Line intensities and Collisional-Radiative...
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Line intensities and Collisional-Radiative Modeling
H. K. Chung
(many slides from Y. Ralchenko & J. Seely presentations at ICTP-IAEA School in 2017)
http://indico.ictp.it/event/7950/other-view?view=ictptimetable https://www-amdis.iaea.org/Workshops/ICTP2017/
May 8th, 2019
Joint ICTP-IAEA School on Atomic and Molecular Spectroscopy in Plasmas Trieste, Italy
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INTRODUCTIONSpectroscopic observables of matter states
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Experimental X-Ray Spectra
What are the spectral lines? Can we determine the plasma temperature and density? Other plasma properties? Unexpected discoveries?
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Spectral Line Intensity (optically thin)
Einstein coefficient ortransition probability (s-1)
Upper state density (cm-3)
Photon energy (J)Energy emitted due to a specifictransition from a unit volumeper unit time
(almost) purelyatomic parametersstrongly depends
on plasma conditions ijijjij hANI ν⋅⋅=
j
i
Eij
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INGREDIENTS OF SPECTROSCOPIC ANALYSIS
5 fields of expertize to constitute plasma spectroscopic analysis
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1) A Complete Set of Atomic Data Energy levels of an atom
Continuum
Ground state of ion Z
Ground state of ion Z+1
B1
A3
A1
A2
BOUND-BOUND TRANSITIONS
A1→A2+hv2 Spontaneous emission
A1+hv1↔A2+ hv1+hv2 Photo-absorption or emission
A1+e1↔A2+e2 Collisional excitation or deexcitation
BOUND-FREE TRANSITIONS
B1+e→A2+hv3 Radiative recombination
B1+e↔ A2+hv3 Photoionization / stimulated recombination
B1+e1↔ A2+e2 Collisional ionization / recombination
B1+e1↔ A3 ↔A2+hv3 Autoionization / Dielectronic
Recombination (electron capture + stabilization)
Atomic Physics Codes: FAC, HULLAC, LANL, GRASP-2K
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2) Population Kinetics Modeling
∑∑≠≠
+−=maxmax N
ijjij
N
ijiji
i WnWndtdn
ijeijijeijijij nCnJBW γβ +++= ijeDRji
RRjiejiejijiijji nnDnJBAW δαα 2)( +++++=
Bij Stimulated absorption
Cij Collisional excitation
γij Collisional ionization
βij Photoionization (+st. recom)
Aij Spontaneous emission
Bij Stimulated emission
Dij Collisional deexcitation
αijDR Dielectronic recombination
αijRR Radiative recombination
δij Collisional recombination
The key is to figure out how to manage the infinite set of levels and transitions of atoms and ions into a model with a tractable set of levels and transitions that represents a physical reality! (Completeness + Tractability + Accuracy)
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3) Radiation Transport
• Radiation intensity I(r,n,v,t) is determined self-consistently from the coupled integro-differential radiation transport and population kinetic equations
),,,(),,,(),,,(),,,()]()/([ 1 tItttItc ννχνην nrnrnrnrn −=∇⋅+∂∂−
)1)(,(
)()()(])/([
/
/*
kThe
ikTh
ii
iijjjii ij
i
eTnn
ennnggn
νκκκ
κ
κν
ν
να
ναναχ
−
−
>
−+
−+−=
∑
∑∑∑
• Emissivity η(r,n,v,t) and Opacity χ(r,n,v,t) and are obtained with population densities and radiative transition probabilities
( ) ⎥⎦
⎤⎢⎣
⎡++= −−
>∑∑∑∑ kTh
ei
ikTh
ii ij
ijjji eTnnennggch //*23 ),()()()/(/2 νκκκ
κκ
νν νανανανη
Radiation field carries the information on atoms in plasmas through population distributions
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4) Line Shape Theory for Radiation Transport
• Line shape theory is a theoretically rich field incorporating quantum-mechanics and statistical mechanics
• Line shapes have provided successful diagnostics for a vast range of plasma conditions – Natural broadening (intrinsic) – Doppler broadening (Ti) – Stark broadening (Ne) – Opacity broadening – Resonance broadening (neutrals) Ground state of ion Z
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ννij
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5) Particle Energy Distribution
• Time scales are very different between atomic processes and classical particle motions : separation between QM processes and particle mechanics
• Radiation-Hydrodynamics simulations – Fluid treatment of plasma physics
• Mass, momentum and energy equations solved – Plasma thermodynamic properties – LTE (Local Thermodynamic Equilibrium) (assumed)
• PIC (Particle-In-Cell) simulations – Particle treatment of plasma physics
• Boltzmann transport and Maxwell equations solved – Electron energy distribution function – Simple ionization model (assumed)
Is this a valid assumption?
