TiO₂-2 radiating damages as a result of the irradiation helium ions with energies of 0.12 and 4 MeV on the linear accelerator

On the linear accelerator of helium ions, the irradiation of TiO₂-2 samples with ions energy of 0.12 and 4 MeV to doses of ≈ 1∙10¹⁸ ion/cm² is executed. The elemental composition of TiO₂-2 samples is made by roentgen-fluorescence method. After irradiation a change of electrophysical characteristics...

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Published in:Problems of Atomic Science and Technology
Date:2023
Main Authors: Butenko, V.I., Cenian, A., Dyachenko, O.F., Manuilenko, O.V., Pavlii, K.V., Sawczak, M., Zajtsev, B.V., Zhurba, V.I.
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Language:English
Published: Національний науковий центр «Харківський фізико-технічний інститут» НАН України 2023
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Online Access:https://nasplib.isofts.kiev.ua/handle/123456789/196183
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Journal Title:Digital Library of Periodicals of National Academy of Sciences of Ukraine
Cite this:TiO₂-2 radiating damages as a result of the irradiation helium ions with energies of 0.12 and 4 MeV on the linear accelerator / V.I. Butenko, A. Cenian, O.F. Dyachenko, O.V. Manuilenko, K.V. Pavlii, M. Sawczak, B.V. Zajtsev, V.I. Zhurba // Problems of Atomic Science and Technology. — 2023. — № 4. — С. 96-104. — Бібліогр.: 24 назв. — англ.

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Digital Library of Periodicals of National Academy of Sciences of Ukraine
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author Butenko, V.I.
Cenian, A.
Dyachenko, O.F.
Manuilenko, O.V.
Pavlii, K.V.
Sawczak, M.
Zajtsev, B.V.
Zhurba, V.I.
author_facet Butenko, V.I.
Cenian, A.
Dyachenko, O.F.
Manuilenko, O.V.
Pavlii, K.V.
Sawczak, M.
Zajtsev, B.V.
Zhurba, V.I.
citation_txt TiO₂-2 radiating damages as a result of the irradiation helium ions with energies of 0.12 and 4 MeV on the linear accelerator / V.I. Butenko, A. Cenian, O.F. Dyachenko, O.V. Manuilenko, K.V. Pavlii, M. Sawczak, B.V. Zajtsev, V.I. Zhurba // Problems of Atomic Science and Technology. — 2023. — № 4. — С. 96-104. — Бібліогр.: 24 назв. — англ.
collection DSpace DC
container_title Problems of Atomic Science and Technology
description On the linear accelerator of helium ions, the irradiation of TiO₂-2 samples with ions energy of 0.12 and 4 MeV to doses of ≈ 1∙10¹⁸ ion/cm² is executed. The elemental composition of TiO₂-2 samples is made by roentgen-fluorescence method. After irradiation a change of electrophysical characteristics is investigated, microscopic researches on electronic and optical microscopes are conducted. Numerical calculations of atom sputtering ratios taking into account of input angles of helium ions in a sample, and also phonons formation, atoms redistribution (segregation), appearance of the vacancies and displacements in TiO₂-2 sample are made. Processes of the flaking formation are investigated, and also presence of the metallization effect and long-range interaction effect in the irradiated samples is shown. На лінійному прискорювачі іонів гелію виконано опромінення зразків TiO₂-2 з енергією іонів 0,12 і 4 МеВ до доз ≈ 1∙10¹⁸ іон/см². Елементний склад зразків TiO₂-2 отримано рентгенофлюоресцентним методом. Після опромінення проведено мікроскопічні дослідження на електронному та оптичному мікроскопах, досліджено змінення електрофізичних характеристик. Зроблено числові розрахунки коефіцієнтів розпилення атомів з урахуванням кутів входу іонів гелію в зразок, а також утворення фононів, перерозподілу атомів (сегрегація), утворення вакансій і зміщень у зразкa TiO₂-2. Досліджено процеси утворення флекінгу та показано наявність ефектів металізації й далекодії в опромінених зразках.
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fulltext 96 ISSN 1562-6016. Problems of Atomic Science and Technology. 2023. № 4(146) https://doi.org/10.46813/2023-146-096 TiO2-2 RADIATING DAMAGES AS A RESULT OF THE IRRADIATION HELIUM IONS WITH ENERGIES OF 0.12 AND 4 MeV ON THE LINEAR ACCELERATOR V.I. Butenko 1 , A. Cenian 2 , O.F. Dyachenko 1 , O.V. Manuilenko 1 , K.V. Pavlii 1 , M. Sawczak 2 , B.V. Zajtsev 1 , V.I. Zhurba 1 1 National Science Center “Kharkov Institute of Physics and Technology”, Kharkiv, Ukraine; 2 Institute of Fluid-Flow Machinery, Polish Academy of Sciences, Gdansk E-mail: dyachenkoa@kipt.kharkov.ua On the linear accelerator of helium ions, the irradiation of TiO2-2 samples with ions energy of 0.12 and 4 MeV to doses of ≈ 1∙10 18 ion/cm 2 is executed. The elemental composition of TiO2-2 samples is made by roentgen- fluorescence method. After irradiation a change of electrophysical characteristics is investigated, microscopic re- searches on electronic and optical microscopes are conducted. Numerical calculations of atom sputtering ratios tak- ing into account of input angles of helium ions in a sample, and also phonons formation, atoms redistribution (seg- regation), appearance of the vacancies and displacements in TiO2-2 sample are made. Processes of the flaking for- mation are investigated, and also presence of the metallization effect and long-range interaction effect in the irradi- ated samples is shown. PACS: 29.17+w, 29.27 Bd INTRODUCTION In nuclear power plants ceramics is used as a ther- mal protection (Al2O3, SiO2), nuclear fuel (UO2, PuO2), materials of the regulating units (B4C, Sm2O3), slowing down and reflecting materials (BeO, ZrO2, Be2C), mate- rials of the neutron protection (B4C, HfO3, Sm2O3), electroisolation in an active zone (Al2O3, MgO), fuel element covers (SiC, Si3N4). In thermonuclear power ceramics plan to use for thermal and electric isolation of the first wall of the plasma chamber (SiC, Si3N4), plasma restrictions (SiC, Al2O3, B4C), neutron protection (blankets from LiAlO2, Li2SiO3, Li2O), as a material for windows of the various frequency plasma heating (Al2O3, BeO) and etc. Titan dioxide (TiO2) is widely used in the chemical techniques, instrument making and medicine. Pos- sessing properties of the semiconductor with n-conductivity, TiO2 is a perspective material for for- mation of the solid electrolytes and materials which possess catalytic properties. Wide use TiO2 as solid electrolyte is prevented