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.
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 …
We have investigated the deterioration of field effect transistors based on twodimensional materials due to irradiation with swift heavy ions. Devices were prepared with exfoliated single layers of MoS2 and graphene, respectively. They were characterized before and after irradiation with 1.14 GeV U228+2 ions using three different fluences. By electrical characterization, atomic force microscopy and Raman spectroscopy we show that the irradiation leads to significant changes of structural and electrical properties. At the highest fluence of 4 x 102^11 ions/cm^2, the MoS2 transistor is destroyed…
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…
There is considerable controversy about swift heavy ion (SHI) irradiation induced displacive phase transitions in thermally insulating oxides. We present here unambiguous evidence for tetragonal to monoclinic and rhombohedral to monoclinic phase transitions in BaTiO3 under swift heavy ion irradiation (120MeV 108Ag+9 ions) using in-situ x-ray powder diffraction (XRPD) studies. The anomalous splitting/broadening of 111/222pc, 200pc and 220pc pseudocubic peaks for fluences greater than 3*1012 ions/cm2 reveal structural changes before amorphization at higher fluences. Lebail analysis of XRPD profi…
The single crystal of tris(thiourea)zinc sulphate (Zn[CS(NH2)2]3SO4) was irradiated by 150 MeV Au9+ swift heavy ions and analyzed in comparison with pure crystal for crystalline perfection and optical properties. The Fourier transform infrared and x-ray powder diffraction inferred that swift ions lead the disordering and breaking of molecular bonds in lattice without formation of new structural phases. High resolution X-ray diffraction (HRXRD) revealed the abundance of point defects, and formation of mosaics and low angle grain boundaries in the irradiated region of crystal. The swift ion irra…
In this paper, we have presented the impact of swift heavy ion beam irradiation on the structural, microstructural, electrical and magnetic properties of $Sn_{0.9}Mn_{0.1}O_{2}$ thin films. The structural and electrical results have been interpreted by using properties of native or point defects, whereas the magnetic and morphological variations have been explained in terms of conductivity of material. Efforts have been made to summarize the properties of all possible charged and neutral point defects ($V_{Sn}^{4-}$, $Sn_{i}^{4+}$, $V_{O}^{0}$, $O_{i}^{2-}$, $Sn_{O}^{4+}$, $O_{Sn}^{2-}$, $H_{O…
Ion track formation, amorphisation, and the formation of porosity in crystalline GaSb induced by 185 MeV $^{197}$Au swift heavy ion irradiation is investigated as a function of fluence and irradiation angle relative to the surface normal. RBS/C and SAXS reveal an ion track radius between 3 nm and 5 nm. The observed pore morphology and saturation swelling of GaSb films shows a strong irradiation angle dependence. Raman spectroscopy and scanning electron microscopy show that the ion tracks act as a source of strain in the material leading to macroscopic plastic flow at high fluences and off norm…
The high energy density of electronic excitations due to the impact of swift heavy ions can induce structural modifications in materials. We present a X-ray diffractometer called ALIX, which has been set up at the low-energy IRRSUD beamline of the GANIL facility, to allow the study of structural modification kinetics as a function of the ion fluence. The X-ray setup has been modified and optimized to enable irradiation by swift heavy ions simultaneously to X-ray pattern recording. We present the capability of ALIX to perform simultaneous irradiation - diffraction by using energy discrimination…
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 variou…
Track radii Re induced by swift heavy ions are studied. The experimental track data are analyzed in Gd2Ti2O7 pyrochlore in the range Se=6-54 keV/nm (Se - electronic stopping power) including irradiations by low and high velocity ions. The Analytical Thermal Spike Model (ATSM) is applied whose main features are reviewed. The track data of Gd2Ti2O7 exhibit scaling features which mean simple quantitative relationships with track sizes of other insulators controlled only by a single materials parameter (MP), the melting temperature Tm. The Re2-Se track evolution curve is described in the whole ran…
Atomistic Mechanisms of Temperature-Dependent Ion Track Formation in Gallium Nitride under Swift Heavy Ion Irradiation
School of Nuclear Science and Technology, Xi’an Jiaotong University（西安交通大学核科学与技术学院）；Academy of Chips Technology, China Electronics Technology Group Corporation（中国电子科技集团公司芯片技术研究院）；National Key Laboratory of Integrated Circuits and Microsystems（集成电路与微系统国家重点实验室）
