Environmental and Climate Research using AMS Karin Hain

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Environmental and Climate Research using AMS Karin Hain 16. 12. 2015

Environmental and Climate Research using AMS Karin Hain 16. 12. 2015

AMS in Munich AMS @ MLL in Munich Nuclear Astrophysics Geology e. g. 60

AMS in Munich AMS @ MLL in Munich Nuclear Astrophysics Geology e. g. 60 Fe in ferromanganese crust / sediments e. g. exposure dating with 53 Mn in Antarctica 21. 09. 2015 Karin Hain Dosimetry e. g. Retrospective neutron dosimetry in Hiroshima 2

AMS in Munich Climate Research Environmental Research AMS @ MLL in Munich www. posiva.

AMS in Munich Climate Research Environmental Research AMS @ MLL in Munich www. posiva. fi www. esa. int Nuclear Astrophysics Geology e. g. 60 Fe in ferromanganese crust / sediments e. g. exposure dating with 53 Mn in Antarctica 21. 09. 2015 Karin Hain Dosimetry e. g. Retrospective neutron dosimetry in Hiroshima 3

Climate and Environmental Research Climate Research Environmental Research (Anthropogenic) long-lived nuclides www. posiva. fi

Climate and Environmental Research Climate Research Environmental Research (Anthropogenic) long-lived nuclides www. posiva. fi www. esa. int 21. 09. 2015 Karin Hain 4

Climate and Environmental Research Climate Research Environmental Research (Anthropogenic) long-lived nuclides 99 Tc www.

Climate and Environmental Research Climate Research Environmental Research (Anthropogenic) long-lived nuclides 99 Tc www. esa. int Sea Current Tracing • • www. posiva. fi 93 Zr 237 Np Conservative behaviour? Variations of the North Atlantic Current 21. 09. 2015 Karin Hain 5

Sea current tracing: 99 Tc T 1/2 = 2. 1 ∙ 105 a Reprocessing

Sea current tracing: 99 Tc T 1/2 = 2. 1 ∙ 105 a Reprocessing plant Sellafield 21. 09. 2015 K. S. Leonard et al, 2003 Karin Hain 6

Climate and Environmental Research Climate Research Environmental Research (Anthropogenic) long-lived nuclides 99 Tc www.

Climate and Environmental Research Climate Research Environmental Research (Anthropogenic) long-lived nuclides 99 Tc www. esa. int Sea Current Tracing • • www. posiva. fi 93 Zr 237 Np Conservative behaviour? Variations of the North Atlantic Current Glacier retreat • When did glaciation of Antarctica 53 Mn and Greenland start? 21. 09. 2015 Karin Hain 7

Climate and Environmental Research Climate Research Environmental Research (Anthropogenic) long-lived nuclides 99 Tc www.

Climate and Environmental Research Climate Research Environmental Research (Anthropogenic) long-lived nuclides 99 Tc www. esa. int Sea Current Tracing • • 93 Zr Conservative behaviour? Variations of the North Atlantic Current • • 239, 240 Pu 90 Sr When did glaciation of Antarctica 53 Mn and Greenland start? 21. 09. 2015 Nuclear Waste Repositories 237 Np Glacier retreat • www. posiva. fi Karin Hain • Migration in the environment Chemical behaviour in natural waters Biosorption Nuclear Accidents / Monitoring Nuclear Safeguards 8

Unique Infrastructure in Munich 53 Mn, 93 Zr, 99 Tc, 90 Sr at environmental

Unique Infrastructure in Munich 53 Mn, 93 Zr, 99 Tc, 90 Sr at environmental concentration require high energies (150 – 200 Me. V) 12 MV min. Tandem Accelerator MLL, Munich or ANU, Canberra, Australia 21. 09. 2015 Karin Hain 9

Unique Infrastructure in Munich 53 Mn, 93 Zr, 99 Tc, 90 Sr at environmental

Unique Infrastructure in Munich 53 Mn, 93 Zr, 99 Tc, 90 Sr at environmental concentration require high energies (150 – 200 Me. V) Detection of 237 Np relative to spike Spike material commercially not available! 21. 09. 2015 12 MV min. Tandem Accelerator Karin Hain 10

Unique Infrastructure in Munich 53 Mn, 93 Zr, 99 Tc, 90 Sr at environmental

Unique Infrastructure in Munich 53 Mn, 93 Zr, 99 Tc, 90 Sr at environmental concentration require high energies (150 – 200 Me. V) Detection of 237 Np relative to spike Spike material commercially not available! 21. 09. 2015 12 MV min. Tandem Accelerator Karin Hain Production of non-commercial spike material e. g. 235 Np (TH = 1. 09 a) 11

Unique Infrastructure in Munich Chemical purification & characterization of spike material at Radiochemistry Munich

Unique Infrastructure in Munich Chemical purification & characterization of spike material at Radiochemistry Munich 53 Mn, 93 Zr, 99 Tc, 90 Sr at environmental concentration require high energies (150 – 200 Me. V) Detection of 237 Np relative to spike Spike material commercially not available! 21. 09. 2015 12 MV min. Tandem Accelerator Karin Hain Production of non-commercial spike material e. g. 235 Np (TH = 1. 09 a) 12

Preparatory Works: actinides Aim: • Distribution of Pu & Np in ocean water Chemical

Preparatory Works: actinides Aim: • Distribution of Pu & Np in ocean water Chemical behaviour With AMS: ü Small sampling volume: 20 L ü Improve 237 Np data ü No chemical separation required? KIT (F. Quinto) - Around 50% error in 237 Np measurements 21. 09. 2015 Karin Hain 237 Np a conservative tracer? 13

