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We performed the experimental and theoretical study of the heating and damaging of ruthenium thin films induced by femtosecond laser irradiation. Results of an optical pump-probe thermoreflectance experiment with rotating sample allowing to significantly reduce heat accumulation in irradiated spot are presented. We show the evolution of surface morphology from growth of a heat-induced oxide layer at low and intermediate laser fluences to cracking and grooving at high fluences. Theoretical analysis of pump-probe signal allows us to relate behavior of hot electrons in ruthenium to the Fermi smearing mechanism. The analysis of heating is performed with the two-temperature modeling and molecular dynamics simulation, results of which demonstrate that the calculated melting threshold is higher than experimental damage threshold. We attribute it to heat-induced surface stresses leading to cracking which accumulates to more severe damage morphology. Our results provide an upper limit for operational conditions for ruthenium optics and also direct to further studies of the Fermi smearing mechanism in other transition metals., 23 pages, 11 figures, 1 table, 7 data files in supplementary material

Materials 15(15), 5193 (2022). doi:10.3390/ma15155193, Ultrafast laser irradiation of metals can often be described theoretically with the two-temperature model. The energy exchange between the excited electronic system and the atomic one is governed by the electron–phonon coupling parameter. The electron–phonon coupling depends on both, the electronic and the atomic temperature. We analyze the effect of the dependence of the electron–phonon coupling parameter on the atomic temperature in ruthenium, gold, and palladium. It is shown that the dependence on the atomic temperature induces nonlinear behavior, in which a higher initial electronic temperature leads to faster electron–phonon equilibration. Analysis of the experimental measurements of the transient thermoreflectance of the laser-irradiated ruthenium thin film allows us to draw some, albeit indirect, conclusions about the limits of the applicability of the different coupling parametrizations., Published by MDPI, Basel

We present a concurrent Monte Carlo (MC) - molecular dynamics (MD) approach to modeling of matter response to excitation of its electronic system. The two methods are combined on-the-fly at each time step in one code, TREKIS-4. The MC model describes arrival of irradiation, which in the current implementation can consist of a photon, an electron, or a fast ion. It also traces induced cascades of excitation of secondary particles, electrons and holes, and their energy exchange with atoms due to scattering. The excited atomic system is simulated with an MD model. We propose a simple and efficient way to account for nonthermal effects in the electron-atom energy transfer in covalent materials via conversion of potential energy of the ensemble into the kinetic energy of atoms, which can be straightforwardly implemented into an MD simulation. Such a combined MC-MD approach enables us time-resolved tracing of the excitation kinetics of both, electronic and atomic systems, and their simultaneous response to a deposited dose. As a proof-of-principle example, we show that proposed method describes atomic dynamics after X-ray irradiation in a good agreement with tight-binding MD, with much more affordable computational demands. The new model also allows us to gain insights into behavior of the atomic system during the energy deposition from a nonequilibrium electronic system excited by an ion impact.

Spatially encoded measurements of transient optical transmissivity became a standard tool for temporal diagnostics of free-electron-laser (FEL) pulses, as well as for the arrival time measurements in X-ray pump and optical probe experiments. The modern experimental techniques can measure changes in optical coefficients with a temporal resolution better than 10 fs. This, in an ideal case, would imply a similar resolution for the temporal pulse properties and the arrival time jitter between the FEL and optical laser pulses. However, carrier transport within the material and out of its surface, as well as carrier recombination may, in addition, significantly decrease the number of carriers. This would strongly affect the transient optical properties, making the diagnostic measurement inaccurate. Below we analyze in detail the effects of those processes on the optical properties of XUV and soft X-ray irradiated Si$${_3}$$ 3 N$$_4$$ 4 , on sub-picosecond timescales. Si$${_3}$$ 3 N$$_4$$ 4 is a wide-gap insulating material widely used for FEL pulse diagnostics. Theoretical predictions are compared with the published results of two experiments at FERMI and LCLS facilities, and with our own recent measurement. The comparison indicates that three body Auger recombination strongly affects the optical response of Si$${_3}$$ 3 N$$_4$$ 4 after its collisional ionization stops. By deconvolving the contribution of Auger recombination, in future applications one could regain a high temporal resolution for the reconstruction of the FEL pulse properties measured with a Si$${_3}$$ 3 N$$_4$$ 4 -based diagnostics tool.