The electrical characteristics and microstructures of $β$-Ga$_2$O$_3$ Schottky barrier diode (SBD) devices irradiated with swift heavy ions (2096 MeV Ta ions) have been studied. It was found that $β$-Ga$_2$O$_3$ SBD devices showed the reliability degradation after irradiation, including turn-on voltage Von, on-resistance Ron, ideality factor n and the reverse leakage current density Jr. In addition, the carrier concentration of the drift layer was decreased significantly and the calculated carrier removal rates were 5*106 - 1.3*107 cm-1. Latent tracks induced by swift heavy ions were observed …
We exposed nitrogen-implanted diamonds to beams of swift uranium and gold ions (~1 GeV) and find that these irradiations lead directly to the formation of nitrogen vacancy (NV) centers, without thermal annealing. We compare the photoluminescence intensities of swift heavy ion activated NV- centers to those formed by irradiation with low-energy electrons and by thermal annealing. NV- yields from irradiations with swift heavy ions are 0.1 of yields from low energy electrons and 0.02 of yields from thermal annealing. We discuss possible mechanisms of NV-center formation by swift heavy ions such a…
Epitaxial thin films of La0.7Ba0.3MnO3 manganite, deposited using Chemical Solution Deposition technique, were irradiated by 200 MeV Ag+15 ions with a maximum ion dose up to 1x10^12 ions/cm2. Temperature- and magnetic field-dependent resistivity measurements on all the films (before and after irradiation) reveal a sustained decrease in resistivity with increasing ion dose. A maximum dose of 1x10^12 ions/cm2 suppresses resistivity by factors of 3 and 10, at 330 K [insulator-metal (I-M) transition] and at 10 K, respectively. On the other hand, with increasing ion dose, the magnetoresistance (MR)…
The irradiation of SrTiO$_3$ single crystals with swift heavy ions leads to modifications of the surface. The details of the morphology of these modifications depends strongly on the angle of incidence and can be characterized by atomic force microscopy. At glancing angles, discontinuous chains of nanosized hillocks appear on the surface. The latent track radius can be determined from the variation of the length of the chains with the angle of incidence. This radius is material specific and allows the calculation of the electron-phonon-coupling constant for SrTiO$_3$. We show that a theoretica…
This paper presents experimental data and analysis of the structural damage caused by swift-heavy ion irradiation of single-crystal diamond. The patterned buried structural damage is shown to generate, via swelling, a mirror-pattern on the sample surface, which remains largely damage-free. While extensive results are available for light ion implantations, this effect is reported here for the first time in the heavy ion regime, where a completely different range of input parameters (in terms of ion species, energy, stopping power, etc.) is available for customized irradiation. The chosen ion sp…
Creating mixed-phase states in cadmium sulfide by swift heavy ion irradiation
Institute of Physics, Czech Academy of Sciences（捷克科学院物理研究所）；Higher Institute of Technologies and Applied Sciences, University of Havana（哈瓦那大学高等技术与应用科学学院）；Institute of Plasma Physics, Czech Academy of Sciences（捷克科学院等离子体物理研究所）
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 rec…
Yttria stabilized Zirconia (YSZ) pellets with different crystallite sizes were irradiated with 80 MeV Ag$^{6+}$ ions at room temperature and 1000 K to understand the role of crystallite size/material microstructure and irradiation temperature on the radiation tolerance against high electronic energy loss (S$_e$). X-ray diffraction and Raman spectroscopy measurements reveal that, irrespective of the irradiation temperature, the nano-crystalline samples suffered more damage as compared to the bulk-like sample. A reduction in the irradiation damage i.e. improvement in the radiation tolerance, was…
Muscovite mica sheets with a thickness of 25 μm were irradiated by various kinds of swift heavy ions (Sn, Xe and Bi) in HIRFL. The fluences ranged from 1$\times$10^{10} ions/cm^2 to 8$\times$10^{11} ions/cm^2. The electronic energy loss (dE/dx)_e was increased from 14.7 keV/nm to 31.2 keV/nm. The band gap and Urbach energy of pristine and irradiated mica were analyzed by ultraviolet- visible spectroscopy. Periodic fringes in long wave length of the absorption spectra caused by interference phenomenon, were disturbed as the (dE/dx)_e increased. It was suggested that the chemical bonds between T…
Thermal spike model (TSM) is presently a widely accepted mechanism of swift heavy ion (SHI) - matter interaction. It provides explanation to various SHI induced effects including mixing across interfaces. The model involves electron-phonon (e-p) coupling to predict the evolution of lattice temperature with time. SHI mixing is considered to be a result of diffusion in transient molten state thus achieved. In this work, we assess this conception primarily via tuning the e-p coupling strength by taking a series Pd$_{1-x}$Ni$_x$ of a completely solid soluble binary, and then observing 100 MeV Au i…
