Low-energy Electron Irradiation Research Articles

A novel setup for the determination of absolute cross sections for low-energy electron induced strand breaks in oligonucleotides – The effect of the radiosensitizer 5-fluorouracil*

Low-energy electrons (LEEs) play an important role in DNA radiation damage. Here we present a method to quantify LEE induced strand breakage in well-defined oligonucleotide single strands in terms of absolute cross sections. An LEE irradiation setup covering electron energies <500 eV is constructed and optimized to irradiate DNA origami triangles carrying well-defined oligonucleotide target strands. Measurements are presented for 10.0 and 5.5 eV for different oligonucleotide targets. The determination of absolute strand break cross sections is performed by atomic force microscopy analysis. An accurate fluence determination ensures small margins of error of the determined absolute single strand break cross sections σ SSB . In this way, the influence of sequence modification with the radiosensitive 5-Fluorouracil (5FU) is studied using an absolute and relative data analysis. We demonstrate an increase in the strand break yields of 5FU containing oligonucleotides by a factor of 1.5 to 1.6 compared with non-modified oligonucleotide sequences when irradiated with 10 eV electrons.

Mechanisms of H and CO loss from the uracil nucleobase following low energy electron irradiation

Ionising radiation in cells generates secondary low energy electrons (LEEs) which can induce biomolecular damage when incident upon a particular biomolecule. Notable biomolecules include those contained within double-stranded DNA and RNA helices, which upon exposure to LEEs, may form reactive intermediate products that show detriment to their specific structures and functions. Such damaging processes are understood to proceed via dissociative electron attachment (DEA). Using anion resonance stabilisation methods, coupled to state-of-the-art electronic structure methods, and reaction path mapping, the work presented herein highlights the detailed mechanisms associated with molecular elimination of CO and H from the uracil nucleobase following LEE irradiation - providing a rationale for earlier experiments. The results highlight a subset of resonances that show a labile route for forming CO + anionic 1,3-dihydroimidazole (1,3-DHIM-). The nascent 1,3-DHIM anion is itself unstable with respect to N-H bond fission - ultimately forming anionic 1-imidazole (1-IM-) + H products. This hitherto unknown mechanism sheds light on the possible lesion processes that may be encountered by biomolecular constituents when exposed to electron energies analogous to those present in medicinal X-ray diagnostics, aviation and interstellar space. The work also offers some insight into the reactive processes that may have occurred in prebiotic earth.

Molecular hydrogen production from amorphous solid water during low energy electron irradiation.

This work investigates the production of molecular hydrogen isotopologues (H2, HD, and D2) during low energy electron irradiation of layered and isotopically labelled thin films of amorphous solid water (ASW) in ultrahigh vacuum. Experimentally, the production of these molecules with both irradiation time and incident electron energy in the range 400 to 500 eV is reported as a function of the depth of a buried D2O layer in an H2O film. H2 is produced consistently in all measurements, reflecting the H2O component of the film, though it does exhibit a modest reduction in intensity at the time corresponding to product escape from the buried D2O layer. In contrast, HD and D2 production exhibit peaks at times corresponding to product escape from the buried D2O layer in the composite film. These features broaden the deeper the HD or D2 is formed due to diffusion. A simple random-walk model is presented that can qualitatively explain the appearance profile of these peaks as a function of the incident electron penetration.

