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ACT Beamline

Background

The ACT-Beamline at ANKA is dedicated to actinide research with X-ray spectroscopic techniques. It will be operated by the Institute for Nuclear Waste Disposal (INE) the same way as the INE-Beamline.

 

INE Fig1 Immobilisation

Schematic sketch visualizing some of the actinide mobilization / retention processes possibly following actinide release from corroded HAW.

Research and development at INE are largely aimed at long term safety assessment of proposed deep geological repositories for high-level, heat producing nuclear waste (HAW) disposal. To ensure sound safety assessment, a molecular understanding of processes determinant in the fate of radionuclides, notably the actinides, and thermodynamic quantification is essential. Of central importance in such investigations is determination of actinide speciation (i.e., their chemical and physical form). X-ray spectroscopic methods have proved to be valuable tools for actinide speciation research. Investigations on non-fissile radioisotopes up to 106 times the legal exemption limit and fissile radioisotopes (Pu-239, U-235) up to 200mg, contained within two layers of protection, are possible.

The synchrotron-based activities at the ACT-Beamline are embedded in INE’s in-house research, thereby allowing a combination of analytical and instrumental methods, notably laser techniques and microscopic methods.

 

In situ X-ray spectroscopic investigations on radioactive samples will be routinely performed at the ACT-Beamline for studying, e.g., actinide containing solid-water interface chemical reactions, not possible at other facilities. The special protocol for working with radioactive samples at the INE-Beamline will be used as well for the ACT-Beamline and will be supervised by INE’s own radiation protection officers too. The unique aspect of the ACT-Beamline and INE-Beamline is their close proximity to INE’s active laboratories on-site KIT north campus.

 

The ACT-Beamline will serve three general functional areas:

  • Research = user facility (INE in-house, HGF NUSAFE program, via strategic research cooperation with KIT-INE)
  • Education and dissemination (maintaining nuclear competence)
  • Development & upgrades (adaption of methods, serving user needs)

 

 

 

Layout

 

Layout of the CAT-ACT beamline at ANKA with two in-line experimental stations

 

CAT-ACT optical components designed and manufactured by FMB Oxford (Oxford, United Kingdom). From right to left: frontend components (intensity absorber, X-ray beam position monitor, white beam slit), collimating mirror, double crystal monochromator, diagnostics module, toroidal focusing mirror, beam shutter separating ACT hutch from optics section. Inset: focusing mirror coating scheme.

Experiment

Detectors

 

Detector Type Main specs
Fluorescence

5 element LEGe (Canberra-Eurisys)

 

Ketek SDD

140 eV at 6 keV; 50 mm2 active area/element; 25 µm Be window

 

Absorption

3 ionization chambers (Poikat / Hamburg

low-energy set-up with single entrance window (Oken Ltd. ionization chambers, Japan)

window 12.5 or 25 µm KAPTON, FEMTO low current amplifiers DLPCA-200

ionization chambers and sample chamber form windowless volume – gas tight insertion of SDD into sample chamber for high quality fluorescence spectra


 

Sample holder (HUBER stage, combined with HRXES spectrometer):

 

Movement Range
z stage 90 mm; 50 nm/step
phi circle 360°; 0.001°/step
x stage 80 mm; 100 nm/step
y stage 80 mm°; 100 nm°/step



                    INE Fig4 microfocus
                   Setup for confocal measurements with a µ-focused beam at the INE-Beamline.

 

 

Sample environment

 

Standard holder for transmission and fluorescence measurements of radioactive and non-radioactive samples, e.g., 400 µl and 2 ml PE-tubes, pellets.

