single and multiple ionizaton of ions by electron and
TRANSCRIPT
Merged-Beams ExperimentsSingle and Multiple Ionizaton of Ions by
Electron and Photon Impact
Atom- und Molekülphysik I. Physikalisches Institut
JUSTUS-LIEBIG- UNIVERSITÄT GIESSEN
Photoionization of ions • ALS: Valence-shell ionization
• PIPE@PETRA III: Inner-shell ionization
detector based on secondary electron emission
e-
beam
reaction products • keV-beams of high directionality • high particle energies in lab frame
charge-changing collisions
Faraday cup
pioneered by Dolder et al. Proc. R. Soc. A 264 (1961) 367
other groups: Giessen, Louvain-La-Neuve, ORNL
Giessen Crossed-Beams-Setup
high-power electron gun
Emax = 3.5 keV, Imax = 1 A Ebinger et al., NIMB 408 (2017) 317
animated crossed-beams method absolute cross sections for
electron-impact ionization of ions typical systematic uncertainty <10%
A Fundamental Collision System: e- + Li+
www.uni-giessen.de/amp5
present experiment absolute present overview scan present threshold scan present CCC 13% m.s. + 87 % g.s. Berengut et al. RMPS 13% m.s.
A pp
ar en
Electron-ion collision energy ( eV )
1s 2 1 S
A. Borovik, Jr., A. Müller, S. Schippers, D. Fursa, I. Bray, JPB 42 (2009) 025203
comparison between measurements and CCC calculations for a mixture of Li+(1s2 1S) and Li+(1s 2s 3S) ions
Higher-Order Ionization Processes
www.uni-giessen.de/amp6
electron-impact ionization of metastable N5+(1s 2s 3S) experiment and CCC calculations
A. Müller et al., PRA 90 (2014) 010701(R)
450 500 550 600 650
7.4
7.6
7.8
8.0
s 3l2s 3
l 4 l'
300 400 500 600 700 800 900 1000 0.0
0.2
0.4
0.6
0.8
1.0
1.2
1.4
1.6
DI: 4s EA: 3d
DI: 4p
DI: 4d
0.0
0.5
1.0
1.5
2.0
2.5
EA: 3d
EA: 4s
Sn13+
Sn11+
Sn10+
Sn8+
Sn6+
Sn4+
www.uni-giessen.de/amp7
Ionization of Sn4+ - Sn13+ for EUV-Lithography
Sn ions: A. Borovik, Jr. et al., JPB 46 (2013) 175201 Xe ions: A. Borovik, Jr. et al., JPB 48 (2015) 035203
Importance of Indirect Ionization
D.-H. Zhang & D.-H. Kwon, JPB 47 (2014) 075202
excitations of up to at least n=25 have to be considered
see, e.g., also: D.-H. Kwon & D. W. Savin, PRA 86 (2012) 022701; V. Jonauskas et al., PRA 91 (2015) 012715; A. Borovik Jr. et al., PRA 93 (2016) 012708.