Laser irradiation of metals is widely used in research and applications. In this work, we study how the material geometry affects electron–phonon coupling in nano-sized gold samples: an ultrathin layer, nano-rod, and two types of gold nanoparticles (cubic and octahedral). We use the combined tight-binding molecular dynamics Boltzmann collision integral method implemented within XTANT-3 code to evaluate the coupling parameter in irradiation targets at high electronic temperatures (up to Te~20,000 K). Our results show that the electron–phonon coupling in all objects with the same fcc atomic structure (bulk, layer, rod, cubic and octahedral nanoparticles) is nearly identical at electronic temperatures above Te~7000 K, independently of geometry and dimensionality. At low electronic temperatures, reducing dimensionality reduces the coupling parameter. Additionally, nano-objects under ultrafast energy deposition experience nonthermal damage due to expansion caused by electronic pressure, in contrast to bulk metal. Nano-object ultrafast expansion leads to the ablation/emission of atoms and disorders the inside of the remaining parts. These nonthermal atomic expansion and melting are significantly faster than electron–phonon coupling, forming a dominant effect in nano-sized gold.

It is known that covalently bonded materials undergo nonthermal structure transformations upon ultrafast excitation of an electronic system, whereas metals exhibit phonon hardening in the bulk. Here we study how ionic bonds react to electronic excitation. Density-functional molecular dynamics predicts that ionic crystals may melt nonthermally, however, into an electronically insulating state, in contrast to covalent materials. We demonstrate that the band gap behavior during nonthermal transitions depends on a bonding type: it is harder to collapse the band gap in more ionic compounds, which is illustrated by transformations in Y2O3 vs. NaCl, LiF and KBr.

This review summarizes our results on effects of different stages of the formation kinetics of swift heavy ion (SHI) tracks on final structural changes. The developed multiscale approach describes in detail the formation of individual tracks and inter-track interaction in various amorphizable (Y3Al5O12, Mg2SiO4) and non-amorphizable (Al2O3, MgO) dielectrics. A comparison between the modeling and high-resolution transmission electron microscopy analysis of SHI irradiated samples allows to validate the developed model and to investigate links between the basic properties of the materials and features of the kinetics of structural transformations of the targets. We outline an influence and importance of each successive stage of excitation and relaxation on final observable structure modifications within tracks, starting from the SHI induced electronic excitation, electrons and holes transport, energy exchange with the target lattice, transient excitation and relaxation of the atomic system, and ultimate damage formation.

The thermal decomposition on silicon carbide (SiC) is one of the most used growth techniques for fabrication of epitaxial graphene. However, it significantly diminishes graphene’s otherwise exceptional carrier mobility. Reduction of the substrate influence is therefore essential for keeping conductivity at high levels. Here we present a novel technique where a sample with epitaxial graphene grown on SiC was exposed to intense 21.2 nm radiation. A sub-nanosecond pulse at low fluence in an interval 0.4–0.7 J/cm2 was used to break covalent sp3 bonds between the SiC substrate and buffer (the first graphene layer) which remains, except for release of its intrinsic strain, almost unaffected. A detailed analysis of the irradiated area examined by several microscopic and spectroscopic methods such as white-light interferometry and micro-Raman spectroscopy shows a clear evidence of a graphene layer detached from the substrate. Higher fluences induce damage to SiC substrate which expands due to the amorphization process. Damage thresholds were obtained by an advanced method of ablative imprints and compared with those calculated by the hybrid code XTANT.

Materials exposed to ultrashort intense x-ray irradiation experience various damaging conditions depending on the irradiation temperature. A pre-heated target exposed to intense x-rays plays a crucial role in numerous physical-technical systems, ranging from the heavily and repeatedly radiation-loaded optics at x-ray free-electron laser facilities to the inner-most wall of prospective inertial fusion reactors. We study the temperature dependence of damage thresholds in different classes of materials theoretically: an insulator (diamond), a semiconductor (silicon), a metal (tungsten), and an organic polymer (PMMA). The numerical techniques used here enable us to trace the evolution of both the electronic state and the atomic dynamics of the materials. It includes damage mechanisms such as thermal damage, induced by an increased irradiation temperature due to energy transfer from x-ray-excited electrons, and nonthermal phase transitions, induced by rapid interatomic potential changes due to the excitation of electrons. We demonstrate that in the pre-heated materials, the thermal damage threshold tends to stay the same or lowers with the increase of the irradiation temperature, whereas nonthermal damage thresholds may be lowered or raised, depending on the particular material and specifics of the damage kinetics.

