1. Environmental and Climate Research using AMS Karin Hain 16.12.2015

2. 21.09.2015 AMS in Munich Karin Hain2 AMS @ MLL in Munich Nuclear AstrophysicsGeology Dosimetry e.g. 60 Fe in ferromanganese crust / sediments e.g. exposure dating with 53 Mn in Antarctica e.g. Retrospective neutron dosimetry in Hiroshima

3. 21.09.2015 AMS in Munich Karin Hain3 AMS @ MLL in Munich Climate ResearchEnvironmental Research Nuclear AstrophysicsGeology Dosimetry www.esa.int www.posiva.fi e.g. 60 Fe in ferromanganese crust / sediments e.g. Retrospective neutron dosimetry in Hiroshima e.g. exposure dating with 53 Mn in Antarctica

4. 21.09.2015 Climate and Environmental Research Karin Hain4 Climate Research Environmental Research www.esa.int www.posiva.fi (Anthropogenic) long-lived nuclides

5. 21.09.2015 Climate and Environmental Research Karin Hain5 Climate Research Environmental Research www.esa.int www.posiva.fi (Anthropogenic) long-lived nuclides 99 Tc 237 Np Sea Current Tracing Conservative behaviour? Variations of the North Atlantic Current 93 Zr

6. 21.09.2015Karin Hain6 Sea current tracing: 99 Tc Reprocessing plant Sellafield T 1/2 = 2.1 ∙ 10 5 a K.S. Leonard et al, 2003

7. 21.09.2015 Climate and Environmental Research Karin Hain7 Climate Research Environmental Research www.esa.int www.posiva.fi (Anthropogenic) long-lived nuclides 99 Tc 237 Np Sea Current Tracing Glacier retreat Conservative behaviour? Variations of the North Atlantic Current When did glaciation of Antarctica and Greenland start? 53 Mn 93 Zr

8. 21.09.2015 Climate and Environmental Research Karin Hain8 Climate Research Environmental Research www.esa.int www.posiva.fi (Anthropogenic) long-lived nuclides 99 Tc 237 Np Migration in the environment Chemical behaviour in natural waters Biosorption Nuclear Waste Repositories Nuclear Accidents / Monitoring Nuclear Safeguards Sea Current Tracing 239,240 Pu Glacier retreat Conservative behaviour? Variations of the North Atlantic Current When did glaciation of Antarctica and Greenland start? 53 Mn 93 Zr 90 Sr

9. 21.09.2015 Unique Infrastructure in Munich Karin Hain9 12 MV min. Tandem Accelerator 53 Mn, 93 Zr, 99 Tc, 90 Sr at environmental concentration require high energies (150 – 200 MeV) MLL, Munich or ANU, Canberra, Australia

10. 21.09.2015 Unique Infrastructure in Munich Karin Hain10 12 MV min. Tandem Accelerator 53 Mn, 93 Zr, 99 Tc, 90 Sr at environmental concentration require high energies (150 – 200 MeV) Detection of 237 Np relative to spike Spike material commercially not available!

11. 21.09.2015 Unique Infrastructure in Munich Karin Hain11 12 MV min. Tandem Accelerator 53 Mn, 93 Zr, 99 Tc, 90 Sr at environmental concentration require high energies (150 – 200 MeV) Detection of 237 Np relative to spike Spike material commercially not available! Production of non-commercial spike material e.g. 235 Np (T H = 1.09 a)

12. 21.09.2015 Unique Infrastructure in Munich Karin Hain12 12 MV min. Tandem Accelerator 53 Mn, 93 Zr, 99 Tc, 90 Sr at environmental concentration require high energies (150 – 200 MeV) Detection of 237 Np relative to spike Spike material commercially not available! Production of non-commercial spike material e.g. 235 Np (T H = 1.09 a) Chemical purification & characterization of spike material at Radiochemistry Munich

13. 21.09.2015Karin Hain13 Preparatory Works: actinides Aim: Distribution of Pu & Np in ocean water Chemical behaviour With AMS: Small sampling volume: 20 L Improve 237 Np data No chemical separation required? KIT (F. Quinto)  Around 50% error in 237 Np measurements 237 Np a conservative tracer?

