esr3 wp2 d2 - indico · volume chromatography gas 1 gas 2 solid samples (mass markers) concept for...
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ESR3 – WP2 – D2.4
Target developments for extraction of actinides from thick ISOL targets followed by laser-induced molecular break-up and/or ionization.
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ESR3 – WP2 – D2.4
S.Rothe | LISA Kickoff CERN | ESR3 - Molecular Actinide Beams 2
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ESR3 – WP2 – D2.4
Objectives:
• Study and optimize the reaction conditions required to create volatile molecular species of refractory elements in general and actinides in particular.
• Develop a dissociation scheme for the provision of atomic species suitable for efficient laser ionization or in-source laser spectroscopy.
Expected results:
• Extraction of radiogenic actinide elements from an ISOL target and delivered in atomic form to the users. Determine the production yield and purity of the beams and report the new beam availability to the community.
Planned secondment(s):
• JGU (Christoph E. Düllmann) – M8-10 – working on the sample preparation to be used for the actinide molecular release studies;
• TRIUMF (Thomas Day Goodacre, Peter Kunz) – M15-17 – Extraction of actinides from thick targets at the ISAC facility. Participation in activities around radioactive ion beam development involving actinide beams and molecular beam extraction. Gaining experience in radioactive detection techniques used to assess the quantity and quality of the produced isotopes.
Enrolment in Doctoral degree:
• JGU in the Department of Chemistry under the supervision of Prof Christoph E. Düllmann
S.Rothe | LISA Kickoff CERN | ESR3 - Molecular Actinide Beams 3
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Outline
• Motivation for molecular beams
• Optimization of reaction conditions
• Develop a dissociation / ionization scheme
• Determine production yield
S.Rothe | LISA Kickoff CERN | ESR3 - Molecular Actinide Beams 4
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ISOLDE: Isotope Separation On Line
𝐵𝑒𝑎𝑚 𝐼𝑛𝑡𝑒𝑛𝑠𝑖𝑡𝑦 = 𝜎. 𝑗. 𝛮𝑡. 𝜀
𝜀 = 𝜺𝒅𝒊𝒇𝒇𝜺𝒆𝒇𝒇𝜺𝒊𝒔𝜺𝒔𝒆𝒑𝜺𝒕𝒓𝒂𝒏𝒔
𝑁𝑡 – Nr of exposed atoms [dim]
𝑗 – Proton flux [cm-2]
𝜎 – Cross section [mb]
𝜀 – Efficiency [%]
Extraction opticsMass separator
Target unit
1.4GeV Protons
4. Ionization
3. Effusion
2. Diffusion
1. Production
5. Mass Separation
6. Transport
(pulsed)
Protons
+/- 8V500 A
+/- 9 V1000 A
Ion
Source
Proton
Transfer
line
Extraction
electrode
up to 2300 °C20 cm
Target heating (1 – 2kW), <~10% beam power
Adapted from
S.Rothe | LISA Kickoff CERN | ESR3 - Molecular Actinide Beams 5
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boiling/melting points vs. ISOLDE Yields
actinides
TiB Mo
La
W Th
https://www.periodic-table.org/wp-content/uploads/2019/07/melting-and-boiling-point-chemical-elements-chart-min.png
S.Rothe | LISA Kickoff CERN | ESR3 - Molecular Actinide Beams 6
Target materials operated at < 2200 C
Si
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S.Rothe | LISA Kickoff CERN | ESR3 - Molecular Actinide Beams 7
Molecular Beams – Why?
• Beam purification
• Shift the mass region to a higher mass to avoid
isobaric contaminants. e.g. GeS, SnS, SeCO, LnO
• Beam extraction by In-situ volatilization
• Elements with very low volatility are not released
• Reactive elements can be chemically trapped
Target material
SeCO
8B 8BF3
SF6 (g)
Boron
Low Volatility (m.p. 2076 °C)
reactive with many metals
Boron trifluoride
gaseous even at RT
very stable
HSC simulation
Jochen Ballof | ISOLDE Workshop | 5.DEC.2017
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Optimize reaction conditions
• target material
• U vs. Th
• Metal vs. Carbide vs. Oxide
• target microstructure
• Investigate nano materials , stabilize nanostructure
• Reactive gas
• (O, F, S, …)
• Reaction conditions
• Concentrations, temperatures
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Thorium vs Uranium
S.Rothe | LISA Kickoff CERN | ESR3 - Molecular Actinide Beams 9
! Release properties to be studied
! Simulated results require validation
• ThC is a standard target material at ISOLDE
• Nano ThC possible with new nano lab
• co-development with SCK*CEN possibleFLUKA Simulations: : Joao Pedro Ramos
In-target production
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Nanomaterials
TiC+CB – J.P. Ramos, et al.
No
v-
20
14
No
v-
20
14
LaC2 + 2C – J. Guillot, et al.
No
v -
20
14
UC2 + 2C – A. Gottberg, et al.
Ap
r-2
01
5
MWCNT – C. Seiffert, et al.
SiC - S. Fernandes, et al.
20
10
*submicron
*1st
nanomaterial
at ISOLDE
2011
CaO – J.P. Ramos, et al.
