Radioluminescence degradation of scintillators on a basis of polystyrene and poly-2,4-dimethylstyrene, the ways of their radiating stability increasing

Spectra of radioluminescence of plastic scintillators on a basis of polystyrene and poly-2,4-dimethylstyrene under
 an influence of γ-radiation are obtained. It is shown that the most effective quenchers are macroradicals, on
 which a transmission of excitation energy from “initial”...

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Опубліковано в: :Вопросы атомной науки и техники
Дата:2006
Автори: Voronkina, N.I., Senchyshyn, V.G., Milinchuk, V.K., Sheluhov, I.P.
Формат: Стаття
Мова:Англійська
Опубліковано: Національний науковий центр «Харківський фізико-технічний інститут» НАН України 2006
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Цитувати:Radioluminescence degradation of scintillators on a basis of polystyrene and poly-2,4-dimethylstyrene, the ways of their radiating stability increasing / N.I. Voronkina, V.G. Senchyshyn, V.K. Milinchuk, I.P. Sheluhov // Вопросы атомной науки и техники. — 2006. — № 3. — С. 145-147. — Бібліогр.: 4 назв. — англ.

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Digital Library of Periodicals of National Academy of Sciences of Ukraine
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author Voronkina, N.I.
Senchyshyn, V.G.
Milinchuk, V.K.
Sheluhov, I.P.
author_facet Voronkina, N.I.
Senchyshyn, V.G.
Milinchuk, V.K.
Sheluhov, I.P.
citation_txt Radioluminescence degradation of scintillators on a basis of polystyrene and poly-2,4-dimethylstyrene, the ways of their radiating stability increasing / N.I. Voronkina, V.G. Senchyshyn, V.K. Milinchuk, I.P. Sheluhov // Вопросы атомной науки и техники. — 2006. — № 3. — С. 145-147. — Бібліогр.: 4 назв. — англ.
collection DSpace DC
container_title Вопросы атомной науки и техники
description Spectra of radioluminescence of plastic scintillators on a basis of polystyrene and poly-2,4-dimethylstyrene under
 an influence of γ-radiation are obtained. It is shown that the most effective quenchers are macroradicals, on
 which a transmission of excitation energy from “initial” luminescent additives occurs. The ways to increase PS radiating
 stability are proposed. Получены спектры радиолюминесценции пластмассовых сцинтилляторов на основе полистирола и поли-2,4-диметилстирола при воздействии на них γ-излучения. Показано, что наиболее эффективными тушителями являются макрорадикалы, на которые происходит перенос энергии возбуждения с первичной люминесцирующей добавки. Предложены способы повышения радиационной стойкости ПС. Одержано спектри радіолюмінесценції пластмасових сцинтиляторів на основі полістиролу та полі-2,4-
 диметилстиролу під дією γ-випромінювання. Показано, що найбільш ефективними гасниками є
 макрорадикали, на які відбувається перенос енергії збудження з первинної люмінесціючої домішки.
 Запропоновано способи підвищення радіаційної стійкості ПС.