Liquid sample cell for the investigation of redox labile systems under electrochemically controlled conditions

Environment: atmosphere, inert gas (existing supplies: He, N2, Ar)

 

 

Methods available

 

 

XAFS characterization of bulk species by XANES/EXAFS
XAFS/XRD characterization of phase - pair distribution relationships
XRF measure elemental concentrations
High energy resolution (Johann spectrometer) HRXES: high resolution X-ray emission spectroscopy
RIXS:    resonant inelastic X-ray scattering
Combination of methods combined X-ray methods or X-ray method combined with other techniques, e.g., laser, Raman or UV/VIS spectroscopy

 

ACT characteristics

Radioactive work Infrastructure and licensing for activities 106 times the legal exemption limit as well as Pu-239 and U-235 up to 200mg.
Energy range 3.4 keV - 60 keV
Source 2.5 T superconducting multipole wiggler (Ec=10.2keV, K=11.2, 15mm vacuum gap, 4.7kW radiated power)
Optics • Double double crystal monochromator with Si(111) and Si(311) crystal pairs (fixed-exit, LN2 cooled crystals, direct drive goniometer with maximal speed of 4°/s)
• two mirrors for beam collimation, focusing and rejection of higher harmonics (vertically collimating
Si mirror coated with Rh and Pt stripes and toroidal focusing mirror with Rh and Ir stripes)

• Diagnostic modules
 
Beam size at sample position

~1mm × 1mm (standard beam size with mirror)

mirrorless operation above ~35keV

Flux at sample position ~1011  photons/s/100mA  at 20keV, Si(111)
Experimental set-up/ sample positioning

• Standard sample holders for radioactive samples, other dimensions can be accommodated
• High precision HUBER sample positioning system
• High Resolution X-ray Emission Spectrometer
• 1.2 × 3 m2 breadboard optical table
• Sealed media feed-through chicanes and separate ventilation / filter system for experimental hutch
• Access through lock-room with hand / foot-contamination monitor

Experimental set-up/ detectors • Ionization chambers for nominally high energies (transmission mode)
• Ionization chambers for nominally low energies (Oken Ltd, Japan)
• XRD-setup using image plates (autoradiography films)
• 5 pixel high purity germanium solid state fluorescence detector (Canberra Ultra-LEGe)
• Silicon drift detector (Ketek)
• Fully digital fluorescence detector read-out (XIA Xmap)
 
Publications
Title Author Source Date Link

A. Bremer, C. M. Ruff, D. Girnt, U. Müllich, J. Rothe, P. W. Roesky, P. J. Panak, A. Karpov, T. J. J. Müller, M. A. Denecke, A. Geist 

Inorganic Chemistry 51 (2012) 5199-5207 

2012 PDF

D. Girnt, P. W. Roesky, A. Geist, C. M. Ruff, P. J. Panak, M. A. Denecke 

Inorganic Chemistry 49 (2010) 9627-9635 

2010

K. Holliday, S. Handley-Sidhu, K. Dardenne, J. Renshaw, L. Macaskie, C. Walther, T. Stumpf 

Langmuir 28 (2012) 3845-3851 

2012 PDF

D. Prieur, P. Martin, F. Lebreton, T. Delahaye, D. Banerjee, A. C. Scheinost, A. Jankowiak 

J. Nucl. Mat. 434, 7-16 

2013 PDF

C. Walther, M. A. Denecke 

Chem. Rev. 113, 995-1015 

2013 PDF

T. Vitova, M. A. Denecke, J. Göttlicher, K. Jorissen, J. J. Kas, K. Kvashnina, T. Prüßmann, J. J. Rehr, J. Rothe 

J. Phys.: Conf. Ser. 430, 012117 

2013 PDF

J. Hu, A. Pohl, S. Wang, J. Rothe, M. Fichtner 

Journal of Physical Chemistry C 116 (2012) 20246-20253 

2012 PDF

A. Walshe, T. Prüßmann, T. Vitova, and Robert J. Baker 

Dalton Transact. DOI:10.1039/c3dt52437j 

2014 PDF

J. Majzlan, J.Plášil, R. Škoda, J. Gescher, F. Kögler, A. Rusznyak, K. Küsel, T.R. Neu, S. Mangold, J. Rothe

Environ. Sci. Technol. 48, 13685-13693

2014

PDF

E. Hartmann, B. Brendebach, R. Polly, H. Geckeis, T. Stumpf 

Journal of Colloid and Interface Science 353 (2011) 562-568 

2011
N. Finck, M. Bouby, K. Dardenne, H. Geckeis
Mineralogical Magazine 76(7) (2012) 2723–2740
2012 PDF

J. Rothe, B. Brendebach, C. Bube, K. Dardenne, M. A. Denecke, B. Kienzler, V. Metz, T. Prüßmann, K. Rickers-Appel, D. Schild, E. Soballa, T. Vitova 

