Electron Irradiation Damage Research Articles

Amorphization of a proposed sorbent of strontium, brushite, CaHPO4•2H2O, studied by X-ray diffraction and Raman spectroscopy

We present a systematic study of the transformation of brushite (dicalcium phosphate dihydrate, CaHPO4•2H2O) under irradiation of electrons of well-defined energy (2.5 MeV) and flux as a function of the irradiation dose. Contrarily to model hydroxides such as portlandite and brucite, which are very resistant to electron radiation damage, the studied brushite decomposes quite easily, even for very low irradiation doses. Irradiated brushite samples were characterized using X-ray diffraction (XRD) and Raman spectroscopy to get complementary information about changes in atomic structure and chemical composition respectively under irradiation. XRD showed that irradiation causes a very limited dilatation of unit cell of crystalline brushite, which becomes progressively amorphous with increasing radiation dose. Raman spectroscopy complemented XRD results and confirmed that the transformation of brushite to the amorphous phase was not abrupt, but rather progressive. Raman spectroscopy allowed for the identification of the amorphous phase as a calcium pyrophosphate. Both techniques showed that the amorphization of brushite was not fully complete at the maximum dose used, 5.5 GGy (4 C). Interestingly, monetite phase, (CaHPO4 dicalcium phosphate), was not detected at any step of the transformation as it is the case when brushite is thermally decomposed. This study reveals the high sensitivity to electron radiation of both hydrogen bonds and protonated phosphate units in brushite, thus facilitating the transformation into pyrophosphate. The damage of brushite by energetic electrons is to be carefully considered for applications related to the use of brushite as ion-exchanger in the decontamination of effluents polluted with strontium-90, an efficient beta ray emitter.

Atomically resolved tomographic reconstruction of nanoparticles from single projection: Influence of amorphous carbon support

Nanoparticles have a wide range of applications due to their unique geometry and arrangement of atoms. For a precise structure-property correlation, information regarding atomically resolved 3D structures of nanoparticles is utmost beneficial. Though modern aberration-corrected transmission electron microscopes can resolve atoms with the sub-angstrom resolution, an atomic-scale 3D reconstruction of a nanoparticle using Scanning Transmission Electron Microscopy (STEM) based tomographic method faces hurdles due to high electron irradiation damage and “missing-wedge”. Instead, inline 3D holography based tomographic reconstructions from single projection registered at low electron doses is more suitable for defining atomic positions at nanostructures. Nanoparticles are generally supported on amorphous carbon film for Transmission Electron Microscopy (TEM) experiments. However, neglecting the influence of carbon film on the tomographic reconstruction of the nanoparticle may lead to ambiguity. To address this issue, the effect of amorphous carbon support was quantitatively studied using simulations and experiments and it was revealed that increasing thickness and/or density of carbon support increases distortion in tomograms.

Real-time ab initio simulation of inelastic electron scattering using the exact, density functional, and alternative approaches.

To investigate inelastic electron scattering, which is ubiquitous in various fields of study, we carry out ab initio study of the real-time dynamics of a one-dimensional electron wave packet scattered by a hydrogen atom using different methods: the exact solution, the solution provided by time-dependent density functional theory (TDDFT), and the solutions given by alternative approaches. This research not only sheds light on inelastic scattering processes but also verifies the capability of TDDFT in describing inelastic electron scattering. We revisit the adiabatic local-density approximation (ALDA) in describing the excitation of the target during the scattering process along with a self-interaction correction and spin-polarized calculations. Our results reveal that the ALDA severely underestimates the energy transferred in the regime of low incident energy particularly for a spin-singlet system. After demonstrating alternative approaches, we propose a hybrid ab initio method to deal with the kinetic correlation alongside TDDFT. This hybrid method would facilitate first-principles studies of systems in which the correlation of a few electrons among many others is of interest.

Quantifying Elastic and Inelastic Electron Irradiation Damage in Transmission Electron Microscopy of 2D Materials

Quantifying Elastic and Inelastic Electron Irradiation Damage in Transmission Electron Microscopy of 2D Materials

Simulating the radial dose distribution for charged particles in water medium by a semi-empirical model: An analytical approach

A computational semi-empirical model based on electronic radiation damage to medium has been presented to simulate the radial dose distribution. An analytical approach was used to calculate the deposited energy in water per unit mass within a cylindrical shell of unit length around the ion path at a radial distance between r and r + dr, the so-called radial dose distribution, RDD. Detail steps were given and the final radial dose integration over the electron range between Rmin and Rmax was solved numerically using the Mid-Point Method. A validation for the present model was presented by integrating the RDD over all possible radial distances, r to yield the tabulated LET of the ion. The validation was presented for a range of proton ions of different energies. The RDD for heavy charged particles of proton, alpha, Carbon and Oxygen ions of different energies in liquid water were obtained. Good agreement between the present model and experimental, theoretical, and Monte Carlo (Geant4-DNA) data were obtained for all ions under investigations.