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First, identify lines and then obtain line intensities using a kinetics code and determine the temperature and density of the plasma emission region.
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POPULATION KINETICS MODELS
Statistical Distributions of Electronic Level Population Density 3 Representative Models
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(1) Thermodynamic equilibrium
! Principle of detailed balance– each direct process is
balanced by the inverse! radiative decay
(spontaneous+stimulated) ↔
photoexcitation! photoionization ↔ photorecombination
! excitation ↔ deexcitation
! ionization ↔ 3-body recombination
! autoionization ↔ dielectronic capture
Photons
Atoms Ions
Electrons
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TE: distributions
! Four “systems”: photons, electrons, atoms and ions! Same temperature Tr = Te = Ti
! We know the equilibrium distributions for each of them– Photons: Planck– Electrons (free-free): Maxwell– Populations within atoms/ions (bound-bound): Boltzmann– Populations between atoms/ions (bound-free): Saha
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Ener
gy
Continuum
Bound states
Maxwell
Saha
Boltzmann
Ionization energy
TE: energy scheme
Boltzmann: ⎟⎟⎠
⎞⎜⎜⎝
⎛ −−=
eTEE
gg
NN 21
2
1
2
1 exp
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Planck and Maxwell
! Planck distribution ! Maxwell distribution
( ) dETEE
TdEEf
eeM ⎟⎟
⎠
⎞⎜⎜⎝
⎛−= exp
2 2/12/32/1π
( )1
12/22
3
−= TEechEEB
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Saha Distribution
Z Z+1
AZ (+ e) ↔AZ+1 + e (+ e)
ionization3-body recombination
autoionizationdielectronic capture
∑−
−
−+
+
=
⎟⎠
⎞⎜⎝
⎛=
i
TEE
iZZ
TI
e
e
Z
ZZ
Z
e
i
e
Z
egg
eNh
mTgg
NN
0
,
2/3
21
1 122 π
Which ion is the most abundant?
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=+
Z
Z
NN ( )10~1>>
e
Z
TI
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Local Thermodynamic Equilibrium
• (Almost) never complete TE: photons decouple easily…therefore, let’s forget about the photons!
• LTE = Saha + Boltzmann + Maxwell
• Griem’s criterion for Boltzmann: collisional rates > 10*radiative rates
• Saha criterion for low Te:
[ ] [ ]( ) [ ]( ) 72/1301
143 104.1 ZeVTeVEcmN ee ∝Δ×>−
[ ] [ ]( ) [ ]( ) 62/12/5143 101 ZeVTeVIcmN eze ∝×>−
H I (2 eV): 2×1017 cm-3 C V (80 eV): 2×1022 cm-3
H I (2 eV): 1017 cm-3 C V (80 eV): 3×1021 cm-3
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LTE Line Intensities
! No atomic transition data (only energies and statistical weights) are needed to calculate populations
! Intensity ratio! Or just plot the intensities on a log scale:
⎟⎟⎠
⎞⎜⎜⎝
⎛ −−
Δ
Δ=
Δ
Δ=
eTEE
AEgAEg
AENAEN
II 21
222
111
222
111
2
1 exp
exp( / )
ln( / ) / ln( )
ii e
i i e
gI N A E AE E TG
I g AE E T G
= ⋅ ⋅ = −
= − −
Aragon et al, J Phys B 44, 055002 (2011)
Boltzmann plot
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Saha-LTE conclusions
• Collisions >> radiative processes – Saha between ions – Boltzmann within ions
• Since collisions decrease with Z and radiative processes increase with Z, higher densities are needed for higher ions to reach Saha/LTE conditions – H I: 1017 cm-3 – Ar XVIII: 1026 cm-3
ASD: can calculate Saha/LTE spectra!!!