J. Phys.: Conf. Ser. 430, 012114 

2013 PDF

N. L. Banik, B. Schimmelpfennig, C. M. Marquardt, B. Brendebach, A. Geist, M. A. Denecke 

Dalton Transactions 39 (2010) 5117-5122 

2010

U. Carvajal-Nunez, D. Prieur, T. Vitova, J. Somers 

Inorganic Chemistry 51 (2012) 11762-11768 

2012 PDF

B. Kienzler, V. Metz, B. Brendebach, N. Finck, M. Plaschke, Th. Rabung, J. Rothe, D. Schild 

Radiochimica Acta 98 (2010) 675-684 

2010

C. Bube, V. Metz, D. Schild, J. Rothe, K. Dardenne, M. Lagos, M. Plaschke, B. Kienzler 

Physics and Chemistry of the Earth, in press 

2013 PDF

T. Prüßmann, M. A. Denecke, A. Geist, J. Rothe, P. Lindqvist-Reis, M. Löble, F. Breher, D. R. Batchelor, C. Apostolidis, O. Walter, W. Caliebe, K. Kvashnina, K .Jorissen, J. J. Kas, J. J. Rehr, T. Vitova 

J. Phys.: Conf. Ser. 430, 012115 

2013 PDF

U. Carvajal Nunez, L. Martel, D. Prieur, E. Lopez Honorato, R. Eloirdi, I. Farnan, T. Vitova, J. Somers 

Inorg. Chem. 52, 11669-11676 

2013 PDF

M. W. Löble, P. Oña-Burgos, I. Fernández, C. Apostolidis, A. Morgenstern, O. Walter, F. Bruchertseifer, P. Kaden, T. Vitova, J. Rothe, K. Dardenne, N. L. Banik, A. Geist, M. A. Denecke, F. Breher 

Chem. Sci. 4, 3717-3724 

2013 PDF

M. Vespa, M. Rini, J. Spino, T. Vitova, J. Somers 

Journal of Nuclear Materials 421 (2012) 80-88 

2012 PDF

G. T. W. Law, A. Geissler, J. R. Lloyd, F. R. Livens, C. Boothman, J. D. C. Begg, M. A. Denecke, J. Rothe, K. Dardenne, I. T. Burke, J. M. Charnock, K. Morris 

Environmental Science & Technology 44 (2010) 8924-8929 

2010

G. L. Bovenkamp, A. Prange, W. Schumacher, K. Ham, A. P. Smith, J. Hormes 

Environ. Sci. Technol. 47, 4375-4382 

2013 PDF

D. Prieur, U. Carvajal-Nunez, T. Vitova, J. Somers 

Eur. J. Inorg. Chem. 2013, 1518-1524 

2013 PDF

M. Walter, J. Somers, D. Bouëxière, J. Rothe 

Journal of Solid State Chemistry 184 (2011) 911-914 

2011

T. Schäfer, M. A. Denecke 

AIP Conference Proceedings 1221 (2010) 181-187 

2010

B. Kosog, H. S. La Pierre, M. A. Denecke, F. W. Heinemann, K. Meyer 

Inorganic Chemistry 51 (2012) 7940-7944 

2012 PDF
A. H. Pohl, A. A. Guda, V. V. Shapovalov, R. Witte, B. Das, F. Scheiba, J. Rothe, A. V. Soldatov, M. Fichtner Acta Materialia 68, 179–188 2014