its big resistance (10 13 Ω/cm). Analysis of TiO2 properties and methods of its syn- thesis [1] point out the possibilities to change ionic con- ductivity by introduction in structure TiO2 the oxides SnO, Co2O3, Sb2O5, AgO which have higher conductivi- ty. The same effect as it will be resulted below, is reached by TiO2 helium ions irradiation without addi- tion of an exterior compounds. On a conductivity change it’s possible to judge about physical-chemical processes proceeding in irradiated materials, in particu- lar. The knowledge of conductivity change dependence from an irradiation dose and a current density of helium ions allow to create ionic current gauges, to control pro- cess of materials processing in extreme conditions and etc. The odd researches spent on semiconductors [2, 3] or separate metals and alloys [2, 4 - 7] are devoted the description of an impacts of continuous and pulse elec- tronic and ionic beams on a surface change of the irradi- ated materials. The numerous publications analysis has shown that at processing by ionic beams of solids for the purpose of their modification the ionic beams with energy from a hundred kiloelectronvolts to several me- gaelectronvolts are applied. Beams of easy ions (pro- tons, helium, carbon, nitrogen, boron, oxygen, their mixture and combination) have appeared the most ef- fective as, on the one hand, in comparison with heavy ions it’s easier to receive, and, on the other hand, they have essentially big runs in a target. Ionic beams are capable to create in near-surface layers of materials the ultra-fast heating and superhigh-speed cooling (∆T/∆t~10 8 …10 11 К/s). The temperatures gradient thus on a surface and in near-surface target layers can make 10 9 К/m. It leads to changes of a structure and proper- ties of processed materials. At impact of ionic beams on a solids surface the defining factors influencing of a surface morphology and on a dynamics of structurally- phase transformations, occurring in a surface layers, are spatio-temporal distribution of an energy release power: density of the brought energy, action time, heating, melting, evaporation, ablation, thermal stress and shock wave. The surface defines many properties of solids. So, for example, electric properties of semiconductors and dielectrics depend on composition and structure of a surface layer and define the wear resistance and corro- sion resistance, an endurance limit, the heat resistance, etc. At processing of the dielectrics and semiconductors surface by ionic beams the morphological changes and modifications of its element composition take place. In this work an irradiation parameters of TiO2-2 samples on the linear accelerator of helium ions and methods of their measurement are described. Primary radiating characteristics and atom sputtering ratios are calculated. Experimental results of electrophysical properties TiO2-2 are received and presence of metalli- zation effect and long-range action effect in the irradiat- ed samples is shown. ISSN 1562-6016. Problems of Atomic Science and Technology. 2023. № 4(146) 97 1. SOURCE AND PARAMETERS OF THE IRRADIATION, THE SAMPLE CHARACTERISTICS In NSC KIPT the linear accelerator of helium ions (Не + ) with energy of 0.12…4 MeV [8 - 10] works. Basic elements of the linear accelerator of helium ions are: injector, resonator with the accelerating structure, placed in a vacuum casing, and system of a beam for- mation and transport from output of the accelerating section to the irradiation chamber with accompanying diagnostic devices for carrying out of experimental works. Feature of the interdigital accelerating structure of the section linear accelerator of helium ions is use of the alternating-phase focusing variant with step-by-step change of a synchronous phase and accruing amplitude of a RF field in accelerating gaps on a grouping area of the accelerating-focusing path. New effective induct- ance-capacitor adjusting devices (‘сontrivances’) for this section in a form of rods located on a side of drift tubes, opposite to their suspension brackets are devel- oped [10 - 13]. For an irradiation and studying of constructional ma- terial characteristics on the accelerator the special chamber and system of the experimental parameters measurement [14, 15] are created. Vacuum in the cham- ber is carried out with the help of the fore vacuum and turbo-molecular pumps, it provides without the oxygen environment in the chamber volume and the same vacu- um as in accelerating structure. A temperature of irradi- ated samples is set by the heating element located di- rectly in the irradiation chamber and measured by the thermocouple attached to the sample backside. The digi- tal oscillograph ZET-302 and DAC/ADC ZET-210 for registration of irradiated sample parameters which are connected to the computer with the further data record- ing and their processing are used. For change (increase/decrease) of the beam current density falling on a sample and shortening of an irradia- tion time, in front of the irradiation chamber the focus- ing triplet which allows changing beam radius, and, hence, a current density depending on requirements of an experiment is established [16]. A system of the beam formation and transport from accelerating section output to the irradiation chamber is shown in Fig. 1. Photos in absence of a current in triplet quadrupole lenses and at a currents selection are shown in Figs. 2, 3. The chosen focusing system has allowed increasing density of a beam helium ions current in several times (to 7). Currents of ions beam are measured by means of the induction contactless flying gauges established on an input and output from a triplet, and also directly ahead of the irradiated sample [17]. Table 1 Irradiation parameters Parameter Value Beam energy, MeV 0.12…4 Pulse current, µА 1100…300 Pulse length, µs 500 Repetition rate, imp./s 2…5 Sample temperature, °С up to 900 Basic parameters of helium ions beam at an irradia- tion of samples on the linear accelerator are resulted in Table 1. Diameter of helium ions beam made ~15 mm, it corresponds to TiO2-2 irradiated samples. TiO2-2 samples (diameter is 19.6 mm, thickness is 1.00 mm and weight is 1.0459 g) have been chosen for an irradiation. The samples elemental composition was defined by X-ray fluorescent method which is based on dependence of X-ray fluorescence intensity on the ele- ment concentration in a sample. Impurities composition in TiO2-2 sample (a basic element – 95.096%) in per- cent is following: Si-2.325, S-0.222, Cl-0.262, Ca- 0.067, V-0.895, Fe-0.936, Ni-0.016, Cu-0.055, Zr- 0.007, Nb-0.010, Mo-0.009, Pb-0.013, Sn-0.023, I-0.065. TiO2-2 sample surface and its appearance are shown in Fig. 4. Fig. 1. System of the beam formation and transport from accelerating section output to the irradiation chamber Fig. 2. Accelerated beam visualization in absence of a current in triplet quadrupole lenses Fig. 3. Accelerated beam visualization at currents selection in quadrupole lenses (spot diameter of ~1 cm) Fig. 4. TiO2-2 sample surface and appearance 98 ISSN 1562-6016. Problems of Atomic Science and Technology. 