first_indexed 2025-12-07T17:32:29Z
format Article
fulltext RADIOLUMINESCENCE DEGRADATION OF SCINTILLATORS ON A BASIS OF POLYSTYRENE AND POLY-2,4-DIMETHYLSTYRENE, THE WAYS OF THEIR RADIATING STABILITY INCREASING N.I. Voronkina, V.G. Senchyshyn, V.K. Milinchuk, I.P. Sheluhov Institute for scintillation materials NANU E-mail: sench@isc.kharkov.com Spectra of radioluminescence of plastic scintillators on a basis of polystyrene and poly-2,4-dimethylstyrene un- der an influence of γ-radiation are obtained. It is shown that the most effective quenchers are macroradicals, on which a transmission of excitation energy from “initial” luminescent additives occurs. The ways to increase PS radi- ating stability are proposed. PACS: 29.40.Mc 1. INTRODUCTION It is known that many factors have an influence on decrease of the plastic scintillators (PS) light output due to ionizing radiations; these factors are: type and rate of radiation, temperature, environment, etc. Therefore, it is difficult to compare data on PS radiation resistance giv- en in literature. Besides, different authors give values of PS light output change, measured after different time since the termination of irradiation. "Post-radiation" transformation can occur to some extent in scintillators in that period [1]. In order to estimate the influence of radiation on PS scintillation properties more correctly, degradation of PS radioluminescence (RL) from the absorbed doze is investigated in present work on radioluminescence spec- tra which were registered under continuous γ-irradiation by a specially created installation. The installation consists of a drum with samples, placed near 60Co-source (60,000 g-equivalent radium ac- tivity, the absorbed doze rate being 3 Gy/s.) in canyon; systems of fibers transmitting scintillation signal from the sample on photomultiplier-100, located behind a lead shield; systems of device communication SKVU- 100 from the PC. Concentration of macroradicals was determined by EPR spectra, spectra of absorption with the help of "Specord-M40" spectrophotometer. 2. RESULTS AND DISCUSSION As active additives p – diphenyl phenylene (РТ) of 2% mass and 1,4-di/2-(5-fenyloxazolyl)/benzene (РО- РОР) of 0,1% are used in them. Series of samples of various structures have been measured. Degradation of radioluminescence was estimated on curves of spectra relative intensity dependence on the absorbed doze (Fig.2). (PBD – 2-(4-diphenylyl)-5-phenyl-oxazole- 1,3,4; TPB 1,1,4,4 – especially if one takes into account smaller density of tetraphenylbutadiene; MBD – 2- metyl-5(p-diphynylyl)-oxadiazole-1,3,4). Apparently, this dependence has a complex charac- ter and depends on PS structure and γ -irradiation doze. It is established that RL degradation is strongest at dozes up to 40 kGy. For larger absorbed dozes, the curves of degradation of PS with various luminescent additives (LA) differ insignificantly but depend on a polymeric matrix nature. PS based on poly-2,4- dimethylstyrene show more radiation resistance than that on the basis of polystyrene with the same LA. Fig.1. Curves of degradation of scintillation composi- tions radioluminescence: p-dmst (1, 2) and pst (3, 4, 5): 1 – PBD(5%)+POPOP(0,1%); 2 - PT(2%)+POPOP(0,1%); 3 - PT(2%)+POPOP(0.1%); 4 - PBD(2%)+TPB(0.1%); 5 – MBD(2%)+POPOP(0.1%) Mechanisms of radiochemical processes resulting in damages of polymers and scintillators on their basis have been already investigated. It has been shown that primary products formed by radiolysis (ions, ions - radi- cals, short-lived radicals, and captured electron) turn into long-living (about several months) macroradicals under the action of temperature and light quanta. It was revealed that basically macroradicals with a broken chain (an end radical Re) are stabilized in polystyrene, and alkyl-type macroradicals of "middle" type are in p- 2,4-dmst [2, 3]. During the research of absorption spectra of the irra- diated polymers we observed an increase in optical den- sity in the 310…350 nm range. The comparison of de- pendences of paramagnetic centers accumulation, the increase in optical density and intensity of luminescence from the absorbed doze, and also a symbate decrease of these parameters during the "post-radiating" period have allowed identification of the strips of absorption caused by various macroradicals. Apparently, absorption of macroradicals lies in the field of luminescence of initial LA and in the field of absorption of secondary LA. Thus, the probability of transmission of energy of elec- tronic excitation (TEE) from initial LA on macroradi- cals instead of secondary LA is large. According to known Ferster-Galanin's formulas TEE calculations in the investigated polymeric systems have been carried out taking into account products of radioly- sis. kdd( R ) = 1/τ0D(R0/R)6, ____________________________________________________________ PROBLEMS OF ATOMIC SCIENCE AND TECHNOLOGY. 