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Deviations from LTE
• Radiative processes are non-negligible – LTE: coll.rates (~ne) >
10*rad.rates
• Non-Maxwellian plasmas • Unbalanced processes • Anisotropy • External fields • …
21R
adia
tive
(~n-
3 )
Collisional (~n
4)
Partial LTE (PLTE) for high excited states
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(2) The other limiting case:Coronal Equilibrium
Low electron densities!Aug 21, 2017
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Coronal Model
• High temperature, low density and optically thin plasmas (Jv = 0)
• Excitations (and ionization) only from ground state…
• …and metastables • Does require a complete set of
collisional cross sections • Do we have to calculate all direct and
inverse processes?..
x
x x
x
x
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Coronal Model
• Rates (Ne2) << Rates (Ne) << Rates
(spontaneous) – 3-body recombination not important – Collisional processes from excited levels
dominated by spontaneous radiative decays – Left with collisional processes from ground levels
and radiative processes from excited levels
• Atomic processes: – Collis. ionization (including EA), – Radiative recombination (including DR) – Collisional excitation – Radiative decay (including cascades)
• Ions basically in their ground state • Ionization decoupled from excitation
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x
x x
x
x
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Line Intensities under CE
Ng
N1
Rexc Arad
Balance equation:
ERNEANIANN
ARN
N
ANRN
excgrad
rad
eg
rad
excg
radexcg
==
==
=
1
1
1
vσ
I ∝ NeLine intensity does NOT depend on Arad!
small populations!
If more than one radiative transition:
Ng
Nj
∑
∑∑
∑
<
<<
<
==
==
=
jkkj
ijjgegijijjij
jiij
jgeg
jiij
excgj
jiijjexcg
AA
NNAENI
A
NN
ARN
N
ANRN
σ
σ
v
v
Also cascades may be important 25
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Ionization Balance in CE
Z Z+1
Electron-impact ionization: ∝Ne
Photo recombination and Dielectronic recombination: ∝Ne
DReRRe
ione
Z
Z
vNvNvN
NN
σσ
σ
+=+1
Independent of Ne!
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( )303~ <Ne
Z ZTI
Most abundant ion:
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Ionization Balance in a General Case
Z Z+1
Electron-impact ionization: ∝Ne
Photorecombination and Dielectronic recombination: ∝Ne 3-body recombination: ∝Ne
2
Z
Z
NN 1lg +
lgNe
Corona
Ne0 Saha
Ne-1
Ionization from excited states
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From Corona to PLTE
Collisional stronger
Radi
ativ
e st
rong
er
PLTE
Corona1/n3 n4
Griem limit: n ~140 ⋅ Z0.7
Ne2/17Te
1/17
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(3) Collisional-Radiative Model• Population distribution is obtained by rate
equations considering collisional and radiative processes, along with plasma effects
• Excited states are substantially populated and increase the total ionization by step-wise ionization processes
• The 3-body recombination to these states is proportional to n4 and Ne
2 and excited states can significantly enhance the total recombination.
• Plasma effects such as non-local radiation transport, fast particle collisions and density effects should be included in the model.
• Self-absorption (radiation pumping) should be included for treating radiative processes involving optically thick lines. Collisional-Radiative Model
Continuum
Ground state of ion Z
ion Z+1
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Basic rate equation
( ) ( )( ) ( ) ( )tStNTTNNtNtAdttNd
ieieˆˆ...,,,,ˆ,ˆ
ˆ+⋅=
⎟⎟⎟
⎠
⎞
⎜⎜⎜
⎝
⎛
=
...