single ionization of Xe24+
P. Liu et al., PRA 92 (2015) 012701experimental data from Giessen
Cross Sections for Multiple Ionization
www.uni-giessen.de/amp9
0
20
40
60
0.0
0.5
1.0
0.05
0.10
The Giessen Electron-Ion Team
low ion densities: ~ 106 cm-3
long interaction region (~ 1 m) makes up for diluteness of ionic targets
recent review: Schippers, Kilcoyne, Phaneuf, Müller, Contemporary Physics 57 (2016) 215
Aq+
www.uni-giessen.de/amp11
photon-ion end-station at beamline 10.0.1, Covington et al., PRA 66 (2002) 062710
Valence-Shell Photoionization of W4+(5d2)
www.uni-giessen.de/amp12
A. Müller, S. Schippers, J. Hellhund, A. L. D. Kilcoyne, R. A. Phaneuf, B. M. McLaughlin, J Phys. B 50 (2017) 085007
ALS experiment
52-level calculation
730-level calculation
www.uni-giessen.de/amp13
ALS experiment 730-level calculation
statistical average over all 5d2 initial levels
see also Müller et al., J Phys. B 48 (2015) 235203 for W1+
and McLaughlin et al., J. Phys. B 49 (2016) 065201 for W2+ and W3+
Photons from PETRA III
the world‘s most brilliant 3rd generation synchrotron light source
petra3.desy.de
www.uni-giessen.de/amp15
S. Schippers et al., J. Phys. B 47 (2014) 115602
photons from beamline P04 • up to several 1014/s • E = 250 - 3000 eV • E/E up to 30,000
ions
www.uni-giessen.de/amp16
Justus-Liebig-Universität Gießen A. Borovik, T. Buhr, K. Holste, A. Müller, A. Perry-Sassmannshausen, S. Schippers
Universität Hamburg Friedrich-Schiller Universität Jena M. Martins, K. Mertens, S. Reinwardt R. Beerwerth, S. Stock, S. Fritzsche
Johann-Wolfgang-Goethe Universität Frankfurt R. Dörner, T. Jahnke, M. Schöffler, M. Waitz
DESY FS-SCS DESY FS-FL DESY FS-PE (P04) S. Bari, K. Schubert S. Klumpp M. Hoesch, K. Bagschik, J. Seltmann, F. Scholz, F. Trinter
FU Berlin HZB Max-Planck-Institut für Kernphysik, Heidelberg R. Flesch, E. Rühl, G. Ulrich J. Viefhaus A. Dorn, A. Wolf
Universität Kiel & DESY PTB ATOMKI, Debrecen, Hungary M. Schnell J. Ullrich L. Abrok, S. Ricz
Columbia Astrophysics Laboratory, Columbia University, New York, USA D.W. Savin
Advanced Light Source, Berkeley University of Nevada, Reno, USA A.L.D. Kilcoyne R. A. Phaneuf
Current BMBF “Verbundforschung”
www.uni-giessen.de/amp17
50
100
150
57 Fe
View of the Interaction Region
www.uni-giessen.de/amp19
www.uni-giessen.de/amp20
www.uni-giessen.de/amp21
0
10
6f
5f
10
experimental energy spread: 0.16 eV natural resonance width: ~0.6 eV
3d-1 nf resonances
S. Schippers et al., J. Phys. B 47 (2014) 115602 S. Schippers et al., J. Phys. B 48 (2015) 144003
J. Phys. B Highlights 2014 and 2015
stepwise collapse of f-wave functions
with increasing primary charge state
Inner-Shell Ionization of Astrophysically Relevant Ions
www.uni-giessen.de/amp22
2
4
6
8
10
12
Ni
e
Nuclear charge ZM. Asplund et al., Annu. Rev. Astron. Astrophys. 47 (2009) 481
L-shell ionization
K-shell ionization
www.uni-giessen.de/amp23
A. Müller et al., ApJ 836 (2017) 166
E = 500 meV PIPE has lead to a breakthrough in inner-shell ionization of ions
Yamaoka et al., PRA 65 (2001) 012709
Fe+: Experimental Cross Sections
hν + Fe+ → Feq+ + (q-1) e-
680 700 720 740 760 780 800 820 840 860 880 900 0.01
0.1
1
10
100
1000
q=2 q=3 q=4 q=5 q=6 q=7
Cr os
s se
ct io
n (k
b)
Photon energy (eV) S. Schippers et al., ApJ 849 (2018) 5
six orders
ofm agnitude
Accessible Energy Levels after 2p Excitation of Fe+(1s2 2s2 2p6 3s2 3p6 3d6 4s)
www.uni-giessen.de/amp25
Auger processes energetically impossible
Accessible Energy Levels after 2p Excitation of Fe+(1s2 2s2 2p6 3s2 3p6 3d6 4s)
www.uni-giessen.de/amp26
process
Auger processes energetically impossible
and higher charge states
1
10
experiment, E = 1 eV Hartree-Fock theory Verner et al., ADNDT
55 (1993) 233
Photon energy (eV)
S. Schippers et al., ApJ 849 (2018) 5
Charge-State Fractions
0.1
0.02
q=3
= Σ
