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Thermal Annealing of Paramagnetic Defects Induced by Gamma Irradiation in (NH{sub 4}){sub 2}SO{sub 4} and (ND{sub 4}){sub 2}SO{sub 4} Single Crystals: Experimental Verification of the Theory of Fletcher and Brown; Recuit Thermique des Defauts Paramagnetiques Induits par Irradiation Gamma dans des Monocristaux de (NH{sub 4}){sub 2}SO{sub 4} et (ND{sub 4}){sub 2}SO{sub 4}: Verification Experimentale de la Theorie de Fletcher et Brown; 0422 0415 0420 041c 0414 ; Regeneracion Termica de los Defectos Paramagneticos Inducidos por Irradiacion Gamma en Monocristales de (NH{sub 4}){sub 2}SO{sub 4} y (ND{sub 4}){sub 2}SO{sub 4}: Verificacion Experimental de la Teoria de Fletcher y Brown

Abstract

In irradiated (NH{sub 4}){sub 2}SO{sub 4} And (ND{sub 4}){sub 2}SO{sub 4} crystals two paramagnetic species were identified by means of the electron spin resonance method. The g constant of the first radical is 2.014 and of the second 2.020 for the normal hydrogen compound; for the deuterated compound they are 1.996 and 2.0032 respectively. Study of the annealing of the first radical in the 60 Degree-Sign -170 Degree-Sign C range showed that in this case the kinetics display a single plateau corresponding to a total recombination of the radicals. For each isotherm it was possible to obtain the appropriate equation using the errors function derived by Fletcher and Brown and taking as a model the recombination of initially correlated (and subsequently liberated) pairs by a random-walk process. Agreement between this function and experimental results was obtained after correcting the function by a factor {alpha}. The composite annealing curve is in good agreement with the corrected errors function. Using the phenomenological method of Fletcher and Brown for calculating the activation energy we obtained a value of 1.594 eV, corresponding to the first radical in (NH{sub 4}){sub 2}SO{sub 4}. On the basis of the variation of the diffusion coefficient with temperature we  More>>
Authors:
Calusaru, A.; Barbur, I.; Ursu, I.; [1]  Universite 'Babes', Cluj (Romania)]
  1. Institut de Physique Atomique, Bucarest (Romania)
Publication Date:
Apr 15, 1965
Product Type:
Conference
Report Number:
IAEA-SM-57/96
Resource Relation:
Conference: Symposium on Chemical Effects Associated with Nuclear Reactions and Radioactive Transformations, Heidelberg (Germany), 7-11 Dec 1964; Other Information: 18 refs., 13 figs., 2 tabs.; Related Information: In: Chemical Effects of Nuclear Transformations. Vol. II. Proceedings of the Symposium on Chemical Effects Associated with Nuclear Reactions and Radioactive Transformations| 572 p.
Subject:
36 MATERIALS SCIENCE; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY AND NUCLEAR CHEMISTRY; ACTIVATION ENERGY; AMMONIUM SULFATES; ANNEALING; CHEMICAL RADIATION EFFECTS; DEUTERIDES; ELECTRON SPIN RESONANCE; GAMMA RADIATION; GRAPH THEORY; IRRADIATION; ISOTHERMS; MONOCRYSTALS; PARAMAGNETISM; RECOMBINATION
OSTI ID:
22184523
Research Organizations:
International Atomic Energy Agency, Vienna (Austria); Joint Commission on Applied Radioactivity of the International Council of Scientific Unions, Paris (France)
Country of Origin:
IAEA
Language:
French
Other Identifying Numbers:
Other: ISSN 0074-1884; TRN: XA13M3336008563
Submitting Site:
INIS
Size:
page(s) 293-311
Announcement Date:
Jan 30, 2014

Citation Formats

Calusaru, A., Barbur, I., Ursu, I., and Universite 'Babes', Cluj (Romania)]. Thermal Annealing of Paramagnetic Defects Induced by Gamma Irradiation in (NH{sub 4}){sub 2}SO{sub 4} and (ND{sub 4}){sub 2}SO{sub 4} Single Crystals: Experimental Verification of the Theory of Fletcher and Brown; Recuit Thermique des Defauts Paramagnetiques Induits par Irradiation Gamma dans des Monocristaux de (NH{sub 4}){sub 2}SO{sub 4} et (ND{sub 4}){sub 2}SO{sub 4}: Verification Experimentale de la Theorie de Fletcher et Brown; 0422 0415 0420 041c 0414 ; Regeneracion Termica de los Defectos Paramagneticos Inducidos por Irradiacion Gamma en Monocristales de (NH{sub 4}){sub 2}SO{sub 4} y (ND{sub 4}){sub 2}SO{sub 4}: Verificacion Experimental de la Teoria de Fletcher y Brown. IAEA: N. p., 1965. Web.