PDF

H. Curtius,G. Kaiser, K. Rozov, A. Neumann, K. Dardenne, D. Bosbach Clays and Clay Minerals 61, 424-439 2013 PDF

B. Fulda, A. Voegelin, K. Ehlert, R. Kretzschmar 

Geochimica et Cosmochimica Acta 123, 385-402 

2013 PDF

S. Heathman, J.-P. Rueff, L. Simonelli, M. A. Denecke, J.-C. Griveau, R. Caciuffo, G. H. Lander 

Physical Review B 82 (2010) 201103-1-4 

2010

N. Finck, K. Dardenne, D. Bosbach, H. Geckeis 

Environmental Science & Technology 46 (2012) 10004-10011 

2012 PDF

A. Leon, J. Rothe, H. Hahn, H. Gleiter 

Revue de métallurgie: Cahiers d'informations techniques 109 (2012) 35-39 

2012 PDF

R. Terzano, A. Santoro, M. Spagnuolo, B. Vekemans, L. Medici, K. Janssens, J. Goettlicher, M. A. Denecke, S. Mangold, P. Ruggiero 

Environmental pollution 158 (2010) 2702-2709 

2010

I. Denden, R. Essehli, M. Fattahi 

J. Radioanal. Nucl. Chem. 296, 149-155 

2013 PDF

X. Gaona, J. Tits, K. Dardenne, X. Liu, J. Rothe, M. A. Denecke, E. Wieland, M. Altmaier 

Radiochimica Acta 100 (2012) 759-770 

2012 PDF

G. Kuri, C. Degueldre, J. Bertsch, M. Doebeli 

Nuclear Instruments and Methods in Physics Research B 268 (2010) 2177-2180 

2010

P. Lindqvist-Reis, C. Apostolidis, O. Walter, R. Marsac, N. L. Banik, M. Y. Skripkin, J. Rothe, A. Morgenstern 

Dalton Transact. 42, 15275-15279 

2013 PDF

U. Carvajal Nuñez, R. Eloirdi, D. Prieur, L. Martel, E. López Honorato, I. Farnan, T.Vitova, J. Somers 

J. Alloys Comp. 589, 234-239 

2014 PDF

A. Diener, T. Neumann, U. Kramar, D. Schild 

Journal of Contaminant Hydrology 133 (2012) 30-39 

2012 PDF

I. Pidchenko, S. Salminen-Paatero, J. Rothe, J. Suksi 

J. Environm. Radioactivity 124, 141-146 

2013 PDF

O. N. Batuk, D. V. Szabó, M. A. Denecke, T. Vitova, S. N. Kalmykov 

Radiochim. Acta 101, 233-239 

2013 PDF

A. Diener, R. Köppe 

Journal of Crystal Growth 349 (2012) 55-60 

2012 PDF

J. Rothe, S. Butorin, K. Dardenne, M. A. Denecke, B. Kienzler, M. Löble, V. Metz, A. Seibert, M. Steppert, T. Vitova, C. Walther, H. Geckeis 

Review of Scientific Instruments 83 (2012) 043105-1-13 

2012 PDF
K. Holliday, K. Dardenne, C. Walther, T. Stumpf Radiochimica Acta 101, 267-272 2013 PDF

C. Walther, J. Rothe, B. Schimmelpfennig, M. Fuss 

Dalton Transactions 41 (2012) 10941-10947 

2012 PDF

U. E. Fittschen, G. Falkenberg 

Spectrochimica Acta Part B: Atomic Spectroscopy 66 (2011) 567-580 

2011

F. Huber, D. Schild, T. Vitova, J. Rothe, R. Kirsch, T. Schäfer 

Geochimica et Cosmochimica Acta 96 (2012) 154-173 

2012 PDF

M. A. Denecke, T. Petersmann, R. Marsac, K. Dardenne, T. Vitova, T. Prüßmann, M. Borchert, U. Bösenberg, G. Falkenberg, G. Wellenreuther 

J. Phys.: Conf. Ser. 430, 012113 

2013 PDF