2006. № 3. Series: Nuclear Physics Investigations (47), p. 145-147. 145 mailto:sench@isc.kharkov.com ∫ −= νννεν π dI Nn qФR A u D D 4 45 0 26 0 )()( 128 10ln9000 . Table 1. Absorption spectra of macroradicals in PST and p-2,4-dmst Polymer λmax ε, M-1,sm-1 Polystyrene 316. (e) 328.344 (m) 470.522 104 ~130 Poly-2,4- dimethylstyrene 330-340 (m) 482 2·103 ~200 Table 2. Calculated average critical radii of elec- tronic excitation energy transport in γ-irradiated PS Polystyrene Poly-2,4-dimethyl- styrene Donor Accep- tor Ro, Å Donor Accep- tor Ro, Å M* R. c, R. к 0,6 M* R. c, R. к 18,6 РТ R. к 22,3 РТ R. c 17,8 M* Op 28,2 M* Op 28,2 Op РТ 7,6 where M*− the excited macromolecule; Op − oxygen- containing products of radiolysis; qoD -− [4] As follows from the calculations, TEE from the ex- cited macromolecules of polystyrene effectively occurs in oxygen-containing products of radiolysis by the in- ductive - resonant mechanism. TEE on macroradicals occurs from initial LA. In p-2,4-dmst TEE on macrorad- icals effectively occurs both from the excited macro- molecules and from initial LA. The probability of TEE on macroradicals increases according to their accumulation with absorbed doze (τ0PT = 1.43⋅ns) [4]. As macroradicals have a competitive affect on exci- tation energy capture, it is logical to assume that the in- creasing of concentration of the initial additive will pro- mote the increase of PS radiation resistance Table 3. Dependence of speed constant of energy trans- fer from PT on macroradicals from a dose D, kGy CR ⋅103, M K⋅10-9, m-1⋅c-1 5 0.5 0.7 20 1.0 6.3 45 5.0 140.0 60 10.2 720.0 We have carried out an experiment with LA which is well dissolved in polystyrene. Apparently the depen- dence has maximum at 4…6% of weights; the further increase in concentration of the additive reduces in- creasing in a system degradation, probably because of concentrating quenching. A large role in formation and disappearance of macroradicals plays a molecular oxygen participating in intermediate reactions by the scheme: R. + О2 → ROO, ROO + HR → ROOH + R, ROO + R → products of radiolysis, R + R → products of radiolysis Results of researches on influence of the molecular oxygen dissolved in polymeric matrix are presented in [3]. The induction period, which we have found out in accumulation of macroradicals, indicates a positive role of О2 in preservation of stability of scintillation proper- ties. Reactions with the participation of oxygen are dif- fusion-limited and depend on the permolecular structure of matrix that is on the density of molecular balls and on the mobility of macrochains. After the expenditure of the oxygen dissolved in the polymeric matrix, there is an intensive accumulation of macroradicals with the si- multaneous diffusion of О2 from air with small speed D~1.5.10-9sm2s-1. For acceleration of the diffusion pro- cesses before the reaction of oxygen with macroradicals, we incorporated various plasticizers (stearin, palmitic, threedecan acids) into PS with a standard set of LA. We have received PS with substantial increasing of radia- tion resistance up to 30…40 kGy doze (Fig.2) under the investigated doze rate. At low doze rates the range of preservation of high radiation resistance will extend, if the velocity of radicals formation will be comparable to that of diffusion of О2 from air. To increase radiation resistance of PS irradiated by large dozes, we incorporate 10% of isopropyldiphenyl (IPD). Under ionizing radiation this combination easily forms radicals (it is less radiation-resistant than lumi- nescent additives), which recombine with macroradi- cals, thus protecting the polymer from destruction. The results, which prove such a protective mechanism, are shown in Fig.2. Interaction of radicals of isopropy- ldiphenyl with macroradicals of polystyrene proves to be true by comparison of luminescence spectra of super- precipitate samples of PS before and after γ-irradiation (Fig.2). Fig.2. Curves of degradation of scintillation