Documente Academic
Documente Profesional
Documente Cultură
MINICOURSE Low Temperature Plasma Modeling & Simulation and Applications ~ June 25 (Fri) 14:00-17:00 ~
Yuki Sakiyama, Ph.D. (ysaki@berkely.edu) Research Associate Department of Chemical Engineering, University of California, Berkeley
Outline
1. Problem setting and goals 2. Fluid modeling of atmospheric pressure plasmas 3. Simulation of atmospheric pressure plasmas using COMSOL and MATLAB 4. Plasma chemistry in atmospheric pressure plasmas 5. Neutral gas dynamics in atmospheric pressure plasmas 6. Overview of available codes for simulating low-temperature non-equilibrium plasmas
Understanding the governing equations and boundary conditions COMSOL and MATLAB Plasma chemistry Gas flow and plasma interaction
dark
bright
Y. Sakiyama and D.B.Graves, J.Phys.D 39 3451 (2006) and J.Phys.D 39 3644 (2006)
2.1 Introduction
problem setting
species: electrons (e), positive heavy ions (i), neutrals (n) geometry: 1-D parallel plate, gap 2mm external voltage: RF(= 13.56 MHz) gas pressure: 1 atm (= 760 torr), static gas temperature: room temperature
e n
Which equations to be solved? What is the physical meaning of the governing equations? What is appropriate boundary conditions? How and where are the necessary parameters obtained?
( j = e, i, n)
( ne )
from (eq-1)
qj
j
n j t
+ q j j = R j ,l = 0
j j l
(eq-1) (eq-4')
from (eq-4) 0
n j E = qj t t j
(eq-1) + (eq-4) 0 E + q j j = 0 E + q j j = 0 t t j j
total current continuity equation
(eq-5)
n j t
+ j = R j ,l
l
( j = e, i, n)
local creation/loss
(eq-1)
Reaction term:
Rl = k r nl = k r nl nl = k r nl nl nl
( k [ s ]) ( k [ m s ]) ( k [ m s ])
r r r 1 3 1 6 1
n
( x ) t = n ( x ) ut ( x + x ) t = n ( x + x ) u t
x x x+x
(eq-2)
(eq-6)
(eq-7)
= nE Dn
10
( ne ) t
5 5 + e ne De = e E Qe-N 3 3
electron heating
(eq-3)
Qe-N =
l
Elth klr ni ni ni
me el kb k ne ng (Te Tg ) +3 mg e
(eq-8)
G.J. M. Hagelaar et al., Plasma Sources Sci. Technol. 14, 722 (2005) R.E. Robson, et al., Rev. Mod. Phys. 77, 1303 (2005)
11
neutrals (n) 0
diffusion (D) [m2s1] elastic collision rate coefficient (kel) [m3s1] inelastic collision rate coefficient (kr) [s1, m3s1, m6s1]
f ()
f (T)
f ()
f ()
f () or f (T)
f () or f (T)
12
[m ]
10 10 10 10
10
-2
10
-1
10
(eq-9)
EEDF
10 10 10
-2
-4
-6
10
20 30 40 energy [eV]
50
60
13
10 10
-12
diffusion mobility
0.8
-14
e [m /sV]
[m /s]
De [m /s]
10 10 10
-16
k
-18
ionization
6 8 2 4
-20
0.1
e = e ( ) , De = De ( )
k el = k el ( ) , k r = k r ( )
14
[m2 /Vs]
Bohr radius
(eq-10)
[atm] [g-mol]
polarizability
15
(eq-11)
Ti / Tg
10
N2
He
1 10
4 2 4 6 8
+
6 8
6 8
10
16
1/ 2
Lennard-Jones radius []
