Production and separation of 163 Ho Ulli Köster Institut Laue Langevin Grenoble, France
A bit of history A bit of history A bit of history A bit of history
First ISOL experiment at Niels Bohr Institute First ISOL experiment at Niels Bohr Institute First ISOL experiment at Niels Bohr Institute First ISOL experiment at Niels Bohr Institute ISOL beams of 89 89- -93 93 Kr ISOL beams of ISOL beams of ISOL beams of 89 89 - - 93 93 Kr Kr Kr O. Kofoed O. Kofoed- O. Kofoed O. Kofoed - - -Hansen and K.O. Nielsen, Hansen and K.O. Nielsen, Hansen and K.O. Nielsen, Hansen and K.O. Nielsen, Mat. Fys. Medd. Dan. Vid. Selsk. 26, Mat. Fys. Medd. Dan. Vid. Selsk. 26, Mat. Fys. Medd. Dan. Vid. Selsk. 26, Mat. Fys. Medd. Dan. Vid. Selsk. 26, Nr. 7 (1951). Nr. 7 (1951). Nr. 7 (1951). Nr. 7 (1951).
Conclusions υ υ Mass 1951 υ υ Conclusions Mass 1951 Conclusions Conclusions Mass 1951 Mass 1951 • neutrino physics experiments are highly neutrino physics experiments are highly neutrino physics experiments are highly neutrino physics experiments are highly interdisciplinary interdisciplinary interdisciplinary interdisciplinary • radioactive sources can be obtained in the radioactive sources can be obtained in the radioactive sources can be obtained in the radioactive sources can be obtained in the intensity and purity required intensity and purity required intensity and purity required intensity and purity required • υ υ mass experiment limited by detector: υ υ mass experiment limited by detector: mass experiment limited by detector: mass experiment limited by detector: resolution, accuracy resolution, accuracy resolution, accuracy resolution, accuracy
υ Mass 1982 : 163 Ho decay υ υ υ
υ Mass 1982 : 163 Ho decay υ υ υ
υ Mass 1982 : 163 Ho decay υ υ υ
υ Mass 1982 : 163 Ho decay υ υ υ • 600 MeV proton induced spallation of Ta target • surface ionization ⋅ 10 15 atoms • on-line mass separation at ISOLDE: 1.36 ⋅ ⋅ ⋅ • twice ion exchange chromatography (yield 44%) • total decontamination factor 10 14 - 10 15 ⋅ 10 13 atoms) • vacuum evaporation on Ta (3.1 ⋅ ⋅ ⋅ ⋅ 10 13 atoms) and Be backing (4.5 ⋅ ⋅ ⋅ • source characterisation with tracer, MWPC and RBS J.U. Andersen et al., Phys. Lett. 113B (1982) 72. B. Jonson et al., Nucl. Phys. A396 (1983) 479c.
υ Mass 1982 : 163 Ho decay υ υ υ • reactor irradiation of enriched 162 Er • multiple ion exchange chromatography • ion implantation in Aarhus at 500 keV (+channeling) and 2 MeV into Si detector • measurement of N/M capture ratio • Q EC = 2.82+0.11/-0.08 keV A. Laegsgaard et al,, Proc. AMCO-7, 3-7 Sep 1984, Darmstadt.
Conclusions υ υ Mass 1982 υ υ • neutrino physics experiments are highly interdisciplinary • radioactive sources can be obtained in the intensity and purity required υ mass experiment limited by detector: • υ υ υ resolution, count rate capability
Isotope selection 163 Ho Z N
Comparison of production routes Targ. Reaction E proj. I t irr m Nat. [1 MBq] targ. abund. ( µ µ µ µ A) (MeV) (d) (g) (%) 163 Dy (p,n) 16 100 23 0.4 24.9 164 Dy (p,2n) 30 100 2 1 28.3 164 Er (p,2n)EC-EC 30 100 2 1 1.6 166 Er (p,4n)EC-EC 70 100 0.5 5 33.5 ( α α ,2n)EC α α 163 Dy 40 50 26 0.2 24.9 ( α α α ,3n)EC α 164 Dy 50 50 14 0.3 28.3 159 Tb ( 7 Li,3n)EC 45 50 150 0.07 100 All following with mass separation, 10% overall efficiency. 181 Ta Spallation 1400 2 60 250 100 181 Ta Spallation 800 100 0.3 500 100 (n, γ γ γ )EC γ 162 Er 25E-9 “200” 100 0.003 0.14
Where is the challenge?
