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Since its discovery, the phenomenon of nuclear fission is the object of extensive theoretical and experimental studies. However, we are still far from a complete understanding of the fission process. Nuclear theory can satisfactorily explain the process of neutron-induced fission at thermal neutron energies, but it meets problems at high neutron energies. However, new applications are nowadays developed involving neutron-induced fission in this energy domain. An example of such an application is accelerator-driven systems (ADS) which are dedicated to transmutation of highly radioactive nuclear waste. Conceptual studies of ADS require new nuclear data on neutron-induced reactions within a wide incident energy range. Along with structural, spallation target and other materials, data on neutron-induced fission are especially required for two nuclides, 232Th and 238U. At present, however, there are no published neutron-induced fission yield data for either 232Th or 238U at energies above 20 MeV. In this thesis, I present measurements of fission fragment mass yields at neutron energies from 10 to 60 MeV for 232Th and 238U. The experiment was done at the Louvain-la-Neuve quasi-monoenergetic neutron beam facility. A multi-section Frisch-gridded ionization chamber was used as the fission fragment detector. The fission fragment mass yields were measured at peak neutron energies of 33, 45, and 60 MeV. In addition, data for the neutron-energy intervals 9-11, 16-18, and 24-26 MeV were also extracted from the low-energy tail. The measurement results show that the symmetric fission component increases with incident neutron energy for both uranium and thorium, but it is more enhanced for thorium. The uranium results were compared to the only existing set of experimental data for neutron energies above 20 MeV. Reasonable agreement was found. However, our data show a lower symmetric fission component. For thorium, the present data are the first above 20 MeV. Model calculations with the TALYS code have also been done. This code is based on the multi-modal random neck-rupture model extended for higher excitation energies. We included a phenomenological model into the code and achieved a good description of our experimental results. / Felaktigt tryckt som Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology 723

This work investigates the feasibility to perform an experiment at CERN n_TOF to study the fission cross section and fission fragment angular distribution (FFAD) of the 230Th(n,f) reaction. An analysis of fission fragment energy losses in the experimental target resulted in a choice of target thickness of 0.1 µm (100 µg/cm2 ), which yields good transmission out of the target at up to 45° emission angles from the target normal. A detection setup using ten PPAC detectors with nine thorium targets interleaved in between them was investigated, where the detectors and targets were tilted 45° with respect to the neutron beam. This makes it possible to measure all emission angles needed with respect to the neutron beam in order to determine the FFAD. For the experimental area EAR2 at n_TOF, a prediction of the count rate in the experiment resulted in low statistical uncertainties after a few weeks of beam time, which indicates that an experiment like this is feasible. / Detta projekt undersöker genomförbarheten av ett experiment vid CERN n_TOF för att mäta tvärsnittet och fördelningen av emissionsvinklar av fissionsfragment (FFAD) från 230Th(n,f)-reaktionen. En analys av energiförlusterna av fissionsfragment inuti torium-provet resulterade i en optimal provtjocklek på 0.1 µm (100 µg/cm2 ), vilket medför att fissionsfragment som emitteras i vinklar upp till 45° från provets normal har hög sannolikhet att transmitteras ut ur provet. En detektionsuppställning med tio PPAC-detektorer med nio toriumprov mellan dem undersöktes, där detektorerna och proven antogs vara snedställda med 45° från neutronstrålens riktning. Detta möjliggör detektion av fissionsfragment i alla vinklar som är nödvändiga för att kunna mäta hela FFAD. För experimentanläggningen EAR2 vid n_TOF, resulterade en uppskattning av antalet detekterade fissionsevent per sekund i låga mätosäkerheter efter ett par veckor av mättid, vilket antyder att experimentet är görbart.