Calusaru, A., Barbur, I., Ursu, I., & Universite 'Babes', Cluj (Romania)]. Thermal Annealing of Paramagnetic Defects Induced by Gamma Irradiation in (NH{sub 4}){sub 2}SO{sub 4} and (ND{sub 4}){sub 2}SO{sub 4} Single Crystals: Experimental Verification of the Theory of Fletcher and Brown; Recuit Thermique des Defauts Paramagnetiques Induits par Irradiation Gamma dans des Monocristaux de (NH{sub 4}){sub 2}SO{sub 4} et (ND{sub 4}){sub 2}SO{sub 4}: Verification Experimentale de la Theorie de Fletcher et Brown; 0422 0415 0420 041c 0414 ; Regeneracion Termica de los Defectos Paramagneticos Inducidos por Irradiacion Gamma en Monocristales de (NH{sub 4}){sub 2}SO{sub 4} y (ND{sub 4}){sub 2}SO{sub 4}: Verificacion Experimental de la Teoria de Fletcher y Brown. IAEA.
Calusaru, A., Barbur, I., Ursu, I., and Universite 'Babes', Cluj (Romania)]. 1965. "Thermal Annealing of Paramagnetic Defects Induced by Gamma Irradiation in (NH{sub 4}){sub 2}SO{sub 4} and (ND{sub 4}){sub 2}SO{sub 4} Single Crystals: Experimental Verification of the Theory of Fletcher and Brown; Recuit Thermique des Defauts Paramagnetiques Induits par Irradiation Gamma dans des Monocristaux de (NH{sub 4}){sub 2}SO{sub 4} et (ND{sub 4}){sub 2}SO{sub 4}: Verification Experimentale de la Theorie de Fletcher et Brown; 0422 0415 0420 041c 0414 ; Regeneracion Termica de los Defectos Paramagneticos Inducidos por Irradiacion Gamma en Monocristales de (NH{sub 4}){sub 2}SO{sub 4} y (ND{sub 4}){sub 2}SO{sub 4}: Verificacion Experimental de la Teoria de Fletcher y Brown." IAEA.