14. 21.09.2015 Preparatory Works: 93 Zr Karin Hain14 Master thesis in collaboration with TU Vienna Result: Sensitivity reached 93 Zr/Zr = 2x10 -10 Best sensitivity worldwide  Low detection efficiency

15. 21.09.2015 Preparatory Works: Antarctica Samples Karin Hain15 0.5 t of snow from Antartica collected by Alfred-Wegener-Institut Aim: e.g. global fallout on southern hemisphere Further sample preparation by Atominstitut Wien & Helmholtz Zentrum Dresden-Rossendorf Missing clean lab capacities at MLL

16. 21.09.2015 Required Investments Karin Hain16 3.060.000 € 2 clean laboratories for sample preparation400.000 € Automatized accelerator control200.000 € New injector including Multi-cathode Ion Source100.000 € + Bouncing Magnet200.000 € Silicon Strip Detector 60.000 € Focusing lense100.000 € MICADAS System for complementary Analysis 2.000.000 €

17. 21.09.2015 MICADAS Karin Hain17 www.ionplus.ch MIni CArbon DAting System 3.4 m x 2.6 m x 2 m

18. 21.09.2015 Required Investments Karin Hain18 3.060.000 € 2 clean laboratories for sample preparation400.000 € Automatized accelerator control200.000 € New injector including Multi-cathode Ion Source100.000 € + Bouncing Magnet200.000 € Silicon Strip Detector 60.000 € Focusing lense100.000 € MICADAS System for complementary Analysis2.000.000 €

19. 21.09.2015 Collaboration Partners Karin Hain19 Radiochemie München, TUM Alfred Wegener Institut, Bremerhaven Geomar, Kiel Institut für nukleare Entsorgung, KIT Institut für Umweltphysik, Universität Bremen Helmholtzzentrum Dresden-Rossendorf Lamont-Doherty Earth Observatory, Columbia University, USA Risø DTU National Laboratory for Sustainable Energy, Denmark Atominstitut, TU Wien, Austria Tandar Labor Buenos Aires, Argentina Saha Institute of Nuclear Physics, Kolkata, India IAEA-EL, Monaco National International

20. 21.09.2015Karin Hain20

21. 21.09.2015Karin Hain21

22. 21.09.2015 AMS Setup at the MLL Sample 90 ° Injector Magnet (1 st Mass Separation) 18 ° Electrostatic Deflection Carbon Stripper Foil Wien Filter Wien Filter 90 ° Analyzing Magnet (2 nd Mass Separation) Switching Magnet Negative Ions Positive Ions 2.7m TOF Start − Wien Filter Faraday Cup − − TOF Stop Gas-filled Analyzing Magnet System Current projects: 60 Fe, 53 Mn, 41 Ca, 93 Zr, 99 Tc Karin Hain22

23. 21.09.2015 IAEA-443: spectra 242Pu 5·10 9 atoms TOF (ch) E (ch) TOF (ch) E (ch) TOF (ch) E (ch) 239Pu 238U 240Pu Karin Hain23

24. 21.09.2015 Fission Products W.Koelzer, Lexikon zur Kernenergie; FZK, 2011 Karin Hain24

25. 21.09.2015 Emissions from La Hague & Sellafield Liquid I-129 emissions Emissions of selected isotopes Discharges from reprocessing plants very well known Peaks in release of long-lived isotopes (e.g. Tc-99) can be traced over many decades H.Nies et al, Report, Hamburg, 2008 Karin Hain25

26. 21.09.2015 Previous investigations with I-129 Measurements Alfimov et al. 2004 Results: H.Nies et al, Report, Hamburg, 2008 Karin Hain26

27. 21.09.2015 BUT: Circulation of I-127 extremely complex, can be hardly described by transportation models BUT: Circulation of I-127 extremely complex, can be hardly described by transportation models 1l AMS 50l-100l Conv. Methods e.g. activity measurement Future plans H.Nies et al, Report, Hamburg, 2008 Karin Hain27

28. 21.09.2015 Sample Preparation Radiochemie Muenchen Meier-Leibnitz-Laboratorium Forschungsreaktor Muenchen II 20mg natural, metallic Zr Irradiated for 18h + 2 Zr foils as Flux monitor Karin Hain28

29. 21.09.2015 Isotopic ratios before the accident Credit: J. Zheng et al, Geochemical Journal, Vol 46, pp 361 – 369, 2012 2 main contributions global fallout 240 Pu/ 239 Pu = 0.18 -0.19 (K.O. Buesseler, 1996) 241 Pu/ 239 Pu = 0.0019 (J. Zheng et al, 2013) 237 Np/ 239 Pu = 0.4 – 0.5 (J.M. Kelley et al, 1999) Close-in tropospheric fallout from Pacific Proving Ground 240 Pu/ 239 Pu = 0.21 – 0.36 (K.O. Buesseler, 1996) 241 Pu/ 239 Pu = 0.0057 (J. Zheng et al, 2013) Karin Hain29

30. 21.09.2015 GAMS Beamline Working Principle of the GAMS Using gas-filled 135° Dipole Magnet In evacuated Magnet: Karin Hain30