2023. № 4(146) The conducted microscopic research of samples sur- face has not shown their roughness in limits of ± 0.1 Å. 2. IONIZATION, SEGREGATION, FORMATION PHONONS, VACANCIES AND DAMAGEABILITY For calculation of the ions range in solids the SRIM software package [18, 19] was used which allows to receive following information about: vacancies distribu- tion in a target; redistribution of irradiated material at- oms (segregation); sputtering ratios; phenomena con- nected with ions energy loss; distribution of ionization and phonons formation. These are ‘primary’ characteris- tics which define processes dissociation, radiating diffu- sion of the sample elements, distribution of elastic waves and etc. Calculations in the SRIM program taking into ac- count of the displacement cascades were spent. Energy losses going on the ionization, phonons formation and damageability by a beam of helium ions and the dis- placement cascades for irradiation energies of 0.12 and 4 MeV are resulted in Table 2. Table 2 Calculated characteristics of the samples Energy, MeV Energy loss, % Ionization Phonons Damageability Не + /cascade Не + /cascade Не + /cascade TiO2 0.12 93.7/1.10 0.78/4.15 0.08/0.20 4 99.68/0.07 0.04/0.20 0.00/0.01 TiO2-2 0.12 93.85/1.00 0.77/4.12 0.08/0.18 4 99.69/0.06 0.04/0.20 0.00/0.01 Energy absolute values for TiO2 and TiO2-2, going on these processes are resulted in Table 3. Energy val- ues for pure TiO2 and TiO2-2 are almost identical. It means that in certain cases it’s possible to use calcula- tions nonmetering of additives in TiO2-2. Table 3 Energy values going on the ionization, phonons for- mation and damageability Energy, МeV Energy, keV/ion Ionization Phonons Damageability TiO2 0.12 113.7 5.9 0.34 4 3990.0 9.6 0.51 TiO2-2 0.12 113.8 5.9 0.31 4 3990.0 9.5 0.50 As appears from Tables 2, 3 a most part of a beam energy goes on the ionization. The basic contribution to phonons formation and damageability occurs at the ex- pense of displacement cascades. On phonons formation at beam energies of 0.12 and 4 MeV it’s spent at 17- 19 times more energy, than for damageability. Hence, the role of phonons and ionization in some radiating effects can be defined. The profiles of ionization, pho- nons formation, segregation and helium occurrence, vacancies formation in TiO2-2 at energies 0.12 and 4 MeV, accordingly, are resulted in Figs. 5, 6, in rela- tive units. 0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0 1.1 1.2 -1.0 -0.5 0.0 0.5 1.0 R el at iv e u n it s L, mm Ionization Phonon Range Vacancy TiO2-2 E = 0.12 MeV Fig. 5. Profiles of the ionization, segregation, phonons formation and vacancies in TiO2-2, Е = 0.12 MeV 0 2 4 6 8 10 12 14 16 18 -1.0 -0.8 -0.6 -0.4 -0.2 0.0 0.2 0.4 0.6 0.8 1.0 R el at iv e u n it s L, mm Ionization Phonons Vacancy Range TiO2-2 E=4 MeV Fig. 6. Profiles of the ionization, segregation, phonons formation and vacancies in TiO2-2, Е = 4 MeV As segregation atoms play a dominant role in change of the thermalphysic and electrophysical characteristics of ceramic materials, relations of TiO2-2 redistributed atoms to helium atoms are presented in Table 4. Table 4 Relations of TiO2-2 redistributed atoms to helium atoms Е = 0.12 МeV O/He Ti/He Si/He S/He Cl/He 64.44 42.85 1.68 0.096 0.113 Ca/He V/He Fe/He Cu/He 0.030 0.380 0.408 0.023 Е = 4 МeV O/He Ti/He Si/He S/He Cl/He 99.90 69.13 2.67 0.152 0.181 Ca/He V/He Fe/He Cu/He 0.048 0.614 0.661 0.039 Other elements bring the insignificant contribution to the segregation process. Vacancies formation and quantity of displacement on an ion in TiO2-2 samples play a dominant role in damageability calculations (dpa – quantity of displace- ments per atom). This data has been received at pro- cessing of calculations in the SRIM program. For damageability calculation (dpa) and damageabil- ity distribution profile the curves of Figs. 5, 6 Vacancies and an expression, given lower, were used: ,ion ion m A mole D dpi D dpi dpa N N m      ISSN 1562-6016. Problems of Atomic Science and Technology. 2023. № 4(146) 99 where ionD is a radiation dose [ion/cm 2 ] (an experi- mental parameter), dpi is a quantity of displacements per ion (from SRIM calculations), AN is the Avogadro number, mole m m M  , 0m SL  , where 0 is the sample measured density, S  1 cm 2 is the sample unit area, L is the maximum ions range in a sample, 1 100 i i i M nm  is the sample molar mass, im is the molecular weight of i-th element sample, in is percent- age i-th element of a sample. Final expression for calcu- lation of displacements per atom (dpa) looks like: 0 1 . 100 ion i i iA D dpi dpa n N SL m        . Damageability (dpa) for Е = 0.12 MeV has made ≈ 49 displacements/atom, for Е = 4 MeV has made ≈ 5.0 displacements/atom (for irradiation doses of 10 18 ion/cm 2 ). The calculated damageability (dpa) pro- files for TiO2-2 samples at helium ions energies of 0.12 and 4 MeV are resulted in Figs. 7, 8. 