Präzise neutroneninduzierte Spaltquerschnitte von Actinoiden wie den Plutoniumisotopen haben für die Entwicklung zukünftiger Transmutationstechnologien eine große Bedeutung. Die Unsicherheiten des Pu(242)-Spaltquerschnitts im schnellen Bereich des Spektrums betragen derzeit etwa 21 %. Aktuelle Sensitivitätsstudien haben gezeigt, dass nur eine Reduzierung dieser Unsicherheiten auf unter 5% verlässliche neutronenphysikalische Simulationen zulässt. Diese anspruchsvolle Aufgabe konnte im Rahmen der vorliegenden Arbeit an der Neutronenfugzeitanlage nELBE durchgeführt werden. Dünne, homogene und großfächige Actinoiden-Proben wurden dem Helmholtz-Zentrum Dresden-Rossendorf innerhalb des TRAKULA-Verbundprojektes zur Verfügung gestellt. Eingesetzt in eine neu entwickelte Spaltionisationskammer ermöglichten sie eine akkurate Bestimmung des Pu(242)- Spaltquerschnitts relativ zu U(235). Die Flächendichten der Plutoniumschichten wurden anhand der spontanen Spaltrate von Pu(242) bestimmt. Aufwändige Teilchentransportsimulationen (durchgeführt mit Geant 4, MCNP 6 und FLUKA) wurden genutzt, um die auftretende Neutronenstreuung zu korrigieren. Die gewonnenen Ergebnisse sind im Rahmen ihrer Unsicherheiten in guter Übereinstimmung mit aktuellen Kerndatenevaluierungen. / Neutron induced fssion cross sections of actinides like the Pu-isotopes are of relevance for the development of nuclear transmutation technologies. For Pu(242), current uncertainties are of around 21%. Sensitivity studies show that the total uncertainty has to be reduced to below 5% to allow for reliable neutron physics simulations. This challenging task was performed at the neutron time-of-fight facility of the new German National Center for High Power Radiation Sources at HZDR, Dresden. Within the TRAKULA project, thin, large and homogeneous deposits of U(235) and Pu(242) have been produced successfully. Using two consecutively placed fssion chambers allowed the determination of the neutron induced fssion cross section of Pu(242) relative to U(235). The areal density of the Plutonium targets was calculated using the measured spontaneous fssion rate. Experimental results of the fast neutron induced fssion of Pu(242) acquired at nELBE will be presented and compared to recent experiments and evaluated data. Corrections addressing the neutron scattering are discussed by using results of different neutron transport simulations (Geant 4, MCNP 6 and FLUKA).

Präzise neutroneninduzierte Spaltquerschnitte von Actinoiden wie den Plutoniumisotopen haben für die Entwicklung zukünftiger Transmutationstechnologien eine große Bedeutung. Die Unsicherheiten des Pu(242)-Spaltquerschnitts im schnellen Bereich des Spektrums betragen derzeit etwa 21 %. Aktuelle Sensitivitätsstudien haben gezeigt, dass nur eine Reduzierung dieser Unsicherheiten auf unter 5% verlässliche neutronenphysikalische Simulationen zulässt. Diese anspruchsvolle Aufgabe konnte im Rahmen der vorliegenden Arbeit an der Neutronenfugzeitanlage nELBE durchgeführt werden. Dünne, homogene und großfächige Actinoiden-Proben wurden dem Helmholtz-Zentrum Dresden-Rossendorf innerhalb des TRAKULA-Verbundprojektes zur Verfügung gestellt. Eingesetzt in eine neu entwickelte Spaltionisationskammer ermöglichten sie eine akkurate Bestimmung des Pu(242)- Spaltquerschnitts relativ zu U(235). Die Flächendichten der Plutoniumschichten wurden anhand der spontanen Spaltrate von Pu(242) bestimmt. Aufwändige Teilchentransportsimulationen (durchgeführt mit Geant 4, MCNP 6 und FLUKA) wurden genutzt, um die auftretende Neutronenstreuung zu korrigieren. Die gewonnenen Ergebnisse sind im Rahmen ihrer Unsicherheiten in guter Übereinstimmung mit aktuellen Kerndatenevaluierungen.:1 Einleitung 1.1 Partitionierung und Transmutation 1.2 Die Bedeutung von Pu(242) für P&T 1.3 Bisherige Experimente 1.4 Evaluierungen 1.5 Gliederung dieser Arbeit 2 Spaltwahrscheinlichkeit 2.1 Statistisches Modell und Compoundkern 2.2 Kernreaktionsrechnungen 3 Die Neutronenfugzeitanlage nELBE 4 Spaltionisationskammern 4.1 Die nELBE Spaltkammern 4.1.1 Actinoidenschichten 4.1.2 Aufbau 4.1.3 Gasversorgung 4.1.4 Optimierung des elektrischen