composi- tions radioluminescence: 1) pst+PT(2%)+POPOP(0.1%)+IPD(10%); 2) pst+PT(2%)+POPOP(0,1%)+TDA (0.2%); 3) p-2,4-dmst+PT(2%)+POPOP(0.1%); 4)pst+PT(2%)+POPOP(0.1%) In fluorescence spectra of samples with IPD a typi- cal for biphenyl groups spectrum is observed, spectra are not found out in standard PS from this area, as dur- ing the superprecipitate luminescent additives are washed out from the polymer. Thus, we have proved that basic centers of PS radio- luminescence quenching are macroradicals, especially the end radical Re: ~CH2-C6H5-CH. Rather large radia- tion stability of PS based on p-2,4-dmst is explained by the fact that in p-2,4-dmst macroradicals of "middle" type are stabilized in a greater degree: ~CH2- C6H5(СН3)2-C~, which are conformationally more ac- cessible to reactions with oxygen and other radicals. 146 Fig.3. Spectra of fluorescence of γ-irradiated scintilla- tion compositions on the basis of polystyrene: 1 - PT(2%) + POPOP(0.1%) before superprecipitate; 2 – the same after superprecipitate; 3 - PT(2%)+POPOP(0.1%)+IPB(10%) after superpre- cipitate CONCLUSION The experimental data obtained and their interpreta- tion enable to draw the following conclusions regarding the increase in radiation resistance of polymeric scintil- lation compositions: 1. In the region of absorbed dozes up to 20… 30 kGy: - Selection of LA, which luminescence area is not blocked by the area of absorption of the formed macro- radicals; - Increasing of diffusion rate of molecular oxygen by plasticizer substances in optimal concentrations. 2. In the region of the absorbed dozes 40…100 kGy: - Increase in concentration of "initial" luminescent additive essentially exceeding concentration of macro- radicals formed at these dozes; - Introduction to PS structure of low-molecular com- binations, which during irradiation easily form radicals capable to recombination with incipient stable macro- radicals. REFERENCES 1. V.K. Milinchuk, E.R. Klinshpont, S.J. Pshezhetsky Macroradicals. M.: Chemistry, 1980. 2. V.B. Taraban, I.P. Shelukhov, G.S. Zhdanov, N.I. Voronkina. The role of macroradicals in the decreasing of the plastic scintillators radiation resis- tance // Radiat. Phys. Chem. 1995, v.46, №4-6, p.1321-1324. 3. N.I. Voronkina, O.A. Gunder, G.S. Zhdanov, V.K. Milinchuk. Radiation and photoradiation pros- esses in methyl derivatives of polystyrene and in scintillation compositions based on them // Func- tional materials. 1994, v.1, №1, p.118-127. 4. J.B. Berlman. Handbook of Fluorescence Spectra of Aromatic Molecules. N.Y.: “Acad. Press”, 1965. ДЕГРАДАЦИЯ РАДИОЛЮМИНЕСЦЕНЦИИ СЦИНТИЛЛЯТОРОВ НА ОСНОВЕ ПОЛИСТИРОЛА И ПОЛИ-2,4-ДИМЕТИЛСТИРОЛА, СПОСОБЫ ПОВЫШЕНИЯ ИХ РАДИАЦИОННОЙ СТОЙКОСТИ Н.И. Воронкина, В.Г. Сенчишин, В.К. Милинчук, И.П. Шелухов Получены спектры радиолюминесценции пластмассовых сцинтилляторов на основе полистирола и поли- 2,4-диметилстирола при воздействии на них γ-излучения. Показано, что наиболее эффективными тушителя- ми являются макрорадикалы, на которые происходит перенос энергии возбуждения с первичной люминес- цирующей добавки. Предложены способы повышения радиационной стойкости ПС. ДЕГРАДАЦІЯ РАДІОЛЮМІНЕСЦЕНЦІЇ СЦИНТИЛЯТОРІВ НА ОСНОВІ ПОЛІСТИРОЛУ ТА ПОЛІ-2,4-ДИМЕТИЛСТИРОЛУ, СПОСОБИ ПІДВИЩЕННЯ ЇХ РАДІАЦІЙНОЇ СТІЙКОСТІ Н.І. Воронкіна, В.Г. Сенчишин, В.К. Мілінчук, І.П. Шелухов Одержано спектри радіолюмінесценції пластмасових сцинтиляторів на основі полістиролу та полі-2,4- диметилстиролу під дією γ-випромінювання. Показано, що найбільш ефективними гасниками є макрорадикали, на які відбувається перенос енергії збудження з первинної люмінесціючої домішки. Запропоновано способи підвищення радіаційної стійкості ПС. ____________________________________________________________ PROBLEMS OF ATOMIC SCIENCE AND TECHNOLOGY. 2006. № 3. Series: Nuclear Physics Investigations (47), p. 145-147. 147 ДЕГрадАЦиЯ РАДИолюминесценции сцинтилляторов на основе полистирола и поли-2,4-диметилстирола, способы повышения их радиационной стойкости ДЕГРАДАЦІЯ радіолюмінесценції сцинтиляторів на основі полістиролу та полі-2,4-диметилстиролу, способи підвищення їх радіаційної стійкості
id nasplib_isofts_kiev_ua-123456789-79874
institution Digital Library of Periodicals of National Academy of Sciences of Ukraine
issn 1562-6016
language English
last_indexed 2025-12-07T17:32:29Z
publishDate 2006
publisher Національний науковий центр «Харківський фізико-технічний інститут» НАН України
record_format dspace
spelling Voronkina, N.I.