700 750 800 850 900
3.0
3.5
4.0
q
www.uni-giessen.de/amp29
LS-coupling, Kaastra & Mewe, AAS 97 (2003) 443
High-Resolution Measurement
comparison with Hartree-Fock and Dirac-Fock theory theoretical curves shifted by -2.8 and 1.0 eV
E=0.1 eV
natural line widths: ~ 0.4 eV uncertainty of the energy scale: ~ 0.2 eV
0,0
1,0
2,0 hν + O- → O+ + 2e-
524 526 528 530 532 534 536 538 540 542 0,0
0,1
Cr os
s se
ct io
n (M
0.0
0.1
0.2
0.3
Cr os
s se
ct io
n (M
S. Schippers et al., PRA 94 (2016) 041401(R) (editors‘ suggestion)
photodetachment of O-
KLL-Auger decay
single Auger
double Auger
triple Auger
2s 2p
DESY Highlight 2015 A. Müller et al., PRL 114 (2015) 013002
(editors‘ suggestion)
0.5
1.0
PI of C4+(1s 2s 3S) - 2s 2p 3PJ resonances
A. Müller et al., Phys. Rev. A 98 (2018) 033416
resolving power E/E = 25 800
theoretical uncertainty of
resonance energy: 1meV
1
Cr os
s se
ct io
n (M
S. Klumpp et al., Phys. Rev. A 97 (2018) 033401
ionization of IH+ at the iodine 3d edge
molecular resonance
Cross sections for (multiple) ionization
Role of many-electron processes
Benchmarks for atomic structure and atomic collision theories
Thank you for your attention!
Single and Multiple Ionizaton of Ions by Electron and Photon Impact
Outline
Higher-Order Ionization Processes
The Photon-Ion Merged-Beams Technique
Photons from PETRA III
User Community & Collaborators
Mass/Charge Selection of Ions
First Results: 3d-Ionization of Xe Ions
Inner-Shell Ionization of Astrophysically Relevant Ions
K-Shell Ionization of Ne+ Ions
Fe+: Experimental Cross Sections
Accessible Energy Levels after 2p Excitation of Fe+(1s2 2s2 2p6 3s2 3p6 3d6 4s)
Accessible Energy Levels after 2p Excitation of Fe+(1s2 2s2 2p6 3s2 3p6 3d6 4s)
Fe+ Absorption Cross-Section
High-Resolution Measurement
Atom- und Molekülphysik I. Physikalisches Institut
JUSTUS-LIEBIG- UNIVERSITÄT GIESSEN
Photoionization of ions • ALS: Valence-shell ionization
• PIPE@PETRA III: Inner-shell ionization
detector based on secondary electron emission
e-
beam
reaction products • keV-beams of high directionality • high particle energies in lab frame
charge-changing collisions
Faraday cup
pioneered by Dolder et al. Proc. R. Soc. A 264 (1961) 367
other groups: Giessen, Louvain-La-Neuve, ORNL
Giessen Crossed-Beams-Setup
high-power electron gun
Emax = 3.5 keV, Imax = 1 A Ebinger et al., NIMB 408 (2017) 317
animated crossed-beams method absolute cross sections for
electron-impact ionization of ions typical systematic uncertainty <10%
A Fundamental Collision System: e- + Li+
www.uni-giessen.de/amp5
present experiment absolute present overview scan present threshold scan present CCC 13% m.s. + 87 % g.s. Berengut et al. RMPS 13% m.s.
A pp
ar en
Electron-ion collision energy ( eV )
1s 2 1 S
A. Borovik, Jr., A. Müller, S. Schippers, D. Fursa, I. Bray, JPB 42 (2009) 025203
comparison between measurements and CCC calculations for a mixture of Li+(1s2 1S) and Li+(1s 2s 3S) ions
Higher-Order Ionization Processes
www.uni-giessen.de/amp6
electron-impact ionization of metastable N5+(1s 2s 3S) experiment and CCC calculations
A. Müller et al., PRA 90 (2014) 010701(R)
450 500 550 600 650
7.4
7.6
7.8
8.0
s 3l2s 3
l 4 l'
300 400 500 600 700 800 900 1000 0.0
0.2
0.4
0.6
0.8
1.0
1.2
1.4
1.6
DI: 4s EA: 3d
DI: 4p
DI: 4d
0.0
0.5
1.0
1.5
2.0
2.5
EA: 3d
EA: 4s
Sn13+
Sn11+
Sn10+
Sn8+
Sn6+
Sn4+
www.uni-giessen.de/amp7
Ionization of Sn4+ - Sn13+ for EUV-Lithography
Sn ions: A. Borovik, Jr. et al., JPB 46 (2013) 175201 Xe ions: A. Borovik, Jr. et al., JPB 48 (2015) 035203
Importance of Indirect Ionization
D.-H. Zhang & D.-H. Kwon, JPB 47 (2014) 075202
excitations of up to at least n=25 have to be considered
see, e.g., also: D.-H. Kwon & D. W. Savin, PRA 86 (2012) 022701; V. Jonauskas et al., PRA 91 (2015) 012715; A. Borovik Jr. et al., PRA 93 (2016) 012708.