Feldes 4.1.5 Simulationen von Impulshöhenverteilungen 4.2 Die PTB U(235) Spaltkammer H19 5 Experimente zur Spaltung von Pu(242) 5.1 Experimentelle Bestimmung neutroneninduzierter Spaltquerschnitte 5.2 Messaufbau 5.3 Datenaufnahme und -verarbeitung 5.4 Datenanalyse 5.4.1 Bestimmung der Spontanspaltrate 5.4.2 Bestimmung des neutroneninduzierten Spaltquerschnitts von Pu(242) 5.5 Ergebnisse und Diskussion 5.5.1 Diskussion 5.5.2 Unsicherheiten 5.5.3 Vergleich mit Kernreaktionsrechnungen 6 Zusammenfassung und Ausblick Anhang A.1 Depositionszelle A.2 Neutronenfugzeitanlagen A.3 Spaltfragmentverteilungen mit GEF A.4 Experimenteller Aufbau A.5 Aufbau der Datenaufnahme/-verarbeitung A.5.1 Verwendete Elektronik A.6 Stabilität der Datenaufnahme A.7 Konsistenzbetrachtung der Querschnittsbestimmung Literaturverzeichnis Abbildungsverzeichnis Tabellenverzeichnis Liste der verwendeten Akronyme Publikationen / Neutron induced fssion cross sections of actinides like the Pu-isotopes are of relevance for the development of nuclear transmutation technologies. For Pu(242), current uncertainties are of around 21%. Sensitivity studies show that the total uncertainty has to be reduced to below 5% to allow for reliable neutron physics simulations. This challenging task was performed at the neutron time-of-fight facility of the new German National Center for High Power Radiation Sources at HZDR, Dresden. Within the TRAKULA project, thin, large and homogeneous deposits of U(235) and Pu(242) have been produced successfully. Using two consecutively placed fssion chambers allowed the determination of the neutron induced fssion cross section of Pu(242) relative to U(235). The areal density of the Plutonium targets was calculated using the measured spontaneous fssion rate. Experimental results of the fast neutron induced fssion of Pu(242) acquired at nELBE will be presented and compared to recent experiments and evaluated data. Corrections addressing the neutron scattering are discussed by using results of different neutron transport simulations (Geant 4, MCNP 6 and FLUKA).:1 Einleitung 1.1 Partitionierung und Transmutation 1.2 Die Bedeutung von Pu(242) für P&T 1.3 Bisherige Experimente 1.4 Evaluierungen 1.5 Gliederung dieser Arbeit 2 Spaltwahrscheinlichkeit 2.1 Statistisches Modell und Compoundkern 2.2 Kernreaktionsrechnungen 3 Die Neutronenfugzeitanlage nELBE 4 Spaltionisationskammern 4.1 Die nELBE Spaltkammern 4.1.1 Actinoidenschichten 4.1.2 Aufbau 4.1.3 Gasversorgung 4.1.4 Optimierung des elektrischen Feldes 4.1.5 Simulationen von Impulshöhenverteilungen 4.2 Die PTB U(235) Spaltkammer H19 5 Experimente zur Spaltung von Pu(242) 5.1 Experimentelle Bestimmung neutroneninduzierter Spaltquerschnitte 5.2 Messaufbau 5.3 Datenaufnahme und -verarbeitung 5.4 Datenanalyse 5.4.1 Bestimmung der Spontanspaltrate 5.4.2 Bestimmung des neutroneninduzierten Spaltquerschnitts von Pu(242) 5.5 Ergebnisse und Diskussion 5.5.1 Diskussion 5.5.2 Unsicherheiten 5.5.3 Vergleich mit Kernreaktionsrechnungen 6 Zusammenfassung und Ausblick Anhang A.1 Depositionszelle A.2 Neutronenfugzeitanlagen A.3 Spaltfragmentverteilungen mit GEF A.4 Experimenteller Aufbau A.5 Aufbau der Datenaufnahme/-verarbeitung A.5.1 Verwendete Elektronik A.6 Stabilität der Datenaufnahme A.7 Konsistenzbetrachtung der Querschnittsbestimmung Literaturverzeichnis Abbildungsverzeichnis Tabellenverzeichnis Liste der verwendeten Akronyme Publikationen

Nowadays we are all witnesses of a competition of facilities at different countries to study unknown regions of neutron rich nuclei. Much efforts are devoted to understand the role of neutron excess and its influence on nuclei in vicinity of closed neutron shells. One of the means to investigate nuclear structure is in beta-decay. Once a nucleus is proven to exist, its beta-decay properties, such as T1/2 and Pn (probability of beta-delayed neutron emission), which are relatively easy to measure, can provide the first hints on the nuclear structure. On the r-process site, "waiting points"(nuclei on closed neutron shells) has significant effects on the r-process dynamics and the abundance distribution. The actual side and