Cancer and efficiency of treatments At time of diagnosis Primary With Total tumor metastases Diagnosed 58% 42% 100% Cured by: Surgery 22% Radiation therapy 12% Surgery+radiation therapy 6% All other treatments and 5% combinations incl. chemotherapy Total cured 40% 5% 45% Fraction cured 69% 12% 45% Per year over one million cancer deaths in the EU. ⇒ improve early diagnosis ⇒ improve systemic treatments
Multidisciplinary collaboration to fight cancer Target antibody, antigen Linker peptide, peptide receptor etc. etc. Radionuclide Receptor Immunology Coordination Nuclear physics Structural biology chemistry and radiochemistry Roelf Valkema, EANM-2008.
Roelf Valkema, EANM-2008.
Lymphoma therapy: RITUXIMAB+ 177 Lu
Production of non-carrier-added 177 Lu 1. Irradiation of enriched isotope 176 Yb 2. Radiochemical Lu/Yb separation
Welding of irradiation container.
Fixation of irradiation shuttle in irradiation position.
Extraction of samples in hot cell.
Shipping to radiochemical lab
Radiochemistry: a challenge ? 2.0 ⋅ ⋅ ⋅ 10 18 atoms ⋅ 2.4 TBq (65 Ci) of 177 Lu 3.4 ⋅ ⋅ ⋅ 10 21 atoms ⋅ in 1 g of enriched 176 Yb chemical separation in <1 day radioisotopic purity >99.99% 2.1 ⋅ ⋅ ⋅ 10 18 atoms ⋅ 10 MBq of 163 Ho 3.7 ⋅ ⋅ ⋅ 10 19 atoms ⋅ in 10 mg of enriched 162 Er
Production of non-carrier-added 177 Lu 1. Irradiation of enriched isotope 176 Yb 2. Radiochemical Lu/Yb separation
Production of non-carrier-added 161 Tb 1. Irradiation of enriched 160 Gd 2. Radiochemical Tb/Gd separation S. Lehenberger et al., Nucl. Med. Biol. 38 (2011) 917.
Production of non-carrier-added 163 Ho 1. Irradiation of enriched 162 Er 2. Radiochemical Ho/Er separation 3. Optionally mass separation
?
Resonance Ionization Laser Ion Source Spectrochimica Acta B58 (2003) 1047 Ho ionization with 20% efficiency
Conclusions υ υ υ υ Mass 2013 • neutrino physics experiments are highly interdisciplinary • radioactive sources can be obtained in the intensity and purity required • υ υ mass experiment limited by detector: υ υ count rate capability, granularity, cross-talk
Conclusions υ υ υ Mass 2044 ? υ • 1951 – 1982 – 2013 – 2044 • major progress in neutrino mass experiments always takes a generation …
Reverse planning 163 Ho experiment present data at υ υ Mass 2016 υ υ 2016 2015 take data in 2015 04-05/2014 mass separation (implantation) at ISOLDE early 2014 chemical separation (MZ, PSI…) 07/2013 extraction of irradiated sample at ILL 13/06/2013 end of irradiation at ILL 19/02/2013 start of irradiation at ILL 15/02/2013 He leak test of irradiation shuttle 14/02/2013 welding of irradiation shuttle 13/02/2013 closing of irradiation capsules 11/02/2013 closing of irradiation ampoules decision to irradiate 162 Er at ILL 06/02/2013
6 February 2013 17:30-18:30 “Happy hour” Order 1 MBq of Order 1 MBq of Order 1 MBq of 163 Order 1 MBq of 163 Ho Ho now, Ho Ho now, now, now, 163 163 get one 1 MBq free! get one 1 MBq free! get one 1 MBq free! get one 1 MBq free!
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