Senchyshyn, V.G.
Milinchuk, V.K.
Sheluhov, I.P.
2015-04-06T14:47:03Z
2015-04-06T14:47:03Z
2006
Radioluminescence degradation of scintillators on a basis of polystyrene and poly-2,4-dimethylstyrene, the ways of their radiating stability increasing / N.I. Voronkina, V.G. Senchyshyn, V.K. Milinchuk, I.P. Sheluhov // Вопросы атомной науки и техники. — 2006. — № 3. — С. 145-147. — Бібліогр.: 4 назв. — англ.
1562-6016
PACS: 29.40.Mc
https://nasplib.isofts.kiev.ua/handle/123456789/79874
Spectra of radioluminescence of plastic scintillators on a basis of polystyrene and poly-2,4-dimethylstyrene under
 an influence of γ-radiation are obtained. It is shown that the most effective quenchers are macroradicals, on
 which a transmission of excitation energy from “initial” luminescent additives occurs. The ways to increase PS radiating
 stability are proposed.
Получены спектры радиолюминесценции пластмассовых сцинтилляторов на основе полистирола и поли-2,4-диметилстирола при воздействии на них γ-излучения. Показано, что наиболее эффективными тушителями являются макрорадикалы, на которые происходит перенос энергии возбуждения с первичной люминесцирующей добавки. Предложены способы повышения радиационной стойкости ПС.
Одержано спектри радіолюмінесценції пластмасових сцинтиляторів на основі полістиролу та полі-2,4-
 диметилстиролу під дією γ-випромінювання. Показано, що найбільш ефективними гасниками є
 макрорадикали, на які відбувається перенос енергії збудження з первинної люмінесціючої домішки.
 Запропоновано способи підвищення радіаційної стійкості ПС.
en
Національний науковий центр «Харківський фізико-технічний інститут» НАН України
Вопросы атомной науки и техники
Применение ускорителей в радиационных технологиях
Radioluminescence degradation of scintillators on a basis of polystyrene and poly-2,4-dimethylstyrene, the ways of their radiating stability increasing
Деградация радиолюминесценции сцинтилляторов на основе полистирола и поли-2,4-диметилстирола, способы повышения их радиационной стойкости
Деградація радіолюмінесценції сцинтиляторів на основі полістиролу та полі-2,4-диметилстиролу, способи підвищення їх радіаційної стійкості
Article
published earlier
spellingShingle Radioluminescence degradation of scintillators on a basis of polystyrene and poly-2,4-dimethylstyrene, the ways of their radiating stability increasing
Voronkina, N.I.
Senchyshyn, V.G.
Milinchuk, V.K.
Sheluhov, I.P.
Применение ускорителей в радиационных технологиях
title Radioluminescence degradation of scintillators on a basis of polystyrene and poly-2,4-dimethylstyrene, the ways of their radiating stability increasing
title_alt Деградация радиолюминесценции сцинтилляторов на основе полистирола и поли-2,4-диметилстирола, способы повышения их радиационной стойкости
Деградація радіолюмінесценції сцинтиляторів на основі полістиролу та полі-2,4-диметилстиролу, способи підвищення їх радіаційної стійкості
title_full Radioluminescence degradation of scintillators on a basis of polystyrene and poly-2,4-dimethylstyrene, the ways of their radiating stability increasing
title_fullStr Radioluminescence degradation of scintillators on a basis of polystyrene and poly-2,4-dimethylstyrene, the ways of their radiating stability increasing
title_full_unstemmed Radioluminescence degradation of scintillators on a basis of polystyrene and poly-2,4-dimethylstyrene, the ways of their radiating stability increasing
title_short Radioluminescence degradation of scintillators on a basis of polystyrene and poly-2,4-dimethylstyrene, the ways of their radiating stability increasing
title_sort radioluminescence degradation of scintillators on a basis of polystyrene and poly-2,4-dimethylstyrene, the ways of their radiating stability increasing
topic Применение ускорителей в радиационных технологиях
topic_facet Применение ускорителей в радиационных технологиях
url https://nasplib.isofts.kiev.ua/handle/123456789/79874
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