0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0 1.1 1.2 0 10 20 30 40 50 60 70 80 90 100 110 d p a L, mm TiO2-2 E= 0.12 MeV Fig. 7. Profile of the displacements formation in TiO2-2 sample at helium ions irradiation with E = 0.12 MeV 0 2 4 6 8 10 12 14 16 18 0 1 2 3 4 d p a L, mm TiO2-2 E = 4 MeV Fig. 8. Profile of the displacements formation in TiO2-2 sample at helium ions irradiation with E = 4 MeV As follows from the spent calculations the phonons formation occurs in areas of ionization, segregation and vacancies formation; ionization occurs basically before phonons formation, segregation and vacancies for- mation. Since samples at irradiation are earthed and electrons mobility more than in 5000 times more ions mobility the ionization area will be positively charged. Hence, the accelerated ions irradiation leads to for- mation of a considerable quantity of radiating defects in a thin surface layer of a substance and causes change of the chemical composition of this layer as at the expense of ions penetration (an ion-implantation doping), and at the expense of change of the chemical elements concen- tration which are a part of targets (if they consist of two or more components). Formation of radiating defects and chemical composition change stimulate passing of secondary processes [7], such as formation of new crys- tal phases, amorphous layers, micro voids and etc. From the spent calculations follows that energy ex- pended for the ionization in samples volume is equal ≈ 94% for 0.12 MeV and 99.7% for 4 MeV and occurs mainly at the expense of helium ions. Formation of va- cancies and phonons take place mainly at the expense of displacement cascades. As a segregation occurs mainly after ionization process and electrons mobility is a min- imum in 5·10 3 times above ions mobility, there is a po- larization of the redistributed atoms in a sample volume with their following acceleration. This process changes electrophysical, thermalphysic and other characteristics of irradiated samples. Phonons formation at samples irradiation create an additional excitation collective mode, it results as in change of some characteristics of irradiated samples. All these effects as it will be shown below, lead to blistering and flaking formation both on an irradiated surface, and on the back (not irradiated) side of samples. 3. SPUTTERING RATIOS For calculations of sputtering ratios also the SRIM program has been used which with adequate accuracy considering the displacement cascades, counts sputter- ing ratios of the all atoms of TiO2-2 ceramics structure. Since for sputtering the cascades which come back to a target surface are important for a sputtering calculation the small surface layer of a sample is enough to use. The necessary thickness of samples for calculations was estimated at start some fast examples and, having looked on what depth efficiency of a sputtering remains to a constant, this value selected. For cascades in a tar- get at very low energy which is a sputtering major fac- tor, the SRIM a hard-sphere model for scattering uses. For definition of an optimum quantity of helium ions at calculation of atoms sputtering of TiO2-2 samples the calculations in the SRIM program are made at doses to 9∙10 6 particles. The sufficient number of helium ions for calculations in the SRIM program makes ≈ (3…5)∙10 6 for energies 0.12 and 4 MeV. The scheme of calcula- tions in the SRIM program is presented in Fig. 9 (with indication of an entry angle of helium ions beam in a sample). Fig. 9. Scheme for calculations in the SRIM program In the beginning calculations for TiO2-2 have been carried out at α = 0°. Change of a total sputtering ratio on a sample depth for energy of helium ions beam of 100 ISSN 1562-6016. Problems of Atomic Science and Technology. 2023. № 4(146) 4 MeV is shown in Fig. 10. The same calculations have been made for Е = 0.12 MeV. 0 10 20 30 40 50 60 70 80 90 100 0 5 10 15 20 25 30 35 E = 4 MeV k , 1 0 -5 a to m /i o n L, Ang. TiO2-2 Fig. 10. Change of a total sputtering ratio on TiO2-2 sample depth for energy of helium ions beam of 4 MeV Change of sputtering ratios O and Ti, basic ele- ments, is resulted in Fig. 11. The contribution to a total sputtering ratio of TiO2-2 other elements is less 1%. 0 10 20 30 40 50 60 70 80 90 100 0 5 10 15 20 25 k , 1 0 -5 a to m /i o n L, Ang. O Ti TiO2-2 E = 4 MeV Fig. 11. Change of sputtering ratios O and Ti on TiO2-2 sample depth for energy of helium ions beam of 4 MeV Sputtering occurs when the cascade of displacement atoms gives to a target atom the energy exceeding the surface binding energy (≈ 3.5 еV). That there would be a sputtering, the atom energy directed perpendicularly to a sample surface should be above surface energy. Hence, for sputtering only displacement cascades which come back to a target surface are important. For helium ions energy of 0.12 and 4 MeV, at α = 0°, total sputtering ratios are following: k ≈ 83·10 –5 atom/ion, E = 0.12 MeV; k ≈ 0.1·10 –5 atom/ion, E = 4 MeV. However, in process of a dose set a sample the target becomes rough, efficiency of a sputtering will increase, as each surface atom is connected with a surface smaller electron quantity. Calculation of a sputtering at α = 0° does not include effects of a roughness change which changes in time irradiation. At change of a surface bind- ing energy, a sputtering efficiency will increase no more than in 2 times regardless of a fact that occurs with irra- diated surface. At TiO2-2 irradiation on the linear accelerator of he- lium ions with energies of 0.12 and 4 MeV a surface change occurs, at the expense of a blistering and flaking formation, and as a result of structure atoms of samples sputtering also. So, after TiO2-2 irradiation the surface micrographs have been made. A surface structure of TiO2-2 irradiated sample is resulted in Fig. 12. After irradiated sample micrographs processing the dependence of a roughness along of TiO2-2 surface has been received (Fig. 13). Fig. 12. TiO2-2 surface structure. Е = 0.12 MeV, an irradiation dose was ≈ 1.2∙10 18 ion/cm 2 0 10 20 30 40 50 0 1 2 3 4 5 h , A n g . L, mm Fig. 13. Dependence of a roughness of TiO2-2 irradiated sample on a length of its surface. Е = 0.12 MeV, an irradiation dose was ≈ 1.2∙10 18 ion/cm 2 From the resulted data (see Figs. 12, 13) it’s visible that a surface is non-uniform, have a developed relief, the hollows maximum depth is no more than 5 Å. And with relief change of samples surface at an irradiation the entry angle of helium ions changes and the sputter- ing ratio of TiO2-2 elements can change. At calculations in the SRIM program these facts have been considered by means of ions entry angle change in irradiated sam- ples and the hollows maximum depth. In Table 5 values of TiO2-2 sputtering ratios are re- sulted at entry angles of helium ions beam of 0…90° and the maximum value of the hollows depth of 5 Å. Table 5 TiO2-2 total sputtering ratios at E = 0.12 МeV and E = 4 МeV k·10 –2 atom/ion, E = 0.12 МeV α° 0 6 12 18 24 30 36 42 k 1.9 1.92 1.93 2.25 2.26 2.24 2.23 2.20 α° 48 54 60 66 72 78 84 89 k 2.18 2.42 2.39 2.63 3.15 3.88 6.01 29.2 k·10 –5 atom/ion, E = 4 МeV α° 0 6 12 18 24 30 36 42 k 82.7 82.9 82.0 98.2 99.7 98.2 97.2 95.1 α° 48 54 60 66 72 78 84 89 k 92.7 103 102 111 137 165 255 1183 The dependences of the total sputtering ratios change on an entry angle of helium ions beams taking into account the hollows maximum depth of 5 Å and ion range of 100 Å are resulted in Figs. 14, 15. ISSN 1562-6016. Problems of Atomic Science and Technology. 