Electron-beam-induced annealing of natural zircon: a Raman spectroscopic study

The annealing of radiation damage in zircon by low-energy electron irradiation was explored systematically. Natural zircon samples spanning a wide range of self-irradiation damage were irradiated with the focused electron beam of an electron probe microanalyser. The effects of beam current and irradiation time were tested systematically, and the changes in zircon were measured using Raman spectroscopy. Our results confirm the damage-annealing effect of an accelerated electron beam. We demonstrate that non-thermal annealing occurs through electron-enhanced defect reactions and that the extent of the annealing is a function of both the irradiation time and the beam current. The complete annealing of radiation damage in zircon by an accelerated electron beam was not possible under the conditions of our experiments. Our results indicate that Raman band broadening in ion-irradiated zircon can possibly be explained through phonon confinement, as the estimated domain sizes of the crystalline volume amid recoil clusters decrease with increasing α dose. The results underlay the importance of doing Raman spectroscopy before electron-beam and ion-beam analysis. To avoid unwanted beam-induced annealing of damage in zircon during EPMA analysis, the electron energy transferred per volume unit of sample should be minimised, for instance by keeping the integrated charge low and/or by defocusing the electron beam.

Pathogens Inactivated by Low-Energy-Electron Irradiation Maintain Antigenic Properties and Induce Protective Immune Responses.

Inactivated vaccines are commonly produced by incubating pathogens with chemicals such as formaldehyde or β-propiolactone. This is a time-consuming process, the inactivation efficiency displays high variability and extensive downstream procedures are often required. Moreover, application of chemicals alters the antigenic components of the viruses or bacteria, resulting in reduced antibody specificity and therefore stimulation of a less effective immune response. An alternative method for inactivation of pathogens is ionizing radiation. It acts very fast and predominantly damages nucleic acids, conserving most of the antigenic structures. However, currently used irradiation technologies (mostly gamma-rays and high energy electrons) require large and complex shielding constructions to protect the environment from radioactivity or X-rays generated during the process. This excludes them from direct integration into biological production facilities. Here, low-energy electron irradiation (LEEI) is presented as an alternative inactivation method for pathogens in liquid solutions. LEEI can be used in normal laboratories, including good manufacturing practice (GMP)- or high biosafety level (BSL)-environments, as only minor shielding is necessary. We show that LEEI efficiently inactivates different viruses (influenza A (H3N8), porcine reproductive and respiratory syndrome virus (PRRSV), equine herpesvirus 1 (EHV-1)) and bacteria (Escherichia coli) and maintains their antigenicity. Moreover, LEEI-inactivated influenza A viruses elicit protective immune responses in animals, as analyzed by virus neutralization assays and viral load determination upon challenge. These results have implications for novel ways of developing and manufacturing inactivated vaccines with improved efficacy.

Contact Resistance and Channel Conductance of Graphene Field-Effect Transistors under Low-Energy Electron Irradiation.

We studied the effects of low-energy electron beam irradiation up to 10 keV on graphene-based field effect transistors. We fabricated metallic bilayer electrodes to contact mono- and bi-layer graphene flakes on SiO2, obtaining specific contact resistivity and carrier mobility as high as 4000 cm2·V−1·s−1. By using a highly doped p-Si/SiO2 substrate as the back gate, we analyzed the transport properties of the device and the dependence on the pressure and on the electron bombardment. We demonstrate herein that low energy irradiation is detrimental to the transistor current capability, resulting in an increase in contact resistance and a reduction in carrier mobility, even at electron doses as low as 30 e−/nm2. We also show that irradiated devices recover their pristine state after few repeated electrical measurements.

Low energy electron irradiation induced carbon etching: Triggering carbon film reacting with oxygen from SiO2 substrate

We report low-energy (50–200 eV) electron irradiation induced etching of thin carbon films on a SiO2 substrate. The etching mechanism was interpreted that electron irradiation stimulated the dissociation of the carbon film and SiO2, and then triggered the carbon film reacting with oxygen from the SiO2 substrate. A requirement for triggering the etching of the carbon film is that the incident electron penetrates through the whole carbon film, which is related to both irradiation energy and film thickness. This study provides a convenient electron-assisted etching with the precursor substrate, which sheds light on an efficient pathway to the fabrication of nanodevices and nanosurfaces.