Preparatory Works: 93 Zr Master thesis in collaboration with TU Vienna Result: ü Sensitivity

Preparatory Works: 93 Zr Master thesis in collaboration with TU Vienna Result: ü Sensitivity reached 93 Zr/Zr = 2 x 10 -10 ü Best sensitivity worldwide - Low detection efficiency 21. 09. 2015 Karin Hain 14

Preparatory Works: Antarctica Samples 0. 5 t of snow from Antartica collected by Alfred-Wegener-Institut

Preparatory Works: Antarctica Samples 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 21. 09. 2015 Karin Hain 15

Required Investments • 2 clean laboratories for sample preparation 400. 000 € • Automatized

Required Investments • 2 clean laboratories for sample preparation 400. 000 € • Automatized accelerator control 200. 000 € • New injector including Multi-cathode Ion Source 100. 000 € + Bouncing Magnet 200. 000 € • Silicon Strip Detector 60. 000 € • Focusing lense 100. 000 € • MICADAS System for complementary Analysis 2. 000 € 3. 060. 000 € 21. 09. 2015 Karin Hain 16

MICADAS MIni CArbon DAting System 3. 4 m x 2. 6 m x 2

MICADAS MIni CArbon DAting System 3. 4 m x 2. 6 m x 2 m www. ionplus. ch 21. 09. 2015 Karin Hain 17

Required Investments • 2 clean laboratories for sample preparation 400. 000 € • Automatized

Required Investments • 2 clean laboratories for sample preparation 400. 000 € • Automatized accelerator control 200. 000 € • New injector including Multi-cathode Ion Source 100. 000 € + Bouncing Magnet 200. 000 € • Silicon Strip Detector 60. 000 € • Focusing lense 100. 000 € • MICADAS System for complementary Analysis 2. 000 € 3. 060. 000 € 21. 09. 2015 Karin Hain 18

Collaboration Partners National • • • Radiochemie München, TUM Alfred Wegener Institut, Bremerhaven Geomar,

Collaboration Partners National • • • Radiochemie München, TUM Alfred Wegener Institut, Bremerhaven Geomar, Kiel Institut für nukleare Entsorgung, KIT Institut für Umweltphysik, Universität Bremen Helmholtzzentrum Dresden-Rossendorf International • • • 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 21. 09. 2015 Karin Hain 19

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21. 09. 2015 Karin Hain 21

AMS Setup at the MLL 90° Analyzing Magnet (2 nd Mass Separation) 7 m

AMS Setup at the MLL 90° Analyzing Magnet (2 nd Mass Separation) 7 m 2. Wien Filter TOF Start − − Positive Ions Negative Ions Switching Magnet Gas-filled Analyzing Magnet System Current projects: 60 Fe, 53 Mn, 41 Ca, 93 Zr, 99 Tc − Wien Filter Faraday Cup TOF Stop Carbon Stripper Foil Faraday Cup 18°Electrostatic Deflection Sample 21. 09. 2015 90° Injector Magnet (1 st Mass Separation) Karin Hain 22

E (ch) 242 Pu 5· 109 atoms 240 Pu E (ch) IAEA-443: spectra 239

E (ch) 242 Pu 5· 109 atoms 240 Pu E (ch) IAEA-443: spectra 239 Pu TOF (ch) 238 U TOF (ch) 21. 09. 2015 Karin Hain 23

Fission Products W. Koelzer, Lexikon zur Kernenergie; FZK, 2011 21. 09. 2015 Karin Hain

Fission Products W. Koelzer, Lexikon zur Kernenergie; FZK, 2011 21. 09. 2015 Karin Hain 24

Emissions from La Hague & Sellafield Liquid I-129 emissions • Discharges from reprocessing plants

Emissions from La Hague & Sellafield Liquid I-129 emissions • Discharges from reprocessing plants very well known Emissions of selected isotopes • Peaks in release of long-lived isotopes (e. g. Tc-99) can be traced over many decades H. Nies et al, Report, Hamburg, 2008 21. 09. 2015 Karin Hain 25

Previous investigations with I-129 Measurements Alfimov et al. 2004 Results: H. Nies et al,

Previous investigations with I-129 Measurements Alfimov et al. 2004 Results: H. Nies et al, Report, Hamburg, 2008 21. 09. 2015 Karin Hain 26

Future plans BUT: Circulation of I-127 extremely complex, can be hardly described by transportation

Future plans BUT: Circulation of I-127 extremely complex, can be hardly described by transportation models H. Nies et al, Report, Hamburg, 2008 Conv. Methods e. g. activity measurement AMS 1 l 50 l-100 l 21. 09. 2015 Karin Hain 27

Sample Preparation 20 mg natural, metallic Zr Forschungsreaktor Muenchen II Radiochemie Muenchen Irradiated for

Sample Preparation 20 mg natural, metallic Zr Forschungsreaktor Muenchen II Radiochemie Muenchen Irradiated for 18 h + 2 Zr foils as Flux monitor Meier-Leibnitz-Laboratorium 21. 09. 2015 Karin Hain 28

Isotopic ratios before the accident 2 main contributions • global fallout 240 Pu/ 239

Isotopic ratios before the accident 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) 21. 09. 2015 Credit: J. Zheng et al, Geochemical Journal, Vol 46, pp 361 – 369, 2012 Karin Hain 29

GAMS Beamline Working Principle of the GAMS In evacuated Magnet: Using gas-filled 135° Dipole

GAMS Beamline Working Principle of the GAMS In evacuated Magnet: Using gas-filled 135° Dipole Magnet 21. 09. 2015 Karin Hain 30

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