2023. № 4(146) 101 The range of sputtering ratios changes at α = 0…90° has made: E = 0.12 MeV, k = (1.9…29.2)∙10 –2 atom/ion; E = 4 MeV, k = (83…1183)∙10 –5 atom/ion. Average values of total sputtering ratios, disregard- ing extreme values, that is at α = 0° and α = 90°, are following: E = 0.12 MeV, k = 2.6·10 –2 atom/ion; E = 4 MeV, k = 114·10 –5 atom/ion. Since at calculations the maximum hollows depth was used the averaging sputtering ratios on hollows depth is received: E = 0.12 MeV, k = 1.3·10 –2 atom/ion; E = 4 MeV, k = 57·10 –5 atom/ion. We consider that it’s the greatest possible sputtering ratios at E = 0.12 and E = 4 MeV. 0 10 20 30 40 50 60 70 80 2 3 4 5 6 k , 1 0 -2 a to m /i o n α, degree TiO2-2 EHe+ = 0.12 MeV Fig. 14. Dependence of a total sputtering ratio on an entry angle of helium ions with E=0.12 МeV in TiO2-2 sample 0 10 20 30 40 50 60 70 80 80 100 120 140 160 180 200 220 240 260 k , 1 0 -5 a to m /i o n α, degree TiO2-2 EHe+ = 4 MeV Fig. 15. Dependence of a total sputtering ratio on an entry angle of helium ions with E = 4 МeV in TiO2-2 sample 4. EFFECTS OF TiO2-2 METALLIZATION AND LONG-RANGE INTERACTION, ELECTROPHYSICAL CHARACTERISTICS AND SWELLING We develop such experimental techniques of re- searches: microscopic, measurements of electrophysical characteristics and frictional parameters of ceramic ma- terials, ultrasonic researches. The technique of ceramic materials researches is fol- lowing. After set a sample of an irradiation certain dose the microscopic researches are conducted which allow to study the blistering and flaking formations and their change dynamics from an irradiation dose and tempera- ture, dimensional stability (swelling, sintering), grains size changes, to investigate a surface roughness and to study influence of dusting processes of various materi- als at an irradiation on the blistering and flaking dynam- ics. For finding-out of a metallization effect formation in irradiated samples TiO2-2 irradiation on the linear ac- celerator of helium ions with energy of 0.12 MeV has been made. The irradiation dose has made ~1.2∙10 18 ion/cm 2 , a temperature was ≈ 60°С. The ob- served effect of a surface metallization of TiO2-2 sam- ple irradiated surface is shown in Fig. 16. The surface linear profile in the metallization area of TiO2-2 irradiated sample in a red spectrum is shown in Fig. 17. Fig. 16. Metallization surface of the irradiated sample 0 1 2 3 4 5 6 7 8 9 10 11 160 170 180 190 200 210 220 230 240 250 260 In te n si ty , re la ti v e u n it s L, mm Red spectrum Metallization area Fig. 17. Spectrum of TiO2-2 surface in the metallization field after irradiation by helium ions with Е = 0.12 MeV It’s possible to explain metallization effect TiO2 dis- sociation with the subsequent of titan and oxygen diffu- sion to a sample surface. At an irradiation of TiO2-2 sample by helium ions with energy of 4 MeV a surface metallization was not revealed. As the segregation of TiO2-2 elements at energy of 4 MeV is maximum on depth of 14…18 mm (see Fig. 6), and at Е = 0.12 MeV a segregation maximum is located on a depth 0.1…1.1 mm (see Fig. 5) for revealing of a surface met- allization, it’s necessary to increase an irradiation dose and an irradiation to spend at more high temperature. Under existing conditions of an irradiation (Е = 4 MeV), it’s necessary to expect that owing to TiO2 dissociation in an irradiated sample volume the electro- physical characteristics will change. After samples irradiation by helium ions a certain dose with energy of 4 MeV the surface electroresistanc- es of a front side and a back side of samples, the volume electroresistance were measured, the microscopic re- searches on optical and electronic microscopes were conducted. After measurements there was a further irra- diation of these samples with subsequent measurements. Surfaces of the front side (irradiated) and the back side (not irradiated) of TiO2-2 sample are resulted in Figs. 18, 19. A dose of an irradiation was ~1.2∙10 18 ion/cm 2 , a temperature was ≈ 60°С. 102 ISSN 1562-6016. Problems of Atomic Science and Technology. 2023. № 4(146) From the photos made on optical and electronic mi- croscopes, it’s visible that the surface is non-uniform, has the developed relief on which concentric traces from an ionic beam and craters, splashes of a sample material and metallization area with small grains are looked. Fig. 18. Front side of TiO2-2 irradiated sample (Е = 4 MeV) Fig. 19. Back side of TiO2-2 irradiated sample (Е = 4 MeV) The flaking formation both on the front side and on the back side of a sample is clearly visible. The blister- ing formation on the front side and the back side of the irradiated samples is not observed. The flaking filling ratios k=S/S0, where S is a surface area of a sample, flaking occupied; S0 is the irradiated front side or back side of a sample have been calculated. Dependences of the flaking filling ratios from an irradiation dose are shown in Fig. 20. 