Dynamic charge transport characteristics in polyimide surface and surface layer under low-energy electron radiation

Charge transport behaviors of dielectric under electron radiation have an important influence on surface flashover performance. In this paper, charging process and model of dielectric during electron radiation are investigated based on the synergistic effect of electron movement on dielectric surface and charge transport properties in dielectric surface layer. For one thing, electrons accumulated in dielectric surface layer will form a reverse electric field acting against kinetic electrons flowing to dielectric surface, which affects the energy and density of electrons reaching the surface. For another, the changes of electron energy and density will further affect the dynamic processes of electron deposition, transport and accumulation in the surface layer. A dielectric charging model is proposed, and charge transport characteristics in dielectric surface and surface layer are obtained, including the temporal behavior of the incident kinetic electrons flowing to dielectric surface, the temporal behavior of secondary electrons and surface conduction charge, as well as the spatial and temporal behavior of the interior potential and electric field. Based on surface potential decay curves of polyimide under different electron energy levels (3-11 keV), the surface potential decay process and model are investigated. The surface trap distribution of polyimide shows different properties under different energy levels. The shallow trap level increases slightly with the increase of electron energy, ranging from 0.81 eV-0.85 eV, while the deep trap level remains unchanged about 0.94 eV. Besides, the amount of trap charge density gradually increases with the increase of electron energy.

Nanosized graphene sheets enhanced photoelectric behavior of carbon film on p-silicon substrate

We found that nanosized graphene sheets enhanced the photoelectric behavior of graphene sheets embedded carbon (GSEC) film on p-silicon substrate, which was deposited under low energy electron irradiation in electron cyclotron resonance plasma. The GSEC/p-Si photodiode exhibited good photoelectric performance with photoresponsivity of 206 mA/W, rise and fall time of 2.2, and 4.3 μs for near-infrared (850 nm) light. The origin of the strong photoelectric behavior of GSEC film was ascribed to the appearance of graphene nanosheets, which led to higher barrier height and photoexcited electron-collection efficiency. This finding indicates that GSEC film has the potential for photoelectric applications.

Low energy electron beam processing of YBCO thin films

Effects of low energy 30keV electron irradiation of superconducting YBa2Cu3O7−δ thin films have been investigated by means of transport and micro-Raman spectroscopy measurements. The critical temperature and the critical current of 200nm thick films initially increase with increasing fluency of the electron irradiation, reach the maximum at fluency 3−4×1020 electrons/cm2, and then decrease with further fluency increase. In much thinner films (75nm), the critical temperature increases while the critical current decreases after low energy electron irradiation with fluencies below 1020 electrons/cm2. The Raman investigations suggest that critical temperature increase in irradiated films is due to healing of broken CuO chains that results in increased carrier’s concentration in superconducting CuO2 planes. Changes in the critical current are controlled by changes in the density of oxygen vacancies acting as effective pinning centers for flux vortices. The effects of low energy electron irradiation of YBCO turned out to result from a subtle balance of many processes involving oxygen removal, both by thermal activation and kick-off processes, and ordering of chains environment by incident electrons.

Low-energy electron irradiation of preheated and gas-exposed single-wall carbon nanotubes

We investigate the conditions under which electron irradiation at 2keV of single-wall carbon nanotube (SWCNT) bundles produces an increase in the Raman D peak. We find that irradiation of SWCNTs that are preheated in situ at 600°C for 1h in ultrahigh vacuum before irradiation does not result in an increase in the D peak. Irradiation of SWCNTs that are preheated in vacuum and then exposed to air or gases results in an increase in the D peak, suggesting that adsorbates play a role in the increase in the D peak. Small diameter SWCNTs that are not preheated or preheated and then exposed to air show a significant increase in the D and G bands after irradiation. X-ray photoelectron spectroscopy shows no chemical shifts in the C 1s peak of SWCNTs that have been irradiated versus SWCNTs that have not been irradiated, suggesting that chemisorption of adsorbates is not responsible for the increase in the D peak.