1
2 p LJ LJ
(eq-12)
collision integral [-]
LJ []
H He N O H2O N2 2.313 2.576 2.937 2.663 2.591 3.0985
LJ [-] 0.7713 0.6257 0.7298 0.7367 0.888 0.7487 NO O2 H2O2 N2O NO2 O3
LJ []
3.099 3.017 3.017 3.202 3.038 3.338
R.B. Bird, et al., Transport Phenomena (Wiley, New York, 2002), page 526 R.J. Kee, et al., Sandia Report SAND86-8246 (1986)
17
8kbTi 1 i n = ni + s i ni E mi 4 8kbTn 1 n n = nn mn 4
switching function
s =
1 (E n 0) 0 (E n < 0) 1 (E n < 0) 0 (E n 0) (eq-16)
E
i e e n e n
E
i
s =
G.J.M. Hagelaara, et al., Phys. Rev. E 62, 14521454 (2000) Y.B. Golubovskii, et al, J. Phys. D 35, 751 (2002)
18
E
i
~ 0.016 E th 2
(eq-17)
work function
[eV]
Al Fe Ni W Pt 4.25 4.31 4.5 4.54 5.32 He* He+ He2* He2+ N+
19
5 3
inward flux
(eq-18)
m ]
-3
ne (BC-1)
ne (BC-2)
4 3 2 1 0 0.0
(BC-2)
[10
17
density
(BC-1)
0.5
1.0 x [mm]
1.5
2.0
0.5
1.0 x [mm]
1.5
2.0
20
0 E = 0 r Ed + e s d s
dt
from Gausss law
(eq-19) (eq-20)
interface (s, s) dielectric gas E x 0 ld
= q j j
j
Ed =
s 0 Ld
Ed
21
EEDF (F0)
= 0 3 2 F0 d
= f (E)
10
18
energy [eV]
[m ] density
Table Fitting
-3
1 0.1
10
17
10
16
ne EEE LFA
ni
nn
10
10
10
10
10
10
15
0.0
0.5
1.0 x [mm]
1.5
2.0
22
ne e E
Dene
e e x
( ne ) t
e E = ( ne e E Dene ) E < 0
heating rate
EEE:
5 5 + e ne De = e E Qe-N ~ 0 3 3
Not negligible
Y. Sakiyama et al., J. Appl. Phys. 101, 073306 (2007) V.R. Soloviev et al., J. Phys. D 42, 15208 (2009)
23
24
3.1 Introduction
Problem setting
n j t + j = R j ,l
l
( j = e, i, n)
e n
j = n j j E D j n j ( j = e, i, n)
5 5 + e ne De = e E Qe-N 3 t 3 ( j = e, i, n) 0 E = q j n j
j
( ne )
How to set up and run a model in COMSOL? How to evaluate the simulation results? How to control the current/power, instead of voltage?
25
26
reaction rate
e, D e
27
28
29
normalized variables
1.5
nn
1.2
ne
ni
m ]
-3 17
1.0
ne
0.5
ni
density
[10
3 2
nn
1 0 2.0
0.0
100
200
300
400
500
0.0 0.0
0.5
number of RF cycles
1.0 x [mm]
1.5
30
computational environment
CPU: dual AMD Opteron 250 memory: 12 GB OS: Linux (OpenSuse)
31
RF
E + q j j dt (eq-22) t j
(eq-23)
32
2.0
1.5
current control
100
200
300
400
500
33
E. Stoffels et al., Plasma Phys. Control. Fusion 46, B167 (2004) Applications in biomedicine
34
Mesh size: 3 140 m Number of mesh: 3,000 5,000 Shape function: Lagrange-quadratic Number of DOF: 70,000 90,000 1 mm
= 30 m
needle RF (13.56 MHz) 1 mm axis of symmetry
35
36
Current properties
0.2 1.0
19
density [m ]
10 10 10 10
18
current [mA]
0.1
Idsp Ie Itotal
0.5
normalized voltage
-3
0.0
0.0
17
Iion
-0.1
16
Vext
-0.5
15
0.0
0.2
0.4
0.6
0.8
1.0
-0.2 0.0
0.2
0.4
0.6
0.8
-1.0 1.0
z [mm]
ft
37