@misc{etde_22184523,
title = {Thermal Annealing of Paramagnetic Defects Induced by Gamma Irradiation in (NH{sub 4}){sub 2}SO{sub 4} and (ND{sub 4}){sub 2}SO{sub 4} Single Crystals: Experimental Verification of the Theory of Fletcher and Brown; Recuit Thermique des Defauts Paramagnetiques Induits par Irradiation Gamma dans des Monocristaux de (NH{sub 4}){sub 2}SO{sub 4} et (ND{sub 4}){sub 2}SO{sub 4}: Verification Experimentale de la Theorie de Fletcher et Brown; 0422 0415 0420 041c 0414 ; Regeneracion Termica de los Defectos Paramagneticos Inducidos por Irradiacion Gamma en Monocristales de (NH{sub 4}){sub 2}SO{sub 4} y (ND{sub 4}){sub 2}SO{sub 4}: Verificacion Experimental de la Teoria de Fletcher y Brown}
author = {Calusaru, A., Barbur, I., Ursu, I., and Universite 'Babes', Cluj (Romania)]}
abstractNote = {In irradiated (NH{sub 4}){sub 2}SO{sub 4} And (ND{sub 4}){sub 2}SO{sub 4} crystals two paramagnetic species were identified by means of the electron spin resonance method. The g constant of the first radical is 2.014 and of the second 2.020 for the normal hydrogen compound; for the deuterated compound they are 1.996 and 2.0032 respectively. Study of the annealing of the first radical in the 60 Degree-Sign -170 Degree-Sign C range showed that in this case the kinetics display a single plateau corresponding to a total recombination of the radicals. For each isotherm it was possible to obtain the appropriate equation using the errors function derived by Fletcher and Brown and taking as a model the recombination of initially correlated (and subsequently liberated) pairs by a random-walk process. Agreement between this function and experimental results was obtained after correcting the function by a factor {alpha}. The composite annealing curve is in good agreement with the corrected errors function. Using the phenomenological method of Fletcher and Brown for calculating the activation energy we obtained a value of 1.594 eV, corresponding to the first radical in (NH{sub 4}){sub 2}SO{sub 4}. On the basis of the variation of the diffusion coefficient with temperature we obtained a value of 1.592 eV for the same activation energy. With the Vand- Primack method we obtained 1.45 eV, which is lower than the two preceding values. We concluded that the recombination of correlated pairs by a random-walk process can be used as a model in the form given by the theory if the interaction between the species formed and the lattice is fairly weak; in this way the pairs which are initially correlated can be liberated. (author) [French] Dans les cristaux irradies de (NH{sub 4}){sub 2}SO{sub 4} et (ND{sub 4}){sub 2}SO{sub 4}, on a identifie deux especes paramagnetiques en utilisant la methode de resonance du spin electronique. La constante g du premier radical est 2,014, et celle du second 2,020, pour le sulfate d'ammonium avec hydrogene; les memes constantes pour le cristal deutere sont 1,9996 et 2,0032. L'etude du recuit du premier radical pour des temperatures comprises entre 60 Degree-Sign et 170 Degree-Sign C a montre qu'il y a dans ce cas une cinetique a un seul plateau correspondant a une recombinaison totale des radicaux. Il a ete possible d'etablir une equation pour chaque isotherme, en utilisant la fonction des erreurs deduite par Fletcher et Brown, et en prenant pour modele la recombinaison, selon un processus aleatoire (random-walk process), des paires initialement conelees, puis liberees. L'accord entre cette fonction et l'experience a ete obtenu apres correction de cette fonction par un facteur a. La courbe de recuit ainsi etablie verifie tres bien la fonction des erreurs corrigee. En appliquant la methode phenomenologique de Fletcher et Brown pour le calcul de l'energie d'activation, on a trouve la valeur 1,594 eV, qui correspond au premier radical en (NH{sub 4}){sub 2}SO{sub 4}. En utilisant la variation du coefficient de diffusion en fonction de la temperature, on a obtenu pour la meme energie d'activation la valeur 1,592 eV. Par la methode de Vand-Primack on a trouve la valeur 1,45 eV, qui est plus petite que les deux precedentes. On a considere, en