0.0 0.5 1.0 1.5 2.0 2.5 3.0 0.0 0.1 0.2 0.3 0.4 0.5 face side of the sample reverse side of the sample 17 2D 10 , ion / cm k TiO2-2 Fig. 20. Dependences of the flaking filling ratios from an irradiation dose of the front side and the back side of TiO2-2 sample From Fig. 20 follows that at an irradiation dose of ~1∙10 17 ion/cm 2 , the surface areas values of a flaking formation practically coincide. However, the flaking depth on the front side of a sample is approximately twice more than on the back side. More careful re- search, further, will be given this point in a question. After each irradiation gathered dose the surface and volume electroresistances have been measured. These dependences on an irradiation dose are resulted in Figs. 21, 22, accordingly. Initial values of the surface and volume electroresistances of not irradiated samples are indicated on figures. From the mentioned results follows that electrore- sistance change, both on the front side and on the back side of TiO2-2 sample, occurs owing to basic elements dissociation. It’s necessary to notice that after each irra- diation session the exposure of samples was made. Then the surface and volume electroresistances were meas- ured. Partial restoration of the electroresistance no more than 5% has been registered. From the mentioned results on measurements of the flaking change and electroresistance follows that there is an effect of the long-range interaction. To experi- mental and theoretical researches of this effect are de- voted numerous works [20 - 24]. However, for today there is no unambiguous mechanism explaining this effect. In our opinion, it’s possible to explain effect of the long-range interaction by complex action on a sam- ple surface, namely, generation of thermoelastic ten- sions and shock waves, at the expense of the formation and distribution phonons and stimulating diffusion of impurities, as on interstices, and to borders of grains. 0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0 0 5 10 15 200 220 240 260 280 300 320 340 R S u rf ac e (M Ω /c m ) D∙1018, ion/cm2 front side backside TiO2-2 E= 4 MeV Fig. 21. Dependences of TiO2-2 surface electrore- sistance on an irradiation dose. Initial value was 20 GΩ/сm (on the front and back sides of a sample) 0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0 0 500 1000 1500 2000 2500 3000 3500 4000 R V o lu m e (M Ω /c m 3 ) D∙1018, ion/cm2 TiO2-2 E= 4 MeV Fig. 22. Dependence of TiO2-2 volume electroresistance on an irradiation dose. Initial value was 50 GΩ/cm 3 Fig. 23. Front surface of TiO2-2 sample ISSN 1562-6016. Problems of Atomic Science and Technology. 2023. № 4(146) 103 As at TiO2-2 irradiation at a dose of ~1∙10 18 ion/cm 2 a swelling of a sample material was revealed. The photo of a sample front surface is resulted in Fig. 23. The sample right part is not irradiated surface; left part is the irradiated surface. Analysis has shown that a swelling value is order of 1 mm, at an irradiation dose of ~1∙10 18 ion/сm 2 . A swell- ing is connected with diffusion of gaseous elements (Не, О) to a surface at the expense of internal bubbles formation and grains growth. CONCLUSIONS On the linear accelerator the irradiation of TiO2-2 samples by helium ions with energies of 0.12 and 4 MeV is spent. For these energies the ionization pro- files, formation of vacancies and phonons, redistribution of sample atoms and damageability are calculated. Also sputtering ratios taking into account change of a surface samples profile are calculated. At Е = 0.12 MeV more than 94% of energy goes on the ionization, an order of 5% on the phonons formation and less than 0.3% on a damageability. For Е = 4 MeV, more than 99.7% of energy goes on the ionization, an order of 0.2% on the phonons formation and less than 0.02% on a damageability. Therefore, damageability for Е = 0.12 MeV makes 49 displacements/atom, for Е = 4 MeV is 5.0 displacements/atom. Taking into account the displacement cascades the sputtering ratios of all atoms of TiO2-2 ceramics struc- ture have been calculated. Nonmetering of samples pro- file change, for energy of helium ions of 0.12 and 4 MeV, at an entry angle in samples α = 0°, the total sputtering ratios are following: k ≈ 83·10 –5 atom/ion, E = 0.12 MeV; k ≈ 0.1·10 –5 atom/ion, E = 4 MeV. Tak- ing into account change of samples profile for the entry angles of 0…90° the average sputtering ratios have made: E = 0.12 MeV, k = 1.3·10 –2 atom/ion; E = 4 MeV, k = 57·10 –5 atom/ion. After TiO2-2 irradiation the microscopic researches of the front side (irradiated) and the back side (not irra- diated) of a sample have been conducted. The metalliza- tion effect on the front side of a sample (E = 0.12 MeV) which is possible to explain for the account TiO2 disso- ciation with the subsequent diffusion of the titan to a sample surface is revealed. At E = 4 MeV the metalliza- tion effect was not found. This results from the fact that the segregation of TiO2-2 elements at energy of 4 MeV is located on a depth of 14…18 mm, and at Е = 0.12 MeV the segregation profile is located on a depth of 0.1…1.1 mm. For revealing of surface metalli- zation it’s necessary to increase an irradiation dose and an irradiation to spend at more high temperature. Also at TiO2-2 irradiation at an irradiation dose of ~1∙10 18 ion/cm 2 swelling of a sample material was re- vealed which is connected with diffusion of gaseous elements (Не, О) to a surface at the expense of internal bubbles formation and grains growth. An effect of the long-range interaction is defined by change (reduction) of the surface electroresistance both on the front side of a sample, and on the back side. Also the volume electroresistance decreases at increase of an irradiation dose. Besides, on both sides the flaking for- mation is observed. And, the flaking areas on the front side and back side of a sample increase with increase of an irradiation dose. It’s possible to explain reduction of the surface and volume electroresistances TiO2 dissocia- tion. That is in all volume of an irradiated sample there is a metal (Ti), only it leads to electroresistance reduc- tion. But there is a question, whence takes energy on the back side of a sample for the formation flaking and TiO2 dissociation? TiO2 binding energy an order of 12…15 eV, a thickness of a sample is ≈ 1 mm, and the helium ions range and primary processes formation area are no more than 18.5 mm. In our opinion, it’s possible to explain a complex influence. First, the phonon excit- ed propagation with additional frequency mode for- mation from helium ions beam. This energy has enough for TiO2 dissociation and tensions formation on the back side of a sample. Secondly, in a sample ionization area the positive charge accumulates, under Coulomb field action there is a polarization of the segregation atoms and structure molecules. This energy has enough for acceleration of segregation atoms and structure mole- cules with formation of the cyclic primary processes. The essential role at the flaking formation is played by oxygen and helium diffusion. With increase of an irra- diation dose appear diffused channels for oxygen and helium directly in the areas of the flaking formation (Fig. 24). Fig. 24. Flaking formation with diffused channels REFERENCES 1. H. Ullmaier. The influence of helium on the bulk properties of fusion reactor structural materials // Nuclear fusion. 