Highly conducting $SnO_{2}$ thin films were prepared by chemical spray pyrolysis technique. One set of as-deposited films were annealed in air for 2 h at 850$^{o}$C. These as-deposited and annealed films were irradiated using $Au^{9+}$ ions with energy of 120 MeV at different fluences ranging from $1\times10^{11}$ to $3\times10^{13}$ $ions/cm^{2}$. Electrical measurement shows that as-deposited $SnO_{2}$ films are in conducting state with n = $3.164 \times 10^{20}$ $cm^{-3}$ and annealed $SnO_{2}$ films are in insulating state. The amorphized latent tracks are created only above a certain thre…
Unveiling Nanoscale Surface Damage Dynamics in Swift Heavy Ion Irradiated Gallium Nitride
School of Nuclear Science and Technology, Xi’an Jiaotong University（西安交通大学核科学与技术学院）；Academy of Chips Technology, China Electronics Technology Group Corporation（中国电子科技集团公司芯片技术研究院）；National Key Laboratory of Integrated Circuits and Microsystems（集成电路与微系统国家重点实验室）；National Key Laboratory for High Energy Pulsed Power（高能量脉冲功率国家重点实验室）
Controversy over nature and existence of the velocity effect [G. Szenes, Phys. Rev. B 87, 056101 (2013)], [M. Toulemonde et al., Phys. Rev. B 87, 056102 (2013)] reignited after new experimental data on swift heavy ion tracks in CaF2 was reported recently [M. Toulemonde et al., Phys. Rev. B 85, 054112 (2012)]. Here we show that results of the analysis in ref. [G. Szenes, Phys. Rev. B 87, 056101 (2013)] should be interpreted differently within analytical thermal spike model. We also propose explanation for apparently missing velocity effect.
The irradiation with fast ions with kinetic energies of > 10 MeV leads to the deposition of a high amount of energy along their trajectory (up to several ten keV/nm). The energy is mainly transferred to the electronic subsystem and induces different secondary processes of excitations which result in significant material modifications. A new setup to study these ion induced effects on surfaces will be described in this paper. The setup combines a variable irradiation chamber with different techniques of surface characterizations like scanning probe microscopy, time-of-flight secondary ion and n…
A combined experimental and computational study of the recrystallization process induced by swift heavy ions in pre-damaged silicon carbide crystals was reported in a recent paper by Debelle et al. [Phys. Rev. B 86, 100102(R) (2012)]. In this study, the authors tried to mimic by means of molecular dynamic simulations both damage production induced by low energy ion irradiation in SiC and the recrystallization effect generated by subsequent swift heavy ion irradiation. Here we show that the simulations performed by the authors are far from being realistic and cannot reproduce, even qualitativel…
Modification induced by 110 MeV Ni ion irradiated thin film samples of C60 on Si and quartz substrates were studied at various fluences. The pristine and irradiated samples were investigated using Raman spectroscopy, electrical conductivity and optical absorption spectroscopy. The Raman data and band gap measurements indicate that swift ions at low fluences result in formations that involve multiple molecular units like dimer or polymer. High fluence irradiation resulted in sub-molecular formations and amorphous semiconducting carbon, indicating overall damage of the fullerene molecules. These…
Anions of the molecules ZnO, O2 and atomic Zn and O constitute mass spectra of the species sputtered from pellets of molecular solid of ZnO under Cs+ irradiation. Their normalized yields are independent of energy of the irradiating Cs+. Collision cascades cannot explain the simultaneous sputtering of atoms and molecules. We propose that the origin of the molecular sublimation, dissociation and subsequent emission is the result of localized thermal spikes induced by individual Cs+ ions. The fractal dimension of binary collision cascades of atomic recoils in the irradiated ZnO solid increases wi…
By combining classical molecular dynamics simulations and density functional theory total energy calculations, we study the possibility of doping graphene with B/N atoms using low-energy ion irradiation. Our simulations show that the optimum irradiation energy is 50 eV with substitution probabilities of 55% for N and 40% for B. We further estimate probabilities for different defect configurations to appear under B/N ion irradiation. We analyze the processes responsible for defect production and report an effective swift chemical sputtering mechanism for N irradiation at low energies (~125 eV) …