...ˆ
,iZNN Vector of atomic states populations
Rate matrix Source function
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Off-diagonal: total rates of all processes between two levels Diagonal: total destruction rates for a level
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Basic rate equation (cont’d)
( )
( )
( )
( )
( ) ( )
( )
( )
i
ZZ Zk
cxkZZi
ionpkZZi
ionikZZi
ionekZZi
ZZ Zk
cxkZZi
dckZZi
rrkZZi
bkZZi
ij
radstjiZ
radspjiZ
dexchjiZ
dexcejiZ
ij
excpijZ
exchijZ
exceijZ
iZ
ZZ Zk
cxZikZ
ionpZikZ
ioniZikZ
ioneZikZkZ
ZZ Zk
cxZikZ
dcZikZ
rrZikZ
bZikZkZ
ij
radstjiZ
radspjiZ
dexchjiZ
dexcejiZjZ
ij
excpjiZ
exchjiZ
excejiZjZ
Zi
S
SSSS
BARRBRR
N
SSSSN
N
BARRN
BRRNdtdN
+
++++
++++
++++++
×−
++++
++++
++++
++=
∑∑
∑∑
∑∑
∑∑
∑∑
∑
∑
< ∈
−−−
< ∈
<
−−−−
>
−−−
< ∈
−−−
> ∈
>
−−−−
<
−−−
)
(
' '',',',',
' '',',',
3',
,,,,,,,
,
' ',',',','',
' ',',','
3,'',
,,,,,
,,,,
αααα
αααα
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CR model: features
1. Most general approach to population kinetics 2. Depends on detailed atomic data and requires a
lot of it… 3. Should reach Saha/LTE conditions at high
densities and coronal at low 4. May includes tens up to millions of atomic states
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CR model: questions to ask
1. What state description is relevant? 2. Which level of data accuracy is sufficient for this
particular problem? 3. How to calculate the rates? What is the source of
the data? 4. What are the most (and not so) important
physical processes? 5. Which plasma effects are important? Opacity?
IPD?
33
There is NO universal CR model for all cases
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Non-LTE plasmas have well documented problems for experiment and theory
Au M-shell emission Glenzer et al. PRL (2001)
1st Non-LTE workshop (1996) documented large differences between codes for Au
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Dielectronic Recombination and Excitation Autoionization
NLTE 6&7 Mean ion charges for Ar case, ne = 1012 cm-3
NLTE Workshops 6&7, Chung et al. HEDP 9, 645 (2013)
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Pressure ionization / Ionization Potential Depression of HED matter
• For dense plasmas, high-lying states are no longer bound due to interactions with neighbouring atoms and ions leading to a “pressure ionization”
• Ionization potentials are a function of plasma conditions
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K1L8 (MN)24
K2L7 (MN)24
0
1x106
2x106
3x106
4x106
5x106
6x106
8000 8050 8100 8150 8200 8250 8300 8350
300 eV <Z>=17.8
Emissivity[erg/s/Hz/cm
2 ]
Energy
(K1L6)M1 (K1L6)
Copper : Kα spectra Hot electron 1 MeV
SCFLY
FLYCHK
FLYCHK + (K1L6)M3 (K1L6)M2N1 (K1L6)M1N2 (K1L6)M2 (K1L6)M1N1
Completeness in Level Configurations• FLYCHK uses the minimal set of configurations for NLTE plasmas • For WDM matter the set of configurations need to be expanded
K2L8M18N5 (Z=33)
Bound
K1L8 M18N6
L-shell
K-shell
K2L8 M18N5
K2L7 M18N6
M-shell
K2L8 M17N6
K2L8 M16N7
K1L8 M16N8
K2L8 M15N8
K2L7 M16N8
~400 eV
~400 eV
K1L8 M17N7
K2L7 M17N7
HEDP 3, 57 (2007)
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0
1x106
2x106
3x106
4x106
5x106
6x106
8000 8050 8100 8150 8200 8250 8300 8350