Electronic Excitations and Radiation Damage in Macromolecular Crystallography

Macromolecular crystallography at cryogenic temperatures has so far provided the majority of the experimental evidence that underpins the determination of the atomic structures of proteins and other biomolecular assemblies by means of single crystal X-ray diffraction experiments. One of the core limitations of the current methods is that crystal samples degrade as they are subject to X-rays, and two broad groups of effects are observed: global and specific damage. While the currently successful approach is to operate outside the range where global damage is observed, specific damage is not well understood and may lead to poor interpretation of the chemistry and biology of the system under study. In this work, we present a phenomenological model in which specific damage is understood as the result of a single process, the steady excitation of crystal electrons caused by X-ray absorption, which acts as a trigger for the bulk effects that manifest themselves in the form of global damage and obscure the interpretation of chemical information from XFEL and synchrotron structural research.

Atomic and nanoscale imaging of a cellulose nanofiber and Pd nanoparticles composite using lower-voltage high-resolution TEM.

We have examined the advanced application of transmission electron microscopy (TEM) for the structural characterization of a composite of cellulose nanofiber (CNF) and palladium (Pd) nanoparticles. In the present study, we focused on electron-irradiation damage and optimization of high-resolution TEM imaging of the composite. The investigation indicates that the CNF breaks even under low-electron-dose conditions at an acceleration voltage of 200 kV. We then applied lower-voltage TEM at 60 kV using a spherical aberration corrector and a monochromator, in order to reduce electron-irradiation damage and improve the spatial resolution. The TEM observation achieved high-resolution imaging and revealed the existence of small Pd nanoparticles, around 2 nm in diameter, supported on the CNF. It is considered that the use of a monochromator in combination with spherical aberration correction contributed to the atomic and nanoscale imaging of the composite, owing to the improvement of the information limit under a lower-acceleration voltage.

Methodology trends on gamma and electron radiation damage simulation studies in solids under high fluency irradiation environments

The present work deals with the numerical simulation of gamma and electron radiation damage processes under high brightness and radiation particle fluency on regard to two new radiation induced atom displacement processes, which concern with both, the Monte Carlo Method based numerical simulation of the occurrence of atom displacement process as a result of gamma and electron interactions and transport in a solid matrix and the atom displacement threshold energies calculated by Molecular Dynamic methodologies. The two new radiation damage processes here considered in the framework of high brightness and particle fluency irradiation conditions are: 1) The radiation induced atom displacement processes due to a single primary knockout atom excitation in a defective target crystal matrix increasing its defect concentrations (vacancies, interstitials and Frenkel pairs) as a result of a severe and progressive material radiation damage and 2) The occurrence of atom displacements related to multiple primary knockout atom excitations for the same or different atomic species in an perfect target crystal matrix due to subsequent electron elastic atomic scattering in the same atomic neighborhood during a crystal lattice relaxation time. In the present work a review numeral simulation attempts of these two new radiation damage processes are presented, starting from the former developed algorithms and codes for Monte Carlo simulation of atom displacements induced by electron and gamma in

Detecting dynamic responses of materials and devices under an alternating electric potential by phase-locked transmission electron microscopy

An apparatus is developed for transmission electron microscopy (TEM) to acquire image and spectral data, such as TEM images, electron holograms, and electron energy loss spectra, synchronized with the measurement of the dynamic response of a specimen under an applied alternating current (AC) electric potential (voltage, denoted VAC). From a VAC of frequency f, a shutter pulse signal is generated to open and close a pre-specimen shutter in a base TEM apparatus. A pulse is generated per VAC cycle from the targeted phase Φ to Φ +∆Φ with phase width ∆Φ (∆Φ <2π). ∆Φ corresponds to the temporal pulse width τ (τ < 1/f) of an electron beam; i.e., ∆Φ =2πfτ. Because of the high sensitivity of the TEM camera used in this study, the images and spectra that are acquired at the same target phase are integrated by means of stroboscopic illumination to obtain the final phase-locked images and spectra with sufficiently small S/N ratio. Phase-locked (strobe) images and/or spectra are obtained for model specimens of polycrystalline aluminum and an all-solid-state lithium ion battery (LIB). In the phase-locked TEM conditions, f ranges from 1Hz to about 40kHz and ∆Φ from 2π/80 to π. VAC ranges from 2mV to 1V depending on observation conditions. The quality of phase-locked strobe images can be improved markedly using a phase-locked strobe electron beam. Under specific conditions, the spatial resolution in images is better than 0.12nm, even though the spatial resolution generally depends on VAC, f, the base TEM, and the conductivity of the specimen. For the model specimens, it is shown that electrochemical impedance spectroscopy and cyclic voltammetry can be performed in a TEM apparatus, and could potentially be synchronized with phase-locked (strobe) imaging and spectroscopy. Severe electron irradiation damage is detected during phase-locked (strobe) electron holography of the model LIB.