The modern means of controlled irradiation by femtosecond lasers or swift heavy ion beams can transiently produce such energy densities in samples that reach collective electronic excitation levels of the warm dense matter state where the potential energy of interaction of the particles is comparable to their kinetic energies (temperatures of a few eV). Such massive electronic excitation severely alters the interatomic potentials, producing unusual nonequilibrium states of matter and different chemistry. We employ density functional theory and tight binding molecular dynamics formalisms to study the response of bulk water to ultrafast excitation of its electrons. After a certain threshold electronic temperature, the water becomes electronically conducting via the collapse of its band gap. At high doses, it is accompanied by nonthermal acceleration of ions to a temperature of a few thousand Kelvins within sub-100 fs timescales. We identify the interplay of this nonthermal mechanism with the electron-ion coupling, enhancing the electron-to-ions energy transfer. Various chemically active fragments are formed from the disintegrating water molecules, depending on the deposited dose., to be submitted

We study the behavior of poly(methyl methacrylate) (PMMA) exposed to femtosecond pulses of extreme ultraviolet and X-ray laser radiation in the single-shot damage regime. The employed microscopic simulation traces induced electron cascades, the thermal energy exchange of electrons with atoms, nonthermal modification of the interatomic potential, and a triggered atomic response. We identify that the nonthermal hydrogen decoupling triggers ultrafast fragmentation of PMMA strains at the absorbed threshold dose of ~0.07 eV/atom. At higher doses, more hydrogen atoms detach from their parental molecules, which, at the dose of ~0.5 eV/atom, leads to a complete separation of hydrogens from carbon and oxygen atoms and fragmentation of MMA molecules. At the dose of ~0.7 eV/atom, the band gap completely collapses indicating that a metallic liquid is formed with complete atomic disorder. An estimated single-shot ablation threshold and a crater depth as functions of fluence agree well with the experimental data collected.

Formation of swift heavy ion tracks requires extremely fast energy transfer between excited electrons and a lattice. However, electron-phonon energy exchange is too slow, as known from laser-irradiation experiments and calculations. We resolve this contradiction noticing that electron-phonon coupling is not the sole mechanism of energy exchange between electrons and ions: heating of electrons also alters potential energy surface of atoms, accelerating them and increasing their kinetic energy.

Polyethylene (PE) irradiated with femtosecond extreme ultraviolet or X-ray laser pulses in a single-shot damage regime is studied theoretically. The employed microscopic simulation tool XTANT-3 traces nonequilibrium electron kinetics, energy exchange between electrons and atoms, nonthermal modification of interatomic potential, and the induced atomic response. It is found that the nonthermal detachment of hydrogen atoms in bulk PE starts at the threshold deposited dose of ∼0.05 eV per atom. With an increase in the dose, more hydrogen atoms detach from the carbon backbone. At a dose of ∼0.3 eV per atom, hydrogen behaves like a liquid flowing around carbon chains. It is accompanied by the appearance of defect energy levels within the band gap. At a dose of ∼0.5 eV per atom, carbon chains actively bend and cross-link. In the range of doses from ∼0.5 eV per atom to ∼0.9 eV per atom, the electronic excitation induces formation of new carbon structures embedded in the hydrogen liquid, such as benzene-like rings. The band gap collapses at such doses, merging the valence and the conduction bands. Finally, at doses above ∼0.9 eV per atom, the carbon subsystem also melts into liquid. All of these damage mechanisms are mainly nonthermal, triggered by promotion of electrons from the valence into the conduction band of PE. At high doses, however, thermal electron-ion coupling is extremely fast causing equilibration of the electronic and the ionic temperatures within a hundred femtoseconds.