300 eV <Z>=17.8
Emissivity[erg/s/Hz/cm
2 ]
Energy
(K1L6)M1 (K1L6)
Copper : Kα spectra Hot electron 1 MeV
SCFLY
FLYCHK
FLYCHK + (K1L6)M3 (K1L6)M2N1 (K1L6)M1N2 (K1L6)M2 (K1L6)M1N1
Completeness in Level Configurations for Dense Matter
HEDP 3, 57 (2007)For XFEL plasmas
Bound
K1L8 M4
L-shell
K-shell
K2L8 M3
K2L7 M4
K1L8 (MN)4 K1L7 (MN)5 K1L6 (MN)6 K1L5 (MN)7 K1L4 (MN)8 K1L3 (MN)9 K1L2 (MN)10 K1L1 (MN)11 K1 (MN)12
K2L7 (MN)4
K2L6 (MN)5 K2L5(MN)6
K2L4(MN)7 K2L3(MN)8
K2L2(MN)9 K2L1(MN)10
K2(MN)11
K0L8 (MN)5 K0L7 (MN)6 K0L6 (MN)7 K0L5 (MN)8 K0L4 (MN)9 K0L3 (MN)10 K0L2 (MN)11 K0L1 (MN)12 K0 (MN)13
•FLYCHK uses the minimal set of configurations for NLTE plasmas •For WDM matter the set of configurations need to be expanded
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Average charge states as a function of electron density
Stepwise excitation via excited states ! <Z> increase
3-body recombination via Rydberg states ! <Z> decrease
Pressure ionization of excited states and ionization potential depression ! <Z> increase
10 eV
100 eV
1 keV
475 eV
10 keV
4 keV
Krypton
FLYCHK
Te=0.5 eV-100 keV
Ne=1012-1024 cm-3
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LINE INTENSITY RATIO ANALYSIS
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Spectral Line Intensity (optically thin)
Einstein coefficient ortransition probability (s-1)
Upper state density (cm-3)
Photon energy (J)Energy emitted due to a specifictransition from a unit volumeper unit time
(almost) purelyatomic parametersstrongly depends
on plasma conditions ijijjij hANI ν⋅⋅=
j
i
Eij
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(partial-) LTE Line Intensities
! No atomic transition data (only energies and statistical weights) are needed to calculate populations
! Intensity ratio! Or just plot the intensities on a log scale:
⎟⎟⎠
⎞⎜⎜⎝
⎛ −−
Δ
Δ=
Δ
Δ=
eTEE
AEgAEg
AENAEN
II 21
222
111
222
111
2
1 exp
exp( / )
ln( / ) / ln( )
ii e
i i e
gI N A E AE E TG
I g AE E T G
= ⋅ ⋅ = −
= − −
Aragon et al, J Phys B 44, 055002 (2011)
Boltzmann plot
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Line Intensities under CE
Ng
N1
Rexc Arad
Balance equation:
ERNEANIANN
ARN
N
ANRN
excgrad
rad
eg
rad
excg
radexcg
==
==
=
1
1
1
vσ
I ∝ NeLine intensity does NOT depend on Arad!
If more than one radiative transition:
Ng
Nj
∑
∑∑
∑
<
<<
<
==
==
=
jkkj
ijjgegijijjij
jiij
jgeg
jiij
excgj
jiijjexcg
AA
NNAENI
A
NN
ARN
N
ANRN
σ
σ
v
v
43
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General ideas for line intensity ratio diagnostics
• Electron density – Collisional dumping (density-dependent
outflux) – Density-dependent influx
• Electron temperature – Different parts of Maxwellian populate different lines
(upper levels)
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j
i
t ~ 1/A
45
Why are the forbidden lines sensitive to density?
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Let put him into a formula:
g
12
Strong transition
E.g., resonance to intercombination lines in He-like ions
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Dielectronic satellites
1s2 – 1s2p: resonance lines in He-like ions
1s2nl – 1s2pnl: satellite to a resonance line (Li-like ion)
Main population mechanism: dielectronic capture (resonance process!)