conclusion, que le modele de la recombinaison des paires correlees d'apres un processus aleatoire est applicable dans la forme donnee par la theorie lorsqu'il y a une assez faible interaction entre le reseau et les especes formees-, de cette maniere les paires initialement correlees peuvent se liberer. (author) [Spanish] En cristales de (NH{sub 4}){sub 2}SO{sub 4} y (ND{sub 4}){sub 2}SO{sub 4}, sometidos a irradiacion, se han identificado dos especies paramagneticas aplicando el metodo de resonancia del espfn electronico. La constante g del primer radical es de 2,014 y la del segundo de 2,020, para el (NH{sub 4}){sub 2}SO{sub 4}; en el caso del cristal deuterado, dichas constantes son 1,996 y 2,0032, respectivamente. El estudio de la regeneracion por recocido del primer radical en el intervalo 60 Degree-Sign -170 Degree-Sign C revela la existencia de una cinetica con un solo rellano correspondiente a una recombinacion total de los radicales. Se ha podido establecer, para cada isoterma, la ecuacion correspondiente utilizando la funcion de errores deducida por Fletcher y Brown considerando el modelo de recombinacion de pares inicialmente correlacionados (y luego liberados) segun un proceso aleatorio. La concordancia entre los resultados experimentales y la funcion se obtiene corrigiendo esta mediante un factor alfa. La curva compuesta de recocido se ajusta muy bien a la funcion de errores corregida. Aplicando el metodo fenomenologico de Fletcher y Brown para calcular la energia de activacion, se ha hallado el valor de 1,594 eV, correspondiente al primer radical en el (NH{sub 4}){sub 2}SO{sub 4}. Basandose en la variacion del coeficiente de difusion con la temperatura, se ha determinado el valor de 1,592 eV para la misma energia de activacion. Aplicando el metodo de Vand-Primack se ha hallado el valor de 1,45 eV, menor que los dos anteriores. Se estima, en conclusion, que el modelo de recombinacion de pares correlacionados segun un proceso aleatorio es aplicable en la formula dada por la teoria cuando la interaccion de las especies formadas con la red es bastante debil; en esas condiciones, los pares correlacionados inicialmente pueden liberarse. (author) [Russian] V obluchennyh kristallah (NH{sub 4}){sub 2}SO{sub 4} i (ND{sub 4}){sub 2}SO{sub 4} s pomoshh'ju metoda rezonansa spina jelektrona byli identificirovany dva paramagnitnyh vida. Konstanta g pervogo radikala sostavljaet 2,014 i vtorogo-2,020 dlja sul'fata ammonija s vodorodom; te zhe konstanty dlja dejterirovannogo kristalla sostavljajut 1,9996 i 2,0032. Izuchenie otzhiga pervogo radikala pri temperaturah mezhdu 60 Degree-Sign i 170 Degree-Sign C pokazalo, chto v dannom sluchae imeet mesto kinetika s edinym plato, sootvetstvujushhim obshhej rekombinacii radikalov. Dlja kazhdoj izotermy predstavljaetsja vozmozhnym sostavit' sootvetstvujushhee uravnenie, ispol'zuja pri jetom funkciju oshibok, vyvedennuju Fletcherom i Braunom pri rassmotrenii modeli i rekombinacii par, vnachale korrelirovannyh, a zatem vydelennyh v sootvetstvii s processom besporjadochnogo dvizhenija. Posle ispravlenija jetoj funkcii s uchetom kojefficienta q dannaja funkcija byla privedena v sootvetstvie s opytom. Sostavnaja krivaja otzhiga ochen' horosho otrazhaet funkciju ispravlennyh oshibok. Pri primenenii fenomenologicheskogo metoda Fletchera i Brauna dlja rascheta jenergii aktivacii bylo najdeno znachenie 1,594 jev, sootvetstvujushhee pervomu radikalu v (NH{sub 4}){sub 2}SO{sub 4}. Ispol'zuja izmenenie kojefficienta diffuzii'v zavisimosti ot temperatury, dlja toj zhe jenergii aktivacii bylo ustanovleno znachenie v 1,592 jev. S pomoshh'ju metoda Vand-Primak bylo najdeno znachenie v 1,45 jev, kotoroe javljaetsja men'shim po sravneniju s dvumja predydushhimi. V zakljuchenie otmechaetsja, chto model' rekombinacii par, korrelirovannyh v sootvetstvii s processom besporjadochnogo dvizhenija, primenima v forme, privedennoj v teorii, kogda imeetsja dovol'no slaboe vzaimodejstvie mezhdu obrazovavshimisja vidami i reshetkoj; takim putem pervonachal'no korrelirovannye pary mogut byt' vydeleny. (author)}
place = {IAEA}
year = {1965}
month = {Apr}
}