the astrophysical conditions under which the nuclear synthesis takes place are still not certainly known - since r-process nuclei are difficult to produce and to study experimentally, input parameters for r-process calculations are mostly derived from theoretical models. As it has been seen lately, most of the theories have failed to reproduce newly measured data sets near shell closures. With new experimental data already (or shortly) available theoretical approaches can be adjusted. Since a beta-delayed neutron emission becomes strong if not dominating decaying channel for nuclei far stability, a proper neutron detector to study their properties is indispensable. To conduct the appropriate investigations, in the frame of the present thesis, in close collaboration with JINR (Dubna) a new detection system was constructed. It consists of 80 ³He-filled counters, 4π beta detector and a HPGe in order to measure simultaneously beta, gamma, neutron activity. The development of such a detection system system, currently installed at ALTO ISOL facility, was the first objective of the thesis. Then, during two experimental campaigns conducted to investigate beta decay properties of neutron rich nuclei in the neighborhood of N=50, N=82 the workability of the newly produced detection system was proven. In the vicinity of ⁷⁸Ni: half- lives and probability of beta-delayed neutron emission for ⁸º,⁸²,⁸³,⁸⁴Ga were measured. We were the first to observe the structure of ⁸¹,⁸² Ge via beta neutron gated gamma spectra. Thanks to the neutron detection channel the absolute intensities of beta decay were proposed for the first time. In the vicinity of ¹³²Sn the half lives of ¹²³Ag, ¹²⁴Ag, ¹²⁵Ag and ¹²⁷In, ¹²⁸In was measured. For the first time the beta delayed neutron emission was observed for ¹²⁶Cd, its Pn value also measured. Based on the data obtained we come to the conclusion that to figure out the relative contribution of allowed and forbidden decays more theoretical efforts should be done crossing the N=50 shell. Whereas in the vicinity of N=82 shell more experimental challenge are required.

Aujourd'hui, nous sommes tous témoins d'une compétition des installations en pays différents pour étudier les régions inconnues de noyaux riches en neutrons. Beaucoup d'efforts sont consacrés à comprendre le rôle de l'excès de neutrons et son influence sur les noyaux dans les environs de coquilles de neutrons fermées. Un des moyens pour étudier la structure nucléaire est via la désintégration bêta. Une fois un noyau est prouvé d'exister, ses propriétés de désintégration bêta, comme T1/2 et Pn (probabilité de l'émission de neutrons de bêta-retardés), qui sont relativement faciles à mesurer, peuvent fournir les premiers indices sur la structure nucléaire. Sur le site de processus-r des «points d'attente» (noyaux sur des coquilles de neutrons fermés) ont des effets importants sur la dynamique processus-r ainsi que sur la distribution de l'abondance des éléments. Les conditions astrophysiques exactes en vertu de desquelles la synthèse nucléaire a lieu ne sont pas connus avec certitude. Parce que les noyaux participant en processus-r sont difficiles à synthétiser même aujourd'hui et à étudier expérimentalement, les paramètres nécessaires pour les calculs du processus-r sont principalement dérivés de modèles théoriques. Comme on l'a vu récemment, la plupart des théories n'ont pas réussi à reproduire des ensembles de données nouvellement mesurées près de fermetures de couche. Avec de nouvelles données expérimentales déjà (ou bientôt) disponibles les approches théoriques peuvent être ajustées. Comme émission de neutrons retardée bêta devient plus importante voie le canal dominant en désintégration des noyaux loin d'un stabilité, l'utilisation d'un détecteur de neutrons approprié afin d'étudier leurs propriétés est indispensable. C'est pour mener la recherche appropriée que dans le cadre de la thèse, en étroite collaboration avec le JINR (Dubna) un nouveau système de détection a été construit. Il se compose de 80 compteurs de ³He, un détecteur 4π de bêta et un HPGe afin de mesurer simultanément l'activité de