Production and separation of 163 Ho Ulli Kster Institut Laue - - PowerPoint PPT Presentation

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Production and separation of 163 Ho Ulli Kster Institut Laue - - PowerPoint PPT Presentation

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Production and separation of 163 Ho Ulli Kster 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

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SLIDE 1

Production and separation of 163Ho

Ulli Köster Institut Laue Langevin Grenoble, France

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SLIDE 2

A bit of history A bit of history A bit of history A bit of history

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SLIDE 3

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 ISOL beams of ISOL beams of ISOL beams of 89

89 89 89-

  • 93

93 93 93Kr

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).
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Conclusions Conclusions Conclusions Conclusions υ υ υ υMass 1951 Mass 1951 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 υ υ mass experiment limited by detector: mass experiment limited by detector: mass experiment limited by detector: mass experiment limited by detector: resolution, accuracy resolution, accuracy resolution, accuracy resolution, accuracy

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SLIDE 5

υ υ υ υMass 1982 : 163Ho decay

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SLIDE 6

υ υ υ υMass 1982 : 163Ho decay

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SLIDE 7

υ υ υ υMass 1982 : 163Ho decay

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  • 600 MeV proton induced spallation of Ta target
  • surface ionization
  • on-line mass separation at ISOLDE: 1.36⋅

⋅ ⋅ ⋅1015 atoms

  • twice ion exchange chromatography (yield 44%)
  • total decontamination factor 1014 - 1015
  • vacuum evaporation on Ta (3.1⋅

⋅ ⋅ ⋅1013 atoms) and Be backing (4.5 ⋅ ⋅ ⋅ ⋅1013 atoms)

  • 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 υ υ υMass 1982 : 163Ho decay

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SLIDE 9
  • reactor irradiation of enriched 162Er
  • multiple ion exchange chromatography
  • ion implantation in Aarhus at 500 keV (+channeling)

and 2 MeV into Si detector

  • measurement of N/M capture ratio
  • QEC = 2.82+0.11/-0.08 keV
  • A. Laegsgaard et al,, Proc. AMCO-7, 3-7 Sep 1984, Darmstadt.

υ υ υ υMass 1982 : 163Ho decay

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SLIDE 10

Conclusions υ υ υ υMass 1982

  • neutrino physics experiments are highly

interdisciplinary

  • radioactive sources can be obtained in the

intensity and purity required

  • υ

υ υ υ mass experiment limited by detector: resolution, count rate capability

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SLIDE 11

Isotope selection

163Ho

N Z

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SLIDE 12
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SLIDE 13

Comparison of production routes

Targ. Reaction Eproj. (MeV) I (µ µ µ µA) tirr [1 MBq] (d) m targ. (g) Nat. abund. (%)

163Dy

(p,n) 16 100 23 0.4 24.9

164Dy

(p,2n) 30 100 2 1 28.3

164Er

(p,2n)EC-EC 30 100 2 1 1.6

166Er

(p,4n)EC-EC 70 100 0.5 5 33.5

163Dy

(α α α α,2n)EC 40 50 26 0.2 24.9

164Dy

(α α α α,3n)EC 50 50 14 0.3 28.3

159Tb

(7Li,3n)EC 45 50 150 0.07 100 All following with mass separation, 10% overall efficiency.

181Ta

Spallation 1400 2 60 250 100

181Ta

Spallation 800 100 0.3 500 100

162Er

(n,γ γ γ γ)EC 25E-9 “200” 100 0.003 0.14

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SLIDE 14

Where is the challenge?

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Cancer and efficiency of treatments

At time of diagnosis Primary tumor With metastases Total Diagnosed 58% 42% 100%

Cured by: Surgery 22% Radiation therapy 12% Surgery+radiation therapy 6% All other treatments and combinations incl. chemotherapy 5% Total cured

Fraction cured

40%

69%

5%

12%

45%

45% Per year over one million cancer deaths in the EU. ⇒ improve early diagnosis ⇒ improve systemic treatments

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SLIDE 16

Multidisciplinary collaboration to fight cancer

Roelf Valkema, EANM-2008.

Immunology Structural biology Coordination chemistry Nuclear physics and radiochemistry

Target antigen peptide receptor etc. Receptor Radionuclide Linker antibody, peptide, etc.

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SLIDE 17

Roelf Valkema, EANM-2008.

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SLIDE 18

Lymphoma therapy: RITUXIMAB+177Lu

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SLIDE 19

Production of non-carrier-added 177Lu

  • 1. Irradiation of enriched isotope 176Yb
  • 2. Radiochemical Lu/Yb separation
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SLIDE 20
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SLIDE 21
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SLIDE 22

Welding of irradiation container.

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SLIDE 23

Fixation of irradiation shuttle in irradiation position.

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Extraction

  • f samples

in hot cell.

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Shipping to radiochemical lab

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Radiochemistry: a challenge ?

2.4 TBq (65 Ci) of 177Lu 2.0⋅ ⋅ ⋅ ⋅1018 atoms in 1 g of enriched 176Yb 3.4⋅ ⋅ ⋅ ⋅1021 atoms chemical separation in <1 day radioisotopic purity >99.99% 10 MBq of 163Ho 2.1⋅ ⋅ ⋅ ⋅1018 atoms in 10 mg of enriched 162Er 3.7⋅ ⋅ ⋅ ⋅1019 atoms

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SLIDE 27

Production of non-carrier-added 177Lu

  • 1. Irradiation of enriched isotope 176Yb
  • 2. Radiochemical Lu/Yb separation
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Production of non-carrier-added 161Tb

  • 1. Irradiation of enriched 160Gd
  • 2. Radiochemical Tb/Gd separation
  • S. Lehenberger et al., Nucl. Med. Biol. 38 (2011) 917.
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SLIDE 29

Production of non-carrier-added 163Ho

  • 1. Irradiation of enriched 162Er
  • 2. Radiochemical Ho/Er separation
  • 3. Optionally mass separation
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SLIDE 30

?

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SLIDE 31

Resonance Ionization Laser Ion Source

Spectrochimica Acta B58 (2003) 1047

Ho ionization with 20% efficiency

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SLIDE 32

Conclusions υ υ υ υMass 2013

  • neutrino physics experiments are

highly interdisciplinary

  • radioactive sources can be obtained

in the intensity and purity required

  • υ

υ υ υ mass experiment limited by detector: count rate capability, granularity, cross-talk

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SLIDE 33

Conclusions υ υ υ υMass 2044 ?

  • 1951 – 1982 – 2013 – 2044
  • major progress in neutrino mass experiments

always takes a generation …

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Reverse planning 163Ho experiment

2016 present data at υ υ υ υMass 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 06/02/2013 decision to irradiate 162Er at ILL

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SLIDE 35

6 February 2013 17:30-18:30 “Happy hour”

Order 1 MBq of Order 1 MBq of Order 1 MBq of Order 1 MBq of 163

163 163 163Ho

Ho Ho Ho now, now, now, now, get one 1 MBq free! get one 1 MBq free! get one 1 MBq free! get one 1 MBq free!