Molecular dynamics simulations have been used to obtain the three-dimensional distribution of interfacial mixing and cascade defects in Ti/Pt multilayer system due to single 1 keV $Ar^+$ impacts at grazing angle of incidence. The Ti/Pt system was chosen because of its relatively high heat of mixing in the binary alloy and therefore a suitable candidate for testing the effect of heat of mixing on ion-beam mixing. However, the calculated mixing profile is not sensitive to the heat of mixing. Therefore the thermal spike model of mixing is not fully supported under these irradiation conditions. In…
We show that the work function of exfoliated single layer graphene can be modified by irradiation with swift (E_{kin}=92 MeV) heavy ions under glancing angles of incidence. Upon ion impact individual surface tracks are created in graphene on SiC. Due to the very localized energy deposition characteristic for ions in this energy range, the surface area which is structurally altered is limited to ~ 0.01 mum^2 per track. Kelvin probe force microscopy reveals that those surface tracks consist of electronically modified material and that a few tracks suffice to shift the surface potential of the wh…
Two exponents, $δ$, for size distribution of $n$-atom clusters, $Y(n)\sim n^{-δ}$, have been found in Au clusters sputtered from embedded Au nanoparticles under swift heavy ion irradiation. For small clusters, below 12.5 nm in size, $δ$ has been found to be 3/2, which can be rationalized as occurring from a steady state aggregation process with size independent aggregation. For larger clusters, a $δ$ value of 7/2 is suggested, which might come from a dynamical transition to another steady state where aggregation and evaporation rates are size dependent. In the present case, the observed decay …
The ability to manufacture tailored graphene nanostructures is a key factor to fully exploit its enormous technological potential. We have investigated nanostructures created in graphene by swift heavy ion induced folding. For our experiments, single layers of graphene exfoliated on various substrates and freestanding graphene have been irradiated and analyzed by atomic force and high resolution transmission electron microscopy as well as Raman spectroscopy. We show that the dense electronic excitation in the wake of the traversing ion yields characteristic nanostructures each of which may be …
We report depth-resolved photoluminescence measurements of nitrogen-vacancy (NV$^-$) centers formed along the tracks of swift heavy ions (SHIs) in type Ib synthetic single crystal diamonds that had been doped with 100 ppm nitrogen during crystal growth. Analysis of the spectra shows that NV$^-$ centers are formed preferentially within regions where electronic stopping processes dominate and not at the end of the ion range where elastic collisions lead to formation of vacancies and defects. Thermal annealing further increases NV yields after irradiation with SHIs preferentially in regions with …
Anisotropic Core-Shell Swift Heavy Ion Tracks in beta-Ga2O3
School of Nuclear Science and Technology, Xi’an Jiaotong University（西安交通大学核科学与技术学院）；Materials Science and Environmental Engineering Unit, Tampere University（坦佩雷大学材料科学与环境工程单元）；Institute of Modern Physics, Chinese Academy of Sciences（中国科学院近代物理研究所）；Department of Nuclear Physics, China Institute of Atomic Energy（中国原子能科学研究院核物理系）；Department of Physics and Helsinki Institute of Physics, University of Helsinki（赫尔辛基大学物理系与赫尔辛基物理研究所）；The Hong Kong Microelectronics Research and（香港微电子研究）
There is ongoing debate regarding the mechanism of swift heavy ion track formation in CaF2. The objective of this study is to shed light on this important topic using a range of complimentary experimental techniques. Evidence of the threshold for ion track formation being below 3 keV/nm is provided by both transmission electron microscopy and Rutherford backscattering spectroscopy in the channeling mode which has direct consequences for the validity of models describing the response of CaF2 to swift heavy ion irradiation. Advances in the TEM and RBS/c analyses presented here pave the way for b…
In recent experiments the irradiation of insulators of perovskite type with swift heavy ions under glancing incidence has been shown to provide a unique means to generate periodically arranged nanodots at the surface. The physical origin of these patterns has been suggested to stem from a highly anisotropic electron density distribution within the bulk. In order to show the relevance of the electron density distribution of the target we present a model calculation for the system Xe$^{+23}$ $\to$ SrTiO$_{3}$ that is known to produce the aforementioned surface modifications. On the basis of the …