1s2 + e ! 1s2lnl’ ! 1s2nl’ + hv
Also in H-like and other ions
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He-like lines and satellites
O.Marchuk et al, J Phys B 40, 4403 (2007)
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He-like Ar Levels and Lines
1s2 1S0
1s2s 1S0
1s2p 1P1
1s2s 3S1
1s2p 3P0
1s2p 3P1
1s2p 3P2
W
XY
Z
M2 E1 M1E1
2E1 E1+M
1
Line He0 Ar16+ Fe25+ Kr34+
W 1.8(9) 1.1(14) 4.6(14) 1.5(15)
Y 1.8(2) 1.8(12) 4.4(13) 3.9(14)
X 3.3(-1) 3.1(8) 6.5(9) 9.3(10)
Z 1.3(-4) 4.8(6) 2.1(8) 5.8(9)
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Ar XVII Line Ratios
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Density DependenceNe X Lyα and satellites 1snl-2pnl
1019
1021
3×1020
1020
Lyα
BA C
A. 1s2s 3S1 – 2s2p 3P0,1,2
B. 1s2p 3P0,1,2 – 2p2 3P0,1,2
C. 1s2p 1P1 – 2p2 1D2 (J satellite)
Collisions Dielectronic Capture
Radiative Decay
1s 2S
1s2p 3P
2s2p 3P2p2 3P
1s2s 3S
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1s2lnl satellites• 1l2l2l’
• 1s2s2p - 1s2s2 2S1/2 : • 1s2s2p(1P) 2P3/2 (s), 2P1/2 (t) • 1s2s2p(3P) 2P3/2 (q), 2P1/2 (r) • 1s2s2p(3P) 4P3/2 (u), 4P1/2 (v)
• 1s2p2 - 1s22p 2P1/2,3/2 :
• 1s2p2(1D) 2D3/2,5/2 (j,k,l)
• 1s2p2(3P) 2P1/2,3/2; 4P1/2,3/2,5/2
• 1s2p2(1S) 2S1/2
• 1s2lnl’ (n>2) • Closer and closer to w • Only 1s2l3l can be reliably
resolved • Contribute to w line profile
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Temperature diagnostics with Dielectronic Satellites
Ionization limit of 1snl
Ionization limit of 1s2nl
Li-like
He-like1s2
1s2pIonization limit of 1s2l Excitation rate for 1s2p ~
DC rate for 1s2l2lʹ ~
2/1Te TEW−
1s2p2l1s2p3l
2/3Te TEs−
Reminder: for (low-density) coronal conditions line intensity = population influx
Therefore: TTTE
IIW
s 1~
exp ⎟⎠⎞
⎜⎝⎛ Δ−
∝
Independent of ionization balance since the initial state is the same!
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Temperature Dependence: Lyα satellites
H-like Ne X100 eV
130 eV
160 eV
Lyα
1s2l-2l2lʹ
1s1/2-2p1/2
1s1/2-2p3/2
1snl-2lʹnl, n=2,3,4,…
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SPECTROSCOPIC ANALYSIS OF ION-BEAM PRODUCED NON-MAXWELLIAN ARGON PLASMAS
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Spectral Line Intensity (optically thick)
Einstein coefficient ortransition probability (s-1)
Upper state density (cm-3)
Photon energy (J)Energy emitted due to a specifictransition from a unit volumeper unit time
(almost) purelyatomic parametersstrongly depends
on plasma conditions I ij = Nj ⋅ Aij ⋅hν ij ⋅Pe
j
i
Eij
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Radiation escapeProbability
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Line Width Analysis of argon plasma influenced by opacity effects
• ne diagnostics are derived from Stark broadened line widths • Population kinetics needed for correct optical depths Statistical Fitting Analysis of Opacity- and Stark-Broadened Ar+2 Line Profiles Measured in Ion Beam Transport Experiments H.K. Chung et al, JQSRT, vol. 65, p. 135 (2000)
data
calc
Without Opacity With Opacity
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Line intensity and width analysis should include opacity effects
mean charge state
Without opacity effect
With opacity effect
• Analysis of measured spectra from the initial phase of the ion-beam plasma formation using NLTE populations reveals that IPROP (a PIC/Fluid hybrid code) using simple population model overestimates Te
• Note that IPROP uses a simple breakdown ionization model
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Using FLYCHK simulations: What Te and Ne to choose for the spectrum simulations? We know that the most abundant charge states in a thermal plasma have ionization potential ≈ 3Te , so choose Te ≈ 2 keV (1 keV?).
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FLYCHK Simulations of the Ga Spectrum with Te = 2 keV and Variable Ne
Low charge states too low
C is highest. Good
Lower charge states too high
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FLYCHK Simulations of the Ga Spectrum with Variable Te and Fixed NeNe=1x1019 cm-3
Low charge states too low
C is highest. Good
Lower charge states too high
He-like transitions and Li-like satellites have good intensities.
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FLYCHK simulations of the Ga spectrum were performed with variable Te, Ne, and hot electron fraction. The correlations between the calculated and experimental spectra were calculated. The highest correlation occurred for:
Te = 1100 eV ± 5%
Ne = 3x1019 cm-3 ± 50%
Fraction of hot electrons = 0.025 ± 0.005
0.955