single ionization of Xe24+
P. Liu et al., PRA 92 (2015) 012701experimental data from Giessen
Cross Sections for Multiple Ionization
www.uni-giessen.de/amp9
0
20
40
60
0.0
0.5
1.0
0.05
0.10
The Giessen Electron-Ion Team
low ion densities: ~ 106 cm-3
long interaction region (~ 1 m) makes up for diluteness of ionic targets
recent review: Schippers, Kilcoyne, Phaneuf, Müller, Contemporary Physics 57 (2016) 215
Aq+
www.uni-giessen.de/amp11
photon-ion end-station at beamline 10.0.1, Covington et al., PRA 66 (2002) 062710
Valence-Shell Photoionization of W4+(5d2)
www.uni-giessen.de/amp12
A. Müller, S. Schippers, J. Hellhund, A. L. D. Kilcoyne, R. A. Phaneuf, B. M. McLaughlin, J Phys. B 50 (2017) 085007
ALS experiment
52-level calculation
730-level calculation
www.uni-giessen.de/amp13
ALS experiment 730-level calculation
statistical average over all 5d2 initial levels
see also Müller et al., J Phys. B 48 (2015) 235203 for W1+
and McLaughlin et al., J. Phys. B 49 (2016) 065201 for W2+ and W3+
Photons from PETRA III
the world‘s most brilliant 3rd generation synchrotron light source
petra3.desy.de
www.uni-giessen.de/amp15
S. Schippers et al., J. Phys. B 47 (2014) 115602
photons from beamline P04 • up to several 1014/s • E = 250 - 3000 eV • E/E up to 30,000
ions
www.uni-giessen.de/amp16
Justus-Liebig-Universität Gießen A. Borovik, T. Buhr, K. Holste, A. Müller, A. Perry-Sassmannshausen, S. Schippers
Universität Hamburg Friedrich-Schiller Universität Jena M. Martins, K. Mertens, S. Reinwardt R. Beerwerth, S. Stock, S. Fritzsche
Johann-Wolfgang-Goethe Universität Frankfurt R. Dörner, T. Jahnke, M. Schöffler, M. Waitz
DESY FS-SCS DESY FS-FL DESY FS-PE (P04) S. Bari, K. Schubert S. Klumpp M. Hoesch, K. Bagschik, J. Seltmann, F. Scholz, F. Trinter
FU Berlin HZB Max-Planck-Institut für Kernphysik, Heidelberg R. Flesch, E. Rühl, G. Ulrich J. Viefhaus A. Dorn, A. Wolf
Universität Kiel & DESY PTB ATOMKI, Debrecen, Hungary M. Schnell J. Ullrich L. Abrok, S. Ricz
Columbia Astrophysics Laboratory, Columbia University, New York, USA D.W. Savin
Advanced Light Source, Berkeley University of Nevada, Reno, USA A.L.D. Kilcoyne R. A. Phaneuf
Current BMBF “Verbundforschung”
www.uni-giessen.de/amp17
50
100
150
57 Fe
View of the Interaction Region
www.uni-giessen.de/amp19
www.uni-giessen.de/amp20
www.uni-giessen.de/amp21
0
10
6f
5f
10
experimental energy spread: 0.16 eV natural resonance width: ~0.6 eV
3d-1 nf resonances
S. Schippers et al., J. Phys. B 47 (2014) 115602 S. Schippers et al., J. Phys. B 48 (2015) 144003
J. Phys. B Highlights 2014 and 2015
stepwise collapse of f-wave functions
with increasing primary charge state
Inner-Shell Ionization of Astrophysically Relevant Ions
www.uni-giessen.de/amp22
2
4
6
8
10
12
Ni
e
Nuclear charge ZM. Asplund et al., Annu. Rev. Astron. Astrophys. 47 (2009) 481