Laser and particle beams 37(2), 235 - 241 (2019). doi:10.1017/S0263034619000326, Modern free-electron lasers (FEL) operating in XUV (extreme ultraviolet) or X-ray range allow an access to novel research areas. An example is the ultrafast ionization of a solid by an intense femtosecond FEL pulse in XUV which consequently leads to a change of the complex index of refraction on an ultrashort timescale. The photoionization and subsequent impact ionization resulting in electronic and atomic dynamics are modeled with our hybrid code XTANT(X-ray thermal and non-thermal transitions) and a Monte Carlo code XCASCADE(X-ray-induced electron cascades). The simulations predict the temporal kinetics of FEL-induced electron cascades and thus yield temporally and spatially resolved information on the induced changes of the optical properties. In a series of experiments at FERMI and LCLS, single shot measurements with spatio-temporal encoding of the ionization process have been performed by a correlation of the FEL pump pulse with an optical femtosecond probe pulse. An excellent agreement between the experiment and the simulation has been found. We also show that such kind of experiments forms the basis for pulse duration and arrival time jitter monitoring as currently under development for XUV-FELs, Published by Cambridge Univ. Press, Cambridge

Response of dielectric crystals: MgO, Al2O3 and Y3Al5O12 (YAG) to irradiation with 167 MeV Xe ions decelerating in the electronic stopping regime is studied. Comprehensive simulations demonstrated that despite similar ion energy losses and the initial excitation kinetics of the electronic systems and lattices, significant differences occur among final structures of ion tracks in these materials, supported by experiments. No ion tracks appeared in MgO, whereas discontinuous distorted crystalline tracks of ~2 nm in diameter were observed in Al2O3 and continuous amorphous tracks were detected in YAG. These track structures in Al2O3 and YAG were confirmed by high resolution TEM data. The simulations enabled us to identify recrystallization as the dominant mechanism governing formation of detected tracks in these oxides. We analyzed effects of the viscosity in molten state, lattice structure and difference in the kinetics of metallic and oxygen sublattices at the crystallization surface on damage recovery in tracks.

A swift heavy ion leaves a damaged trail (SHI track) while penetrating through a solid. The radius of the track depends on the ion energy loss and velocity, and thereby on its penetration depth. Applying developed Monte Carlo code TREKIS and molecular dynamics approach we describe the damage distribution along the trajectory of an SHI (Xe and U) in olivine. This enables us to obtain the dependencies of the track radius and structure on the ion energy and its energy losses, as well as to identify the track formation thresholds in forsterite (Mg2SiO4) for fast and slow ions. It is found that the position of the maximal damage produced by an ion in a solid does not coincide with the Bragg peak of its electronic stopping. Loop-like dependence of the track radius on the electronic energy loss is identified.

In this report, we analyse X-ray induced damage of B 4 C-coated bilayer materials under various irradiation geometries, following the conditions of our experiment performed at the free-electron-laser facility SACLA. We start with the discussion of structural damage in solids and damage threshold doses for the experimental system components: B 4 C, SiC, Mo and Si. Later, we analyze the irradiation of the experimentally tested coated bilayer systems under two different incidence conditions of a linearly polarized X-ray pulse: (i) grazing incidence, and (ii) normal incidence, in order to compare quantitatively the effect of the pulse incidence on the radiation tolerance of both systems. For that purpose, we propose a simple theoretical model utilizing properties of hard X-ray propagation and absorption in irradiated materials and of the following electron transport. With this model, we overcome the bottleneck problem of large spatial scales, inaccessible for any existing first-principle-based simulation tools due to their computational limitations for large systems. Predictions for damage thresholds obtained with the model agree well with the available experimental data. In particular, they confirm that two coatings tested: 15 nm B 4 C/20 nm Mo on silicon wafer and 15 nm B 4 C/50 nm SiC on silicon wafer can sustain X-ray irradiation at the fluences up to ~10 μJ/μm 2, when exposed to linearly polarized 10 keV X-ray pulse at a grazing incidence angle of 3 mrad. Below we present the corresponding theoretical analysis. Potential applications of our approach for design and radiation tolerance tests of multilayer components within X-ray free-electron-laser optics are indicated.