Molecular dynamics simulations have been used to study the driving force of ion irradiation induced interfacial mixing in metal bilayers in which the relative mass of the constituents is considerable. We find no apparent effect of chemical forces, such as heat of mixing or cohesive energy up to 8 keV ion energy, although a considerable number of liquid and high energy particles (hot atoms) persist up to even 20 ps during the thermal spike. This result is in direct conflict with the widely accepted theory of thermal spike mixing (chemical interdiffusion model). The supersaturation of vacancies …
We have used electron paramagnetic resonance to study the thermal annealing of colour centres induced in cubic yttria-stabilized zirconia by swift electron and heavy ion-irradiations. Single crystals were irradiated with 1 or 2-MeV electrons, and 200-MeV 127I, or 200-MeV 197Au ions. Electron and ion beams produce the same colour centres: namely i) an F+-like centre, ii) the so-called T-centre (Zr3+ in a trigonal oxygen local environment), and iii) a hole center. Isochronal annealing was performed up to 973 K. Isothermal annealing was performed at various temperatures on samples irradiated with…
The shape of metal nanoparticles embedded in dielectric matrices influences the optical properties of the composite material. Swift heavy ion irradiation can induce a controllable shape transformation in gold and other metals embedded in amorphous silicon dioxide, where the particles elongate along the direction of the ion beam. The details of this transformation are not fully understood, but it is presumably related to nanometer-scale phase transitions induced by individual ion impacts. The phenomenon has been reproduced using atomistic simulations, although the time scale limitations and the…
It is shown that the average diameter of tracks produced by swift heavy ions in metals is determined by the size of elementary resonator. The last is introduced in the theory of thermal radiation accounting for the stimulated radiation processes. Due to the inverse density gradient, radiation produced by electronic excitations is locked in the region of track which is formed. Similar effects are applied to the process of nanocavity formation in semiconductors during ion irradiation.
We developed a new sub-nanosecond time-resolved instrument to study the dynamics of UV-visible luminescence under high stopping power heavy ion irradiation. We applied our instrument, called SPORT, on a fast plastic scintillator (BC-400) irradiated with 27-MeV Ar ions having high mean electronic stopping power of 2.6 MeV/μm. As a consequence of increasing permanent radiation damages with increasing ion fluence, our investigations reveal a degradation of scintillation intensity together with, thanks to the time-resolved measurement, a decrease in the decay constant of the scintillator. This com…
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.
Enhancing the Plasmonic Hotspot Density via Structural Engineering of Multi-layered MoO3-Ag-Au Systems Under Extreme Electronic Excitation Conditions for Ultra-Sensitive SERS Applications
The formation of nano-hillocks on CaF2 crystal surfaces by individual ion impact has been studied using medium energy (3 and 5 MeV) highly charged ions (Xe19+ to Xe30+) as well as swift (kinetic energies between 12 and 58 MeV) heavy ions. For very slow highly charged ions the appearance of hillocks is known to be linked to a threshold in potential energy while for swift heavy ions a minimum electronic energy loss is necessary. With our results we bridge the gap between these two extreme cases and demonstrate, that with increasing energy deposition via electronic energy loss the potential energ…
The aim of this work is to investigate feasibility of the ion beam analysis techniques for monitoring swift heavy ion track formation. First, use of the in situ Rutherford backscattering spectroscopy in channeling mode to observe damage build-up in quartz SiO2 after MeV heavy ion irradiation is demonstrated. Second, new results of the in situ grazing incidence time-of-flight elastic recoil detection analysis used for monitoring the surface elemental composition during ion tracks formation in various materials are presented. Ion tracks were found on SrTiO3, quartz SiO2, a-SiO2 and muscovite mic…
A swift chemical route to synthesize Co-doped SnO$_2$ nanopowders is described. Pure and highly stable Sn$_{1-x}$Co$_x$O$_{2-δ}$ (0 $\le$ x $\le$ 0.15) crystalline nanoparticles were synthesized, with mean grain sizes < 5 nm and the dopant element homogeneously distributed in substitutional sites of the SnO$_2$ matrix. The UV-visible diffuse reflectance spectra of the Sn$_{1-x}$Co$_x$O$_{2-δ}$ samples reveal red shifts, the optical bandgap energies decreasing with increasing Co concentration. The Urbach energies of the samples were calculated and correlated with their bandgap energies. The pho…