Fabrication of FeSi and Fe3Si compounds by electron beam induced mixing of [Fe/Si]2 and [Fe3/Si]2 multilayers grown by focused electron beam induced deposition

Fe-Si binary compounds have been fabricated by focused electron beam induced deposition by the alternating use of iron pentacarbonyl, Fe(CO)5, and neopentasilane, Si5H12 as precursor gases. The fabrication procedure consisted in preparing multilayer structures which were treated by low-energy electron irradiation and annealing to induce atomic species intermixing. In this way, we are able to fabricate FeSi and Fe3Si binary compounds from [Fe/Si]2 and [Fe3/Si]2 multilayers, as shown by transmission electron microscopy investigations. This fabrication procedure is useful to obtain nanostructured binary alloys from precursors which compete for adsorption sites during growth and, therefore, cannot be used simultaneously.

Correction to "Monolayer Graphene Platform for the Study of DNA Damage by Low-Energy Electron Irradiation".

Correction to "Monolayer Graphene Platform for the Study of DNA Damage by Low-Energy Electron Irradiation".

Low-voltage-exposure-enabled hydrogen silsesquioxane bilayer-like process for three-dimensional nanofabrication

We report a bilayer-like electron-beam lithographic process to obtain three-dimensional (3D) nanostructures by using only a single hydrogen silsesquioxane (HSQ) resist layer. The process utilizes the short penetration depth of low-energy (1.5 keV) electron irradiation to first obtain a partially cross-linked HSQ top layer and then uses a high-voltage electron beam (30 keV) to obtain self-aligned undercut (e.g. mushroom-shaped) and freestanding HSQ nanostructures. Based on the well-defined 3D resist patterns, 3D metallic nanostructures were directly fabricated with high fidelity by just depositing a metallic layer. As an example, Ag-coated mushroom-shaped nanostructures were fabricated, which showed lower plasmon resonance damping compared to their planar counterparts. In addition, the undercut 3D nanostructures also enable more reliable lift-off in comparison with the planar nanostructures, with which high-quality silver nanohole arrays were fabricated which show distinct and extraordinary optical transmission in the visible range.

Low-energy electron irradiation induced top-surface nanocrystallization of amorphous carbon film

We report a low-energy electron irradiation method to nanocrystallize the top-surface of amorphous carbon film in electron cyclotron resonance plasma system. The nanostructure evolution of the carbon film as a function of electron irradiation density and time was examined by transmission electron microscope (TEM) and Raman spectroscopy. The results showed that the electron irradiation gave rise to the formation of sp2 nanocrystallites in the film top-surface within 4nm thickness. The formation of sp2 nanocrystallite was ascribed to the inelastic electron scattering in the top-surface of carbon film. The frictional property of low-energy electron irradiated film was measured by a pin-on-disk tribometer. The sp2 nanocrystallized top-surface induced a lower friction coefficient than that of the original pure amorphous film. This method enables a convenient nanocrystallization of amorphous surface.

Control of carbon vacancy in SiC toward ultrahigh-voltage power devices

A carbon vacancy defect is one of the most abundant point defects in SiC (as-grown, irradiated, annealed) and of technological importance because the acceptor-like level of a carbon monovacancy (Z1/2 center: EC – 0.63 eV) works as the primary carrier-lifetime killer in 4H–SiC. The carbon vacancy defects can be preferentially generated by either low-energy electron irradiation or high-temperature treatment in an inert gas ambient. On the other hand, the carbon vacancy defects can be almost eliminated by either a carbon-ion implantation process or thermal oxidation. By combination of these techniques, the density of carbon vacancy defects can be controlled in the wide range from 1011 cm−3 to 1015 cm−3 or even higher.

Structural damaging in few -layer graphene due to the low energy electron irradiation

Data of Raman spectroscopy from graphene and few-layer graphene (FLG) irradiated by SEM electron beam in the range of energies 0.2 -30 keV are presented. The obvious effect of damaging the nanostructures by all used beam energies for specimens placed on insulator substrates (<TEX>$SiO_2$</TEX>) was revealed. At the same time, no signs of structural defects were observed in the cases when FLG have been arranged on metallic substrate. A new physical mechanism of under threshold energy defect production supposing possible formation of intensive electrical charged puddles on insulator substrate surface is suggested.