Highly energetic ions traversing a two-dimensional material such as graphene produce strong electronic excitations. Electrons excited to energy states above the work function can give rise to secondary electron emission, reducing the amount of energy that remains the graphene after the ion impact. Electrons can either be emitted (kinetic energy transfer) or captured by the passing ion (potential energy transfer). To elucidate this behavior that is absent in three-dimensional materials, we simulate the electron dynamics in graphene during the first femtoseconds after ion impact. We employ two conceptually different computational methods: a Monte Carlo (MC) based one, where electrons are treated as classical particles, and time-dependent density functional theory (TDDFT), where electrons are described quantum-mechanically. We observe that the linear dependence of electron emission on deposited energy, emerging from MC simulations, becomes sublinear and closer to the TDDFT values when the electrostatic interactions of emitted electrons with graphene are taken into account via complementary particle-in-cell simulations. Our TDDFT simulations show that the probability for electron capture decreases rapidly with increasing ion velocity, whereas secondary electron emission dominates in the high velocity regime. We estimate that these processes reduce the amount of energy deposited in the graphene layer by 15\,\% to 65\,\%, depending on the ion and its velocity. This finding clearly shows that electron emission must be taken into consideration when modelling damage production in two-dimensional materials under ion irradiation., 14 pages, 8 figures

Physical review letters 126(11), 117403 (1-6) (2021). doi:10.1103/PhysRevLett.126.117403, Ultrafast changes of charge density distribution in diamond after irradiation with an intense x-ray pulse (photon energy, 7.8 keV; pulse duration, 6 fs; intensity, 3×10$^{19}$ W/cm$^2$) have been visualized with the x-ray pump–x-ray probe technique. The measurement reveals that covalent bonds in diamond are broken and the electron distribution around each atom becomes almost isotropic within ∼5 fs after the intensity maximum of the x-ray pump pulse. The 15 fs time delay observed between the bond breaking and atomic disordering indicates nonisothermality of electron and lattice subsystems on this timescale. From these observations and simulation results, we interpret that the x-ray-induced change of the interatomic potential drives the ultrafast atomic disordering underway to the following nonthermal melting., Published by APS, College Park, Md.

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.

We recently developed an approach for calculation of the electron-phonon (electron-ion in a more general case) coupling in materials based on tight-binding molecular dynamics simulations. In the present work we utilize this approach to study partial contributions of inter- and intraband electron scattering events into total electron-phonon coupling in Al, Au, Cu elemental metals and in AlCu alloy. We demonstrate that the interband scattering plays an important role in electron-ion energy exchange process in Al and AlCu, whereas intraband $d-d$ transitions are dominant in Au and Cu. Moreover, inter- and intraband transitions exhibit qualitatively different dependencies on the electron temperature. Our findings should be taken into account for interpretation of experimental results on electron-phonon coupling parameter., Comment: To be submitted

The European physical journal / D 75, 224 (2021). doi:10.1140/epjd/s10053-021-00235-z, In this paper, we report on the Boltzmann kinetic equation approach adapted for simulations of warm dense matter created by irradiation of bulk gold with intense ultrashort X-ray pulses. X-rays can excite inner-shell electrons, which triggers creation of deep-lying core holes. Their relaxation, especially in heavier elements such as gold (atomic number Z=79) takes complicated pathways, involving collisional processes, and leading through a large number of active configurations. This number can be so high that solving a set of evolution equations for each configuration becomes computationally inefficient, and another modeling approach should be used instead. Here, we use the earlier introduced ���predominant excitation and relaxation path��� approach. It still uses true atomic configurations but limits their number by restricting material relaxation to a selected set of predominant pathways for material excitation and relaxation. With that, we obtain time-resolved predictions for excitation and relaxation in X-ray irradiated bulk of gold, including the respective change of gold optical properties. We compare the predictions with the available data from high-energy-density experiments. Their good agreement indicates ability of the Boltzmann kinetic equation approach to describe warm dense matter created from high-Z materials after their irradiation with X rays, which can be validated in future experiments., Published by Springer, Heidelberg

This book collects the lectures presented in the first COST TUMIEE Training School held in Greece in 2019, supplemented with specific applications that illustrate how the multi-scale approach is implemented in specific cases of interest. The book is intended both as a reference in the field and as a textbook for people becoming interested or entering the field. The first part focuses on experimental methods, the second on theoretical approaches, and the third on cases of interest.

Atomic heating in a solid takes place after an impact of a swift heavy ion within a time of electronic cooling there, i.e., ∼100 fs. This implies an extremely fast electron–ion energy exchange (“electron–phonon coupling”) necessary for the production of detected ion tracks. In contrast, laser irradiation experiments and calculations show too slow electron–phonon energy exchange to cause structural changes detected in swift heavy ion tracks in solids. We demonstrate that this contradiction can be resolved by taking into account that electron–phonon coupling is not the sole mechanism of energy exchange between electrons and ions in condensed matter. Excitation of the electronic system alters the potential energy surface of atoms, causing them to accelerate and increase their kinetic energy at ultrashort times.