Quality evaluation of ultra‐thin samples: Application to graphene

Many new materials emerging are strictly two dimensional (2D), often only one or two monolayers thick. They include transition metal dichalcogenides, such as MoS2 , and graphene. Graphene in particular appears to have many potential applications. Typically the crystalline film without contamination is of interest. Therefore, a reliable method is needed to routinely evaluate the quality of the synthesized samples. Here, we present one such candidate method that utilizes standard electron diffraction and low/medium magnification imaging in a rudimentary transmission electron microscope. The electron irradiation dose is very low thus reducing electron irradiation damage of the investigated samples. As an example, the method was applied to the evaluation of as-grown graphene sample quality and a study on heating-induced change in graphene. It can be used to evaluate the volume and areal ratio of crystalline to noncrystalline component. The method is amiable to automated film quality evaluation.

Electron radiation damage mechanisms in 2D MoSe2

The contributions of different damage mechanisms in single-layer MoSe2 were studied by investigating different MoSe2/graphene heterostructures by the aberration-corrected high–resolution transmission electron microscopy (AC–HRTEM) at 80 keV. The damage cross–sections were determined by direct counting of atoms in the AC–HRTEM images. The contributions of damage mechanisms such as knock–on damage or ionization effects were estimated by comparing the damage rates in different heterostructure configurations, similarly to what has been earlier done with MoS2. The behaviour of MoSe2 was found to be nearly identical to that of MoS2, which is an unexpected result, as the knock-on mechanism should be suppressed in MoSe2 due to the high mass of Se, as compared to S.

Different Forms of Asphaltene Microstructures Discovered in Transmission Electron Microscopy

AbstractTwo forms of microstructures in different types of asphaltenes and asphalt binder samples were discovered by using transmission electron microscopy (TEM). The first type of the microstructures is needle-shaped with a crystalline structure, while the second type is plate-shaped without a regular pattern. The size of the microstructures ranges from a few nanometers to several micrometers. The microstructures are more prevalent in field-aged asphalt binder and asphaltenes samples than those in nonaged ones. Experimental results indicate that both forms of microstructures are not made of wax, but asphaltenes molecules. The two forms of asphaltenes microstructures differ in morphology, microscopic structure, chemical composition, and resistance to electron radiation damage, indicating that they are formed by different mechanisms and have different physicochemical properties. Both types of microstructures also show thermal stability at elevated temperatures. The prevalence, size, and shape of the micros...

Theranostic Application of Mixed Gold and Superparamagnetic Iron Oxide Nanoparticle Micelles in Glioblastoma Multiforme.

The treatment of glioblastoma multiforme, the most prevalent and lethal form of brain cancer in humans, has been limited in part by poor delivery of drugs through the blood-brain barrier and by unclear delineation of the extent of infiltrating tumor margins. Nanoparticles, which selectively accumulate in tumor tissue due to their leaky vasculature and the enhanced permeability and retention effect, have shown promise as both therapeutic and diagnostic agents for brain tumors. In particular, superparamagnetic iron oxide nanoparticles (SPIONs) have been leveraged as T2-weighted MRI contrast agents for tumor detection and imaging; and gold nanoparticles (AuNP) have been demonstrated as radiosensitizers capable of propagating electron and free radical-induced radiation damage to tumor cells. In this study, we investigated the potential applications of novel gold and SPION-loaded micelles (GSMs) coated by polyethylene glycol-polycaprolactone (PEG-PCL) polymer. By quantifying gh2ax DNA damage foci in glioblastoma cell lines, we tested the radiosensitizing efficacy of these GSMs, and found that GSM administration in conjunction with radiation therapy (RT) led to ~2-fold increase in density of double-stranded DNA breaks. For imaging, we used GSMs as a contrast agent for both computed tomography (CT) and magnetic resonance imaging (MRI) studies of stereotactically implanted GBM tumors in a mouse model, and found that MRI but not CT was sufficiently sensitive to detect and delineate tumor borders after administration and accumulation of GSMs. These results suggest that with further development and testing, GSMs may potentially be integrated into both imaging and treatment of brain tumors, serving a theranostic purpose as both an MRI-based contrast agent and a radiosensitizer.

