project AICO/2019/070).

Nanomaterials made of cerium oxides CeO2 and Ce2O3 have a broad range of applications, from catalysts in automotive, industrial or energy operations to promising materials to enhance hadrontherapy effectiveness in oncological treatments. To elucidate the physico-chemical mechanisms involved in these processes, it is of paramount importance to know the electronic excitation spectra of these oxides, which are obtained here through high-accuracy linear-response time-dependent density functional theory calculations. In particular, the macroscopic dielectric response functions [small epsilon, Greek, macron] of both bulk CeO2 and Ce2O3 are derived, which compare remarkably well with the available experimental data. These results stress the importance of appropriately accounting for local field effects to model the dielectric function of metal oxides. Furthermore, we reckon the energy loss functions Im(−1/[small epsilon, Greek, macron]) of the materials, including the accurate evaluation of the momentum transfer dispersion from first-principles calculations. In this respect, by using Mermin-type parametrization we are able to model the contribution of different electronic excitations to the dielectric loss function. Finally, from the knowledge of the electron inelastic mean free path, together with the elastic mean free path provided by the relativistic Mott theory, we carry out statistical Monte Carlo (MC) electron transport simulations to reproduce the major features of the reported experimental reflection electron energy loss (REEL) spectra of cerium oxides. The good agreement with REEL experimental data strongly supports our approach based on MC modelling, whose main inputs were obtained using ab initio calculated electronic excitation spectra in a broad range of momentum and energy transfers. ; A. P. acknowledges Fondazione Caritro and DICAM (University of Trento) for the financial support under the CARITRO project High-Z ceramic oxide nanosystems for mediated proton cancer therapy. This project has received funding from the European Union's Horizon 2020 Research and Innovation programme under the Marie Sklodowska-Curie grant agreement no. 840752 NanoEnHanCement of P. d. V., as well as from the Spanish Ministerio de Economía y Competitividad and the European Regional Development Fund (Project no. PGC2018-096788-B-I00), from the Fundación Séneca (Project no. 19907/GERM/15) and from the Conselleria d'Educació, Investigació, Cultura i Esport de la Generalitat Valenciana (Project no. AICO/2019/070).