Physical review applied 14(3), 034057 (2020). doi:10.1103/PhysRevApplied.14.034057, Solids irradiated by energetic photons can be eroded in two modes, depending on the radiation intensity. High average, low-peak power sources, e.g., synchrotron radiation and high-order harmonics, induce desorption of the material at a low etch rate. In contrast, high-peak-power radiation from extreme ultraviolet and x-ray lasers usually causes a massive removal of the material even by a single shot. In this contribution, an effective material erosion is reported in PMMA exposed to multiple accumulated pulses generated by the free-electron x-ray-laser Linac Coherent Light Source (LCLS, tuned at a photon energy of 830 eV in this study, operated in Menlo Park at Stanford, CA, USA) at a fluence below the single-pulse ablation threshold. The effect is caused by polymer-chain scissions initiated by single photons carrying enough energy to break the C$—$C bounds. High efficiency of the erosion is supposed to occur due to a correlation of the single-photon effects. The subthreshold damage exhibits a nonlinear dose dependence resulting from a competition between chain scissions and cross-linking processes. The cross-linking is proven by Raman spectroscopy of the irradiated polymer. Two theoretical models of the x-ray free-electron-laser-induced erosion are suggested, which provide an excellent agreement with the experimental results., Published by American Physical Society, College Park, Md. [u.a.]

It is well known that sufficiently thick metals irradiated with ultrafast laser pulses exhibit phonon hardening, in contrast to ultrafast nonthermal melting in covalently bonded materials. It is still an open question how finite size metals react to irradiation. We show theoretically that generally metals, under high electronic excitation, undergo nonthermal phase transitions if material expansion is allowed (e.g. in finite samples). The nonthermal phase transitions are induced via an increase of the electronic pressure which leads to metal expansion. This, in turn, destabilizes the lattice triggering a phase transition without a thermal electron-ion coupling mechanism involved. We find that hexagonal close-packed metals exhibit a diffusionless transition into a cubic phase, whereas metals with a cubic lattice melt. In contrast to covalent solids, nonthermal phase transitions in metals are not ultrafast, predicative on the lattice expansion.

It is predicted theoretically that various oxides (Al2O3, MgO, SiO2 and TiO2) under ultrafast excitation of the electronic system exhibit nonthermal phase transitions. In the bulk, Al2O3 transiently forms a superionic phase via nonthermal phase transition, MgO and SiO2 disorder, TiO2 experiences solid-solid phase transition while thermal effects lead to melting. In the finite-size samples and near-surface regions, MgO undergoes solid-solid phase transition at lower doses than those required for atomic disorder. All studied oxides but TiO2, if allowed to expand, exhibit a lower damage threshold, whereas in TiO2 expansion releases the stress and prevents solid-solid phase transition thereby increasing the damage threshold up to the melting one. The results suggest that a nonthermal phase transition is a general response of oxides to sufficiently high ultrafast electronic excitation. A comparison with nonadiabatic simulations demonstrates that Born-Oppenheimer approximation systematically overestimates damage thresholds, and in some cases misses a phase transition entirely.

Electron-phonon coupling, being one of the most important parameters governing the material evolution after ultrafast energy deposition, yet remains the most unexplored one. In this work, we applied the dynamical coupling approach to calculate the nonadiabatic electron-ion energy exchange in nonequilibrium solids with the electronic temperature high above the atomic one. It was implemented into the tight-binding molecular dynamics code, and used to study electron-phonon coupling in various elemental metals. The developed approach is a universal scheme applicable to electronic temperatures up to a few electron-Volts, and to arbitrary atomic configuration and dynamics. We demonstrate that the calculated electron-ion (electron-phonon) coupling parameter agrees well with the available experimental data in high-electronic-temperature regime, validating the model. The following materials are studied here - fcc metals: Al, Ca, Ni, Cu, Sr, Y, Zr, Rh, Pd, Ag, Ir, Pt, Au, Pb; hcp metals: Mg, Sc, Ti, Co, Zn, Tc, Ru, Cd, Hf, Re, Os; bcc metals: V, Cr, Fe, Nb, Mo, Ba, Ta, W; diamond cubic lattice metals: Sn; specific cases of Ga, In, Mn, Te and Se; and additionally semimetal graphite and semiconductors Si and Ge. For many materials, we provide the first and so far the only estimation of the electron-phonon coupling at elevated electron temperatures, which can be used in various models simulating ultrafast energy deposition in matter. We also discuss the dependence of the coupling parameter on the atomic mass, temperature and density., To be submitted for publication