gamma, bêta et neutrons. Le développement d'un tel système de détection, actuellement installé sur ALTO, a été le premier objectif de la thèse. Puis, au cours de deux campagnes expérimentales menées pour examiner les propriétés de désintégration bêta de noyaux riches en neutrons dans le proximité de N = 50, N = 82 la capacité de travail du système de détection produit a été prouvée. Dans le région de ⁷⁸Ni : le temps de vie et de la probabilité de l'émission de neutrons bêta retardés pour ⁸º,⁸²,⁸³,⁸⁴Ga ont été mesurés. Nous sommes les premiers à observer la structure de ⁸¹,⁸² Ge via spectroscopie gamma spectre conditionnée par bêta et par neutron. Grâce à la détection des neutrons les intensités absolues de la désintégration bêta ont été proposées pour la première fois. Dans le région de ¹³²Sn les temps de vie de ¹²³Ag, ¹²⁴Ag, ¹²⁵Ag et ¹²⁷In, ¹²⁸In ont été mesurées. Pour la première fois l'émission de neutrons retardés bêta a été observée pour le cas de ¹²⁶Cd, sa valeur Pn également mesurée. Sur la base des données obtenues, nous arrivons à la conclusion que, pour déterminer la contribution relative de désintégrations permises et interdites les efforts théoriques doivent être faites en traversant la couche N = 50. Alors que dans le région de N = 82 plus de données expérimentales sont nécessaires. / Nowadays we are all witnesses of a competition of facilities at different countries to study unknown regions of neutron rich nuclei. Much efforts are devoted to understand the role of neutron excess and its influence on nuclei in vicinity of closed neutron shells. One of the means to investigate nuclear structure is in beta-decay. Once a nucleus is proven to exist, its beta-decay properties, such as T1/2 and Pn (probability of beta-delayed neutron emission), which are relatively easy to measure, can provide the first hints on the nuclear structure. On the r-process site, "waiting points"(nuclei on closed neutron shells) has significant effects on the r-process dynamics and the abundance distribution. The actual side and the astrophysical conditions under which the nuclear synthesis takes place are still not certainly known - since r-process nuclei are difficult to produce and to study experimentally, input parameters for r-process calculations are mostly derived from theoretical models. As it has been seen lately, most of the theories have failed to reproduce newly measured data sets near shell closures. With new experimental data already (or shortly) available theoretical approaches can be adjusted. Since a beta-delayed neutron emission becomes strong if not dominating decaying channel for nuclei far stability, a proper neutron detector to study their properties is indispensable. To conduct the appropriate investigations, in the frame of the present thesis, in close collaboration with JINR (Dubna) a new detection system was constructed. It consists of 80 ³He-filled counters, 4π beta detector and a HPGe in order to measure simultaneously beta, gamma, neutron activity. The development of such a detection system system, currently installed at ALTO ISOL facility, was the first objective of the thesis. Then, during two experimental campaigns conducted to investigate beta decay properties of neutron rich nuclei in the neighborhood of N=50, N=82 the workability of the newly produced detection system was proven. In the vicinity of ⁷⁸Ni: half- lives and probability of beta-delayed neutron emission for ⁸º,⁸²,⁸³,⁸⁴Ga were measured. We were the first to observe the structure of ⁸¹,⁸² Ge via beta neutron gated gamma spectra. Thanks to the neutron detection channel the absolute intensities of beta decay were proposed for the first time. In the vicinity of ¹³²Sn the half lives of ¹²³Ag, ¹²⁴Ag, ¹²⁵Ag and ¹²⁷In, ¹²⁸In was measured. For the first time the beta delayed neutron emission was observed for ¹²⁶Cd, its Pn value also measured. Based on the data obtained we come to the conclusion that to figure out the relative contribution of allowed and forbidden decays more theoretical efforts should be done crossing the N=50 shell. Whereas in the vicinity of N=82 shell more experimental challenge are required.