Low-energy (&lt;20 eV) and high-energy (1000 eV) electron-induced methanol radiolysis of astrochemical interest

We report the first infrared study of the low-energy (<20 eV) electron-induced reactions of condensed methanol. Our goal is to simulate processes which occur when high-energy cosmic rays interact with interstellar and cometary ices, where methanol, a precursor of several prebiotic species, is relatively abundant. The interactions of high-energy radiation, such as cosmic rays (Emax ∼ 1020 eV), with matter produce large numbers of low-energy secondary electrons, which are known to initiate radiolysis reactions in the condensed phase. Using temperature programmed desorption (TPD) and infrared reflection absorption spectroscopy (IRAS), we have investigated low-energy (5–20 eV) and high-energy (∼1000 eV) electron-induced reactions in condensed methanol (CH3OH). IRAS has the benefit that it does not require thermal processing prior to product detection. Using IRAS, we have found evidence for the formation of ethylene glycol (HOCH2CH2OH), formaldehyde (CH2O), dimethyl ether (CH3OCH3), methane (CH4), carbon dioxide (CO2), carbon monoxide (CO), and the hydroxyl methyl radical (·CH2OH) upon both low-energy and high-energy electron irradiation of condensed methanol at ∼85 K. Additionally, TPD results, presented herein, are similar for methanol films irradiated with both 1000 eV and 20 eV electrons. These IRAS and TPD findings are qualitatively consistent with the hypothesis that high-energy condensed phase radiolysis is mediated by low-energy electron-induced reactions. Moreover, methoxymethanol (CH3OCH2OH) could serve as a tracer molecule for electron-induced reactions in the interstellar medium. The results of experiments such as ours may provide a fundamental understanding of how complex organic molecules are synthesized in cosmic ices.

The role of low-energy (≤ 20 eV) electrons in astrochemistry

UV photon-driven condensed phase cosmic ice reactions have been the main focus in understanding the extraterrestrial synthesis of complex organic molecules. Low-energy (≤20eV) electron-induced reactions, on the other hand, have been largely ignored. In this article, we review studies employing surface science techniques to study low-energy electron-induced condensed phase reactions relevant to astrochemistry. In particular, we show that low-energy electron irradiation of methanol ices leads to the synthesis of many of the same complex molecules formed through UV irradiation. Moreover, our results are qualitatively consistent with the hypothesis that high-energy condensed phase radiolysis is mediated by low-energy electron-induced reactions. In addition, due to the numbers of available low-energy secondary electrons resulting from the interaction of high-energy radiation with matter as well as differences between electron- and photon-induced processes, low-energy electron-induced reactions are perhaps as, or even more, effective than photon-induced reactions in initiating condensed-phase chemical reactions in the interstellar medium. Consequently, we illustrate a need for astrochemical models to include the details of electron-induced reactions in addition to those driven by UV photons. Finally, we show that low-energy electron-induced reactions may lead to the production of unique molecular species that could serve as tracer molecules for electron-induced condensed phase reactions in the interstellar medium.

Enhancement of Au-induced lateral crystallization in electron-irradiated amorphous Ge on SiO2

We have investigated the acceleration energy (0.5–2.0 MeV)-modulated electron irradiation effect of Au-induced lateral crystallization for amorphous Ge on SiO2. As a result, low-energy electron (≤1.0 MeV) irradiation was not effective for Au-induced lateral crystallization. On the other hand, when high-energy electron (2.0 MeV) irradiation was utilized, the lateral growth velocity was significantly enhanced (∼1.8 times). We have confirmed that the Au-induced lateral growth is enhanced by electron irradiation, which is due to the introduction of point defects into amorphous Ge, allowing the easy diffusion of Au atoms.