A standard Fricke dosimeter was used to measure the absorbed dose via the oxidation yields of Fe3+ ions in an aqueous environment induced by soft X rays within the "water window" spectral range. We also exploited the property of a neutral solution containing terephthalic acid as a tool for selective detection of OH radicals. Both dosimetric systems were irradiated using the experimental pulsed laser-plasma soft X-ray source as well as conventional 1.25-MeV gamma rays. Radiation chemical yields of Fe3+ ions and OH radicals were determined to be (5.13 ± 0.94) × 10-1 µmol·J-1 (4.95 ± 0.91 100eV-1) and (2.33 ± 0.35) × 10-2 µmol·J-1 (0.23 ± 0.03 100eV-1), respectively. Measurements were supported by Monte Carlo simulations to estimate the linear energy transfer of the water window radiation. The simulation results are in good agreement with expected linear energy transfer of ions inducing the same Fe3+ ion and OH radical radiation chemical yield.

Diamond irradiated with an intense femtosecond X-ray free-electron laser (XFEL) pulse is studied theoretically. The modeling is performed with the help of recently developed hybrid approach XTANT. The model includes processes of initial X-ray photon absorption resulting in photoelectron excitation, secondary electron cascades, Auger decays of K-shell holes, energy exchange between electron and atoms (electron-phonon coupling), nonthermal evolution of the atomic potential energy surface, atomic dynamics, and phase transitions. The results show that time-resolved graphitization of diamond irradiated with 24-keV photon energy pulses, as planned to be delivered at the European XFEL, takes slightly longer in comparison to the case of soft-X-ray irradiation.

Data in Brief 28, 104980 - (2020). doi:10.1016/j.dib.2019.104980, Interaction of ultrashort laser pulses with materials can bring the latter to highly non-equilibrium states, where the electronic temperature strongly differs from the ionic one. The properties of such excited material can be considerably different from those in a hot, but equilibrium state. The reliable modeling of laser-irradiated target requires careful analysis of its properties in both regimes. This paper reports a procedure which provides the equations of state of ruthenium using density functional theory calculations. The obtained data are fitted with analytical functions. The constructed equations of state are applicable in the one- and two-temperature regimes and in a wide range of densities, temperatures and pressures. The electron thermal conductivity and electron-phonon coupling factor are also calculated. The obtained analytical expressions can be used in two-temperature hydrodynamics modeling of Ru targets pumped by ultrashort laser pulses. The data is related to the research article “Similarity in ruthenium damage induced by photons with different energies: From visible light to hard X-rays” [1]., Published by Elsevier, Amsterdam [u.a.]

This review concentrates on the specific properties and characteristics of damage structures generated with high-energy ions in the electronic energy loss regime. Irradiation experiments with so-called swift heavy ions (SHI) find applications in many different fields, with examples presented in ion-track nanotechnology, radiation hardness analysis of functional materials, and laboratory tests of cosmic radiation. The basics of the SHI-solid interaction are described with special attention to processes in the electronic subsystem. The broad spectrum of damage phenomena is exemplified for various materials and material classes, along with a description of typical characterization techniques. The review also presents state-of-the-art modeling efforts that try to account for the complexity of the coupled processes of the electronic and atomic subsystems. Finally, the relevance of SHI phenomena for effects induced by fission fragments in nuclear fuels and how this knowledge can be applied to better estimate damage risks in nuclear materials is discussed.