Review—Ionizing Radiation Damage Effects on GaN Devices

Gallium Nitride based high electron mobility transistors (HEMTs) are attractive for use in high power and high frequency applications, with higher breakdown voltages and two dimensional electron gas (2DEG) density compared to their GaAs counterparts. Specific applications for nitride HEMTs include air, land and satellite based communications and phased array radar. Highly efficient GaN-based blue light emitting diodes (LEDs) employ AlGaN and InGaN alloys with different compositions integrated into heterojunctions and quantum wells. The realization of these blue LEDs has led to white light sources, in which a blue LED is used to excite a phosphor material; light is then emitted in the yellow spectral range, which, combined with the blue light, appears as white. Alternatively, multiple LEDs of red, green and blue can be used together. Both of these technologies are used in high-efficiency white electroluminescent light sources. These light sources are efficient and long-lived and are therefore replacing incandescent and fluorescent lamps for general lighting purposes. Since lighting represents 20–30% of electrical energy consumption, and because GaN white light LEDs require ten times less energy than ordinary light bulbs, the use of efficient blue LEDs leads to significant energy savings. GaN-based devices are more radiation hard than their Si and GaAs counterparts due to the high bond strength in III-nitride materials. The response of GaN to radiation damage is a function of radiation type, dose and energy, as well as the carrier density, impurity content and dislocation density in the GaN. The latter can act as sinks for created defects and parameters such as the carrier removal rate due to trapping of carriers into radiation-induced defects depends on the crystal growth method used to grow the GaN layers. The growth method has a clear effect on radiation response beyond the carrier type and radiation source. We review data on the radiation resistance of AlGaN/GaN and InAlN/GaN HEMTs and GaN–based LEDs to different types of ionizing radiation, and discuss ion stopping mechanisms. The primary energy levels introduced by different forms of radiation, carrier removal rates and role of existing defects in GaN are discussed. The carrier removal rates are a function of initial carrier concentration and dose but not of dose rate or hydrogen concentration in the nitride material grown by Metal Organic Chemical Vapor Deposition. Proton and electron irradiation damage in HEMTs creates positive threshold voltage shifts due to a decrease in the two dimensional electron gas concentration resulting from electron trapping at defect sites, as well as a decrease in carrier mobility and degradation of drain current and transconductance. State-of-art simulators now provide accurate predictions for the observed changes in radiation-damaged HEMT performance. Neutron irradiation creates more extended damage regions and at high doses leads to Fermi level pinning while 60Co γ-ray irradiation leads to much smaller changes in HEMT drain current relative to the other forms of radiation. In InGaN/GaN blue LEDs irradiated with protons at fluences near 1014 cm−2 or electrons at fluences near 1016 cm−2, both current-voltage and light output-current characteristics are degraded with increasing proton dose. The optical performance of the LEDs is more sensitive to the proton or electron irradiation than that of the corresponding electrical performances.

(Invited) Radiation Effects in AlGaN/GaN and InAlN/GaN High Electron Mobility Transistors

GaN-based devices are more radiation hard than their Si and GaAs counterparts due to the high bond strength in III-nitride materials. In this paper we review data on the radiation resistance of GaN-based transistors such as AlGaN/GaN and InAlN/GaN High Electron Mobility Transistors (HEMTs) to different types of ionizing radiation. In this paper, the primary energy levels introduced by different forms of radiation, carrier removal rates and role of existing defects are discussed. The carrier removal rates are a function of initial carrier concentration, dose and dose rate but not of hydrogen concentration in the nitride material grown by Metal Organic Chemical Vapor Deposition. Proton and electron irradiation damage in HEMTs creates positive threshold voltage shifts due to a decrease in the two dimensional electron gas concentration resulting from electron trapping at defect sites, as well as a decrease in carrier mobility and degradation of drain current and transconductance. Neutron irradiation created more extended damage regions and at high doses leads to Fermi level pinning while 60Co γ-ray irradiation leads to much smaller changes in HEMT drain current relative to the other forms of radiation.

Electronic damage in S atoms in a native protein crystal induced by an intense X-ray free-electron laser pulse.