1984, v. 24, № 8, p. 1039-1083. 2. J. Wesson. Tokamaks: 3rd ed. Oxford: Clarendon Press, 2004, 749 p. 3. ITER physics basis, Nuclear Fusion. 1999, v. 39, № 12. 4. V. Shakhnov, L. Zinchenko, I. Kosolapov, I. Filippov. Modeling and optimization of radiation tolerant microsystems // Proc. EMS'14. 2014, p. 484-489. 5. V.A. Belous, G.I. Nosov, N.А. Аzarenkov. About influence of an irradiation by ions Ar+ on corrosion resistance of metals and alloys // Surface Physical Engineering. 2010, v. 8, № 2, p. 161-168. 6. K.V. Kosterin. Sputtering of solids by ionic bom- bardment: adatomic mechanisms and a possible role phonons // Physics and Chemistry of Materials Pro- cessing. 1995, № 3, p. 43-48. 7. L.B. Begrambekov. Updating of solids surface at ionic and plasma influence. M.:“МERI”, 2001, 34 p. 104 ISSN 1562-6016. Problems of Atomic Science and Technology. 2023. № 4(146) 8. V.О. Bomko, О.F. Dyachenko, O.M. Yegorov, et al. Development of investigations on the MILAC heavy ion linear accelerator // Proc. of the LINAC08, Van- couver, Victoria, Canada. 2008, p. 187-189. 9. S.N. Dubniuk, R.A. Anokhin, A.F. Dyachenko, et al. Radiation complex on the basis of helium ions linac // Problems of Atomic Science and Technology. Se- ries “Plasma Electronics and New Methods of Ac- celeration”. 2018, № 4, p. 46-51. 10. A.F. Dyachenko. Interdigital structures of heavy ions linear accelerators: their tuning, beams focusing and use (review) // Problems of Atomic Science and Technology. Series “Nuclear Physics Investiga- tions”. 2019, № 6, p. 17-22. 11. V.O. Bomko, O.F. Dyachenko, Ye.V. Ivakhno, et al. New prestripping section of the MILAC linear ac- celerator designed for accelerating a high current beam of light ions // Proc. of the EPAC 2006 Edin- burgh, Scotland. 2006, p. 1627-1629. 12. V.O. Bomko, A.F. Dyachenko, B.V. Zajtsev, et al. Inductance-capacitor system for tuning of interdigi- tal structure of the ion linear accelerator // Problems of Atomic Science and Technology. Series “Nuclear Physics Investigations”. 2007, № 5, p. 180-183. 13. V.O. Bomko, O.F. Dyachenko, Ye.V. Ivakhno, et al. Adjustment of a new pre-stripping section the mul- ticharge ion linear accelerator (MILAC) // Proc. of the 11-th European Particle Accelerator Conference EPAC08, Genoa, Italy. 2008, p. 3410. 14. R.A. Anokhin, B.V. Zaitsev, K.V. Pavlii, et al. Ex- perimental complex for investigation of construction materials on the helium ions linear accelerator // Problems of Atomic Science and Technology. Series “Nuclear Physics Investigations”. 2017, № 6, p. 167-171. 15. R.A. Anokhin, S.N. Dubniuk, A.F. Dyachenko, et al. Beam and target parameters measurement system on helium ions linear accelerator // Problems of Atomic Science and Technology. Series “Plasma Electron- ics and New Methods of Acceleration”. 2018, № 4, p. 30-35. 16. A.F. Dyachenko, R.A. Anokhin, S.N. Dubniuk, et al. The bunch formation and transport system to the target of the helium ions linac // Problems of Atomic Science and Technology. Series “Plasma Electro- nics and New Methods of Acceleration”. 2018, № 4, p. 52-55. 17. A.F. Dyachenko. The high-sensitivity induction gauge of a beam current of heavy ions linear accel- erator // The Journal of Kharkiv National University. Physical Series “Nuclei, Particles, Fields”. 2010, v. 1(45), № 887, p. 118-121. 18. http://www.srim.org. 19. B. Widrow, J.R. Glover, J.M. McCool, et al. Adap- tive noise cancelling: principles and applications // Proc. IEEE, 63, p. 1692-1716. 20. Yu.P. Sharkeev, E.V. Kozlov, A.N. Didenko, et al. The mechanisms of the long-range effect in metals and alloys by ion implantation // Surface and Coat- ing Technology. 1996, v. 83, p. 15-21. 21. Yu.V. Martynenko. Effects of long-range interaction at ionic implantation // Results of science and tech- nics. М., 1993, v. 7, p. 82-112. 22. P.V. Pavlov, Е.С. Demidov, V.V. Karzanov. Effect of long-range interaction in the silicon crystals al- loyed by iron, depending on a dose and intensity of an irradiation argon ions // Proc. of 9th All-Union conference “Interaction of nuclear particles with solid”. М.: “МERI”, 1989, v. 2, p. 84. 23. D.I. Tetelbaum, V.Ya. Bayankin. Effect of long- range interaction // Nature. 2005, № 4, p. 9-17. 24. V.Ya. Bayankin, М.I. Guseva, D.I. Tetelbaum, F.Z. Gilmutdinov. Segregation as demonstration of long-range interaction effect at an irradiation boron ions of the foils of permalloy-79 and Сu-Ni alloys // Surface. X-ray, synchrotron and neutron resear- ches. 2005, № 5, p. 77-81. Article received 28.05.2023 РАДІАЦІЙНІ ПОШКОДЖЕННЯ TiO2-2 У РЕЗУЛЬТАТІ ОПРОМІНЕННЯ НА ЛІНІЙНОМУ ПРИСКОРЮВАЧІ ІОНАМИ ГЕЛІЮ З ЕНЕРГІЯМИ 0.12 І 4 МeВ B.І. Бутенко, A. Cenian, О.Ф. Дьяченко, О.В. Мануйленко, К.В. Павлій, M. Sawczak, Б.B. Зайцев, В.І. Журба На лінійному прискорювачі іонів гелію виконано опромінення зразків TiO2-2 з енергією іонів 0,12 і 4 МеВ до доз ≈ 1∙10 18 іон/см 2 . Елементний склад зразків TiO2-2 отримано рентгенофлюоресцентним мето- дом. Після опромінення проведено мікроскопічні дослідження на електронному та оптичному мікроскопах, досліджено змінення електрофізичних характеристик. Зроблено числові розрахунки коефіцієнтів розпилен- ня атомів з урахуванням кутів входу іонів гелію в зразок, а також утворення фононів, перерозподілу атомів (сегрегація), утворення вакансій і зміщень у зразкa TiO2-2. Досліджено процеси утворення флекінгу та пока- зано наявність ефектів металізації й далекодії в опромінених зразках. http://www.srim.org/
id nasplib_isofts_kiev_ua-123456789-196183
institution Digital Library of Periodicals of National Academy of Sciences of Ukraine
issn 1562-6016
language English
last_indexed 2025-12-07T17:38:12Z
publishDate 2023
publisher Національний науковий центр «Харківський фізико-технічний інститут» НАН України
record_format dspace
spelling Butenko, V.I.