João Pedro Ramos | 07/09/2017
MEDICIS-Promed Specialized Training on Radioisotope
Production
Adopted from
Study effects of reactive gas to actinide nano materials
S.Rothe | LISA Kickoff CERN | ESR3 - Molecular Actinide Beams
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Molecular Beams – The classical approach
U. Köster et al.
NIMB 266 (2008), 4229
EPJ-ST (2007), 285
1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18
1 2
H He
3 4 Halides Al-X Sulfides 5 6 7 8 9 10
Li Be B C N O F Ne
11 12 X-CO Oxides 13 14 15 16 17 18
Na Mg Al Si P S Cl Ar
19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36
K Ca Sc Ti V Cr Mn Fe Co Ni Cu Zn Ga Ge As Se Br Kr
37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54
Rb Sr Y Zr Nb Mo Tc Ru Rh Pd Ag Cd In Sn Sb Te I Xe
55 56 71 72 73 74 75 76 77 78 79 80 81 82 83 84 85 86
Cs Ba La... Hf Ta W Re Os Ir Pt Au Hg Tl Pb Bi Po At Rn
87 88 71 104 105 106 107 108 109 110 111 112 113 114 115 116 117 118
Fr Ra Ac... Rf Db Sg Bh Hs Mt Ds Rg Cn Nh Fl Mc Lv Ts Og
Selected molecular sidebands
Formation of molecules under low pressure conditions and high temperatures
S.Rothe | LISA Kickoff CERN | ESR3 - Molecular Actinide Beams
What are the best sidebands for actinide release ?
1st experiments planned with irradiated targets at MEDICIS
Slide adapted from: Jochen Ballof | ISOLDE Workshop | 5.DEC.2017
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Beyond Uranium
S.Rothe | LISA Kickoff CERN | ESR3 - Molecular Actinide Beams 12
UCx , 1.4GeV, Fluka
Neptunium
NpF6
BP: 55C239Pu: 1E7 /s
Plutonium
Study NpF6 release
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Pump stand (YPS1)
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Offline 1 (YOL1)
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Offline 2 (YOL2)
https://home.cern/news/news/experiments/isoldes-new-offline-2-source-nears-completion
Frontend, Separator magnet
RFQ-CB
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VADIS sourceHeated reaction
volume Chromatography
Gas 1
Gas 2
Solid Samples
(mass markers)
Concept for a dedicated development unit for molecular beams
RGA
MagnetFaraday
CupFaraday
CupScanner
Study chemical reactions
- Injection of gases and vapor of solid
samples into reaction volume
- Suppression by quartz and other materials
Parameters
- 2 gases, controllable flow rates
- 2 mass markers
- Controllable temperatures in reaction volume
and chromatography column
- Materials for chromatography and
- Materials in reaction volume (target matrix)
- better understanding of molecule formation
- improve reliability of existing beams, tailor new beams
Studying molecular beam formation
J.BallofS.Rothe | LISA Kickoff CERN | ESR3 - Molecular Actinide Beams 16
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VADIS sourceHeated reaction
volume Chromatography
Gas 1
Gas 2
Solid Samples
(mass markers)
Concept for a dedicated development unit for molecular beams
RGA
MagnetFaraday
CupFaraday
CupScanner
Studying molecular beam formation
• Move residual gas analyzer to identify
separated beam composition through
molecular break up patterns
JochenS.Rothe | LISA Kickoff CERN | ESR3 - Molecular Actinide Beams 17
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VADIS sourceHeated reaction
volume Chromatography
Gas 1
Gas 2
Solid Samples
(mass markers)
Concept for a dedicated development unit for molecular beams
MagnetFaraday
CupFaraday
CupScanner
Studying molecular beam formation
• Add Multi Reflection Time of Flight (MR-ToF)
mass spectrometer: allows ISOBAR separation.
• Collaboration with MIRACLS experiment launched
RGA
Cu
rte
sy: S
.Ma
lbru
no
t
Example TOF spectrum on mass 46
Ti
Sc
KCa
J.BallofS.Rothe | LISA Kickoff CERN | ESR3 - Molecular Actinide Beams 18
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First prototype for reaction chamber tested at YOL1
BaO + CF4 -> BaF2 + x -> BaF+
1 reacting gas
1 sample supply
Surface ionization
Leak valve
Reaction chamber
Externally heated
V.Samothrakis, M.Ballan, J.Ballof, D.Leimbach, B.Crepieux, S.Rothe et al.
Ion source
Gas supply
Multiple gasses
Plasma sources, Negative ions
3 gas lines to
new Frontends
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Photocathode source
VADIS source at ambient temperatureElectron generation by laser, not thermal evaporation
Motivation- Ionization of fragile molecules- No decomposition on hot surfaces- Diagnostic tool to measure ionization properties
Laser properties
(PHARROS)
Pulse length 265 fs
Power 4.5 W
Wavelength 343 nm
Rep. Rate 50 kHz
First Results: Mass spectrum of Mo(CO)6 + Kr
Two operation modes found
Photo cathode Direct laser breakup
Anode biased Anode off
Magnet 6A Magnet off
Krypton ionized Krypton not ionized
Mo(CO)3 predominant Mo(CO)5 predominant
Set up
J. Ballof, D. Leimbach, B.A. Marsh, A. Ringvall-Moberg, S. Rothe, T. Stora, S. Wilkins
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THE ISOLDE Yield station (YYS)
Proposal: install spare YYS2 at GLM
• Used for beam development
• Can be used in p.sharing mode
with minimal impact to ISOLDE
physics
• Opportunistic development, in-
source laser spectroscopy
• Upgrade (LS3…): integrate
MR-ToF-MS
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THX