L-shell ionization
K-shell ionization
www.uni-giessen.de/amp23
A. Müller et al., ApJ 836 (2017) 166
E = 500 meV PIPE has lead to a breakthrough in inner-shell ionization of ions
Yamaoka et al., PRA 65 (2001) 012709
Fe+: Experimental Cross Sections
hν + Fe+ → Feq+ + (q-1) e-
680 700 720 740 760 780 800 820 840 860 880 900 0.01
0.1
1
10
100
1000
q=2 q=3 q=4 q=5 q=6 q=7
Cr os
s se
ct io
n (k
b)
Photon energy (eV) S. Schippers et al., ApJ 849 (2018) 5
six orders
ofm agnitude
Accessible Energy Levels after 2p Excitation of Fe+(1s2 2s2 2p6 3s2 3p6 3d6 4s)
www.uni-giessen.de/amp25
Auger processes energetically impossible
Accessible Energy Levels after 2p Excitation of Fe+(1s2 2s2 2p6 3s2 3p6 3d6 4s)
www.uni-giessen.de/amp26
process
Auger processes energetically impossible
and higher charge states
1
10
experiment, E = 1 eV Hartree-Fock theory Verner et al., ADNDT
55 (1993) 233
Photon energy (eV)
S. Schippers et al., ApJ 849 (2018) 5
Charge-State Fractions
0.1
0.02
q=3
= Σ
700 750 800 850 900
3.0
3.5
4.0
q
www.uni-giessen.de/amp29
LS-coupling, Kaastra & Mewe, AAS 97 (2003) 443
High-Resolution Measurement
comparison with Hartree-Fock and Dirac-Fock theory theoretical curves shifted by -2.8 and 1.0 eV
E=0.1 eV
natural line widths: ~ 0.4 eV uncertainty of the energy scale: ~ 0.2 eV
0,0
1,0
2,0 hν + O- → O+ + 2e-
524 526 528 530 532 534 536 538 540 542 0,0
0,1
Cr os
s se
ct io
n (M
0.0
0.1
0.2
0.3
Cr os
s se
ct io
n (M
S. Schippers et al., PRA 94 (2016) 041401(R) (editors‘ suggestion)
photodetachment of O-
KLL-Auger decay
single Auger
double Auger
triple Auger
2s 2p
DESY Highlight 2015 A. Müller et al., PRL 114 (2015) 013002
(editors‘ suggestion)
0.5
1.0
PI of C4+(1s 2s 3S) - 2s 2p 3PJ resonances
A. Müller et al., Phys. Rev. A 98 (2018) 033416
resolving power E/E = 25 800
theoretical uncertainty of
resonance energy: 1meV
1
Cr os
s se
ct io
n (M
S. Klumpp et al., Phys. Rev. A 97 (2018) 033401
ionization of IH+ at the iodine 3d edge
molecular resonance
Cross sections for (multiple) ionization
Role of many-electron processes
Benchmarks for atomic structure and atomic collision theories
Thank you for your attention!
Single and Multiple Ionizaton of Ions by Electron and Photon Impact
Outline
Higher-Order Ionization Processes
The Photon-Ion Merged-Beams Technique
Photons from PETRA III
User Community & Collaborators
Mass/Charge Selection of Ions
First Results: 3d-Ionization of Xe Ions
Inner-Shell Ionization of Astrophysically Relevant Ions
K-Shell Ionization of Ne+ Ions
Fe+: Experimental Cross Sections
Accessible Energy Levels after 2p Excitation of Fe+(1s2 2s2 2p6 3s2 3p6 3d6 4s)
Accessible Energy Levels after 2p Excitation of Fe+(1s2 2s2 2p6 3s2 3p6 3d6 4s)
Fe+ Absorption Cross-Section
High-Resolution Measurement