Cenian, A.
Dyachenko, O.F.
Manuilenko, O.V.
Pavlii, K.V.
Sawczak, M.
Zajtsev, B.V.
Zhurba, V.I.
2023-12-11T11:57:26Z
2023-12-11T11:57:26Z
2023
TiO₂-2 radiating damages as a result of the irradiation helium ions with energies of 0.12 and 4 MeV on the linear accelerator / V.I. Butenko, A. Cenian, O.F. Dyachenko, O.V. Manuilenko, K.V. Pavlii, M. Sawczak, B.V. Zajtsev, V.I. Zhurba // Problems of Atomic Science and Technology. — 2023. — № 4. — С. 96-104. — Бібліогр.: 24 назв. — англ.
1562-6016
PACS: 29.17+w, 29.27 Bd
DOI: https://doi.org/10.46813/2023-146-096
https://nasplib.isofts.kiev.ua/handle/123456789/196183
On the linear accelerator of helium ions, the irradiation of TiO₂-2 samples with ions energy of 0.12 and 4 MeV to doses of ≈ 1∙10¹⁸ ion/cm² is executed. The elemental composition of TiO₂-2 samples is made by roentgen-fluorescence method. After irradiation a change of electrophysical characteristics is investigated, microscopic researches on electronic and optical microscopes are conducted. Numerical calculations of atom sputtering ratios taking into account of input angles of helium ions in a sample, and also phonons formation, atoms redistribution (segregation), appearance of the vacancies and displacements in TiO₂-2 sample are made. Processes of the flaking formation are investigated, and also presence of the metallization effect and long-range interaction effect in the irradiated samples is shown.
На лінійному прискорювачі іонів гелію виконано опромінення зразків TiO₂-2 з енергією іонів 0,12 і 4 МеВ до доз ≈ 1∙10¹⁸ іон/см². Елементний склад зразків TiO₂-2 отримано рентгенофлюоресцентним методом. Після опромінення проведено мікроскопічні дослідження на електронному та оптичному мікроскопах, досліджено змінення електрофізичних характеристик. Зроблено числові розрахунки коефіцієнтів розпилення атомів з урахуванням кутів входу іонів гелію в зразок, а також утворення фононів, перерозподілу атомів (сегрегація), утворення вакансій і зміщень у зразкa TiO₂-2. Досліджено процеси утворення флекінгу та показано наявність ефектів металізації й далекодії в опромінених зразках.
en
Національний науковий центр «Харківський фізико-технічний інститут» НАН України
Problems of Atomic Science and Technology
Ion beam dynamics
TiO₂-2 radiating damages as a result of the irradiation helium ions with energies of 0.12 and 4 MeV on the linear accelerator
Радіаційні пошкодження TiO₂-2 у результаті опромінення на лінійному прискорювачі іонами гелію з енергіями 0.12 і 4 МeВ
Article
published earlier
spellingShingle TiO₂-2 radiating damages as a result of the irradiation helium ions with energies of 0.12 and 4 MeV on the linear accelerator
Butenko, V.I.
Cenian, A.
Dyachenko, O.F.
Manuilenko, O.V.
Pavlii, K.V.
Sawczak, M.
Zajtsev, B.V.
Zhurba, V.I.
Ion beam dynamics
title TiO₂-2 radiating damages as a result of the irradiation helium ions with energies of 0.12 and 4 MeV on the linear accelerator
title_alt Радіаційні пошкодження TiO₂-2 у результаті опромінення на лінійному прискорювачі іонами гелію з енергіями 0.12 і 4 МeВ
title_full TiO₂-2 radiating damages as a result of the irradiation helium ions with energies of 0.12 and 4 MeV on the linear accelerator
title_fullStr TiO₂-2 radiating damages as a result of the irradiation helium ions with energies of 0.12 and 4 MeV on the linear accelerator
title_full_unstemmed TiO₂-2 radiating damages as a result of the irradiation helium ions with energies of 0.12 and 4 MeV on the linear accelerator
title_short TiO₂-2 radiating damages as a result of the irradiation helium ions with energies of 0.12 and 4 MeV on the linear accelerator
title_sort tio₂-2 radiating damages as a result of the irradiation helium ions with energies of 0.12 and 4 mev on the linear accelerator
topic Ion beam dynamics
topic_facet Ion beam dynamics
url https://nasplib.isofts.kiev.ua/handle/123456789/196183
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