We performed combined experimental and computational research on damage processes in ruthenium thin films induced by femtosecond lasers with various photon energies. We present an experiment with an optical laser at normal incidence conditions and compare it with previously reported experiments at grazing incidence conditions with XUV and hard X-ray photons, covering a large range of photon energies. Analysis of ablation craters in Ru shows very similar crater morphology and depth of about 10–20 nm for all considered irradiation conditions. Simulations of light-matter interactions are performed with our combined Monte Carlo and two-temperature hydrodynamics approach. The simulation results show that the primal cause of eventual ablation is Auger decay of core-shell holes created after absorption of XUV and hard X-ray photons in the vicinity of ruthenium surface. They lead to the creation of many low-energy electrons which consequently release the absorbed energy near the surface, resembling the optical irradiation case. Similar absorbed energy distributions in the top part of ruthenium induce a similar thermo-mechanical response and, therefore, similar ablation process. Our results suggest that such mechanism is universal in a wide range of photon energies at grazing incidence conditions, when the photon absorption depth is smaller than the photoelectrons range.

Applied surface science 528, 146952 - (2020). doi:10.1016/j.apsusc.2020.146952, The dynamics of a thin ruthenium film irradiated by femtosecond extreme UV laser pulses is studied with a hybrid computational approach, which includes Monte Carlo, two-temperature hydrodynamics and molecular dynamics models. This approach is capable of accurate simulations of all stages of material evolution induced by extreme UV or X-ray photons: from nonequilibrium electron kinetics till complete lattice relaxation. We found that fast energy deposition in a subsurface layer leads to a two-level ablation: the top thin layer is ablated as a gas–liquid mixture due to expansion of overheated material at near and above critical conditions, whereas a thicker liquid layer below is ablated via a cavitation process. The latter occurs due to a thermo-mechanically induced tensile pressure wave. The liquid ablating layer exhibits unstable behaviour and disintegrates into droplets soon after detachment from the rest of the target. Our simulations reveal basic processes leading to formation of specific surface morphologies outside and inside the damage craters. The calculated ablation threshold, crater depth and morphological features are in quantitative agreement with the experimental data, which justifies the applicability of our hybrid model to study laser-induced material damage., Published by Elsevier, Amsterdam

This paper investigates an effect of a target temperature on lattice excitation by the relaxing electron ensemble in a swift heavy ion track. A new version of the Monte-Carlo code TREKIS is used for this purpose. Cross sections implemented in TREKIS are constructed within the dynamic structure factor/complex dielectric function (DSF-CDF) formalism. This enables us to take into account unusual pathways of collective responses of the electronic and ionic subsystems to their femtosecond excitations in SHI tracks. The paper demonstrates that the temperature dependent fundamental asymmetry of the lattice DSF manifests itself in different kinetics of energy exchange between the electronic and atomic systems of alumina in SHI tracks at different temperatures (80 K vs. 300 K).

A structure in overlapping swift heavy ion track regions in Al2O3 is studied using numerical and experimental techniques. A swift heavy ion impact is modeled with Monte-Carlo code TREKIS, describing excitation of the electronic and atomic systems, and with classical molecular dynamics tracing subsequent lattice relaxation. This combined approach is applied to simulate (predict) structure and phase transformations in tracks of heavy ions. The results of simulations are validated by high resolution transmission electron microscopy of irradiated crystals. The data obtained for 167 MeV Xe and 700 MeV Bi ion impacts in Al2O3 demonstrate that relaxation of the excess lattice energy results in formation of a cylinder-like discontinuous disordered region of about 1.8 nm and 3.4 nm in diameter, respectively. The simulation of the overlap of Xe ion tracks revealed the recovery of the pre-existing tracks, whereas higher electronic energy losses around the Bi ion trajectory lead to both damage recovery and formation of a damaged region depending on the distance between tracks, which are in a good agreement with experimental observations.

Journal of the Optical Society of America / B 35(10), B43 - B53 (2018). doi:10.1364/JOSAB.35.000B43, We perform a computational study of damage formation in extreme ultraviolet (XUV)-irradiated ruthenium thin films by means of combining the Monte Carlo approach with the two-temperature model. The model predicts that the damage formation is most affected by ultrafast heating of the lattice by hot electrons, and is not very sensitive to the initial stage of the material excitation. Numerical parameters of the model were analyzed, as well as different approximations for the thermal parameters, showing the importance of the temperature dependence of the electron thermal conductivity and the electron–phonon coupling factor. Our analysis reveals that the details of photoabsorption and ultrafast non-equilibrium electron kinetics play only a minor role in the XUV irradiation regime., Published by OSA, Washington, DC