Current hard X-ray free-electron laser (XFEL) sources can deliver doses to biological macromolecules well exceeding 1 GGy, in timescales of a few tens of femtoseconds. During the pulse, photoionization can reach the point of saturation in which certain atomic species in the sample lose most of their electrons. This electronic radiation damage causes the atomic scattering factors to change, affecting, in particular, the heavy atoms, due to their higher photoabsorption cross sections. Here, it is shown that experimental serial femtosecond crystallography data collected with an extremely bright XFEL source exhibit a reduction of the effective scattering power of the sulfur atoms in a native protein. Quantitative methods are developed to retrieve information on the effective ionization of the damaged atomic species from experimental data, and the implications of utilizing new phasing methods which can take advantage of this localized radiation damage are discussed.

Atomic-Resolution STEM Imaging of Graphene at Low Voltage of 30kV with Resolution Enhancement by Using Large Convergence Angle.

Atomic resolution at a low accelerating voltage with aberration correction is required to reduce the electron irradiation damage in scanning transmission electron microscopy imaging. However, the reduction in resolution caused by the diffraction limit becomes severe with increasing electron wavelength at low accelerating voltages. The developed aberration corrector can compensate for higher-order aberration in scanning transmission electron microscopy to expand the uniform phase angle. The resolution for imaging graphene at 30kV is evaluated by changing the convergence angle for a probe-forming system with a higher-order aberration corrector. A single-carbon atom on graphene is successfully imaged at atomic resolution with a cold-field emission gun by dark-field imaging at an accelerating voltage of 30kV.

Effects of copper diffusion in gallium arsenide solar cells for space applications

High efficiency, thin-film Epitaxial Lift-Off (ELO) III–V solar cells offer excellent characteristics for implementation in flexible solar panels for space applications. However, the current thin-film ELO solar cell design generally includes a copper handling and support foil. Copper diffusion has a potentially detrimental effect on the device performance and the challenging environment provided by space (high temperatures, electron and proton irradiation) might induce diffusion. It is shown that heat treatments induce copper diffusion. The open-circuit voltage (Voc) is the most affected solar cell parameter. The decrease in Voc can be explained by enhanced non-radiative recombination via Cu trap levels in the middle of the band gap. The decrease in Voc is found to be dependent on junction depth. In all Cu cells annealed at T≥300°C signs of Cu diffusion are present, which implies that a barrier layer inhibiting Cu diffusion is necessary. Electron radiation damage was found to have no influence on Cu diffusion.

(Invited) Radiation Effects in AlGaN/GaN and InAlN/GaN High Electron Mobility Transistors

GaN HEMTs are more radiation hard than their Si and GaAs counterparts due to the high bond strength in III-nitride materials. We review data on the radiation resistance of GaN-based transistors such as AlGaN/GaN and InAlN/GaN High Electron Mobility Transistors (HEMTs) to different types of ionizin gradiation. The primary energy levels introduced by different forms of radiation, carrier removal rates and role of existing defects are discussed. The carrier removal rates are a function of initial carrier concentration, dose and dose rate but not of hydrogen concentration in the nitride material grown by Metal Organic Chemical Vapor Deposition. Proton and electron irradiation damage in HEMTs creates positive threshold voltage shifts due to a decrease in the two dimensional electron gas concentration resulting from electron trapping at defect sites, as well as a decrease in carrier mobility and degradation of drain current and transconductance. Neutron irradiation created more extended damage regions and at high doses leads to Fermi level pinning while 60Co γ-ray irradiation leads to much smaller changes in HEMT drain current relative to the other forms of radiation.

Radiation Effects in GaN-Based High Electron Mobility Transistors

GaN-based devices are more radiation hard than their Si and GaAs counterparts due to the high bond strength in III-nitride materials. In this paper, we review data on the radiation resistance of GaN-based transistors such as AlGaN/GaN and InAlN/GaN high electron mobility transistors (HEMTs) to different types of ionizing radiation. The primary energy levels introduced by different forms of radiation, carrier removal rates and role of existing defects are discussed. The carrier removal rates are a function of initial carrier concentration, dose and dose rate but not of hydrogen concentration in the nitride material grown by metal organic chemical vapor deposition. Proton and electron irradiation damage in HEMTs creates positive threshold voltage shifts due to a decrease in the two-dimensional electron gas concentration resulting from electron trapping at defect sites, as well as a decrease in carrier mobility and degradation of drain current and transconductance. Neutron irradiation created more extended damage regions and at high doses leads to Fermi level pinning, while 60Co γ-ray irradiation leads to much smaller changes in HEMT drain current relative to the other forms of radiation.