0 12 -20 8 -40 4 -60 0 0.00 0.10 0.20 z [mm] joule heating inelastic loss elastic loss 0.30
Sheath
-1
-3 9
[1025 m-3s-1] 0 2 4 6 8 10
38
39
Current properties
1.5 1.0 1.0
20
10 10 10 10
19
current [mA]
density [m ]
-3
Ie
0.5
normalized voltage
Idsp
0.0
18
Iion
-0.5
17
Itotal
Vext
0.4 0.6 0.8 -1.0 1.0
16
0.0
0.2
0.8
1.0
0.2
ft
40
100 50 0 -50 -100 0.05 0.10 0.9 0.15 0.8 z [mm] joule heating inelastic loss elastic loss -150 0.20 1.0
Sheath
-1
4 3 2 1 0 -1 0.00 0.7
[1027 m-3s-1] 0 3 6 9 12 15
11
0.20 1.0
41
Treated surface 1 mm
Needle
Needle tip 1 mm
2D axisymmetric Minimum mesh size Number of finite element relative computational cost 3 m 4,000 1
Treated surface
42
10
19
metastables
density [m ]
-3
10
21
density [m ]
metastables
10
18
-3
10
20
10
17
positive ions
10
19
positive ions
10
16
10
18
electrons
10
15
electrons
0.4 0.6 0.8 1.0 10
17
0.0
0.2
0.0
0.2
0.4
0.6
0.8
1.0
43
1 mm He
1000 mW 300 mW 100 mW
27
10 10 10 10 10
26
25
24
23
22
0.0
44
10
20
21
10 density [m ]
-3
19
metastables density [m ]
-3
10
20
10
18
positive ions
10
19
10
17
10 electrons
18
electrons
positive ions
10
16
0.0
0.2
0.4
0.6
0.8
1.0
10
17
0.0
0.2
0.4
0.6
0.8
1.0
45
Time-averaged density
electron He2* density [m ]
10 10 10 10 10
21 20 19 18 17
21 20 19 18 17
He* He2+
He+ N2+
20
-3
1D spherical
power [mW]
15 10
density [m ]
10 10 10 10 10
5 0
-3
80
120
160
200
0.0
0.2
0.8
1.0
46
4.1 Introduction 4.2 Chemical reactions in fluid model 4.3 Example-1: simplified chemistry model for helium with impurity 4.4 Example-2: plasma chemistry in air 4.5 Tips for simulation with detailed chemistry model (advanced)
47
4.1 Introduction
48
e, D e
49
50
51
52
measured waveform
53
He R1
R2
He+ + R3
He2 + e He* + He
2He2* He2+ + 2He + e He2 + e He* + N2 N2+ + He + e He2* + N2 N2+ + 2He + e He2+ + N2 N2+ + He2* N2+ + e N2
Y B. Golubovskii, et al.,J. Phys. D 36, 39 (2003) Y. Sakiyama et al., J. Appl. Phys. 101, 073306 (2007)
54
T. Martens et al., Appl. Phys. Lett. 92, 041504 (2008) X. Yuan, et al., IEEE Trans. Plasma Sci., 31, 495 (2003)
55
56
Drexel, US
Berkeley, US
Max-Planck, DE
Model description
pulse-like plasmas 0D simulation (spatially uniform plasmas) pressure: 1 atm gas temperature: 300 K gas concentration: air with 30% humidity computational time: ~10 hours (Dual Opteron 250, 12GB Mem, comsol3.5a)
n j t
= R j ,l
l
on (100 ns)
1 cycle (100 s)
57
-1 -2 -3 -4 -5 -6 -7 -8 -9
Ox NxOy
neutrals
positive ions
negative ions
density fraction
10 10 10 10 10 10 10
HxOy Nx
+ HxOy + Ox
Ox HxOy
-
NxOy
electron
-7 -5
10
-9
10 time [s]
-7
10
-5
10
-9
10 time [s]
-7
10
-5
10
-9
10 time [s]
10
58
-1 -2 -3 -4 -5
O3
density fraction
10 10 10 10 10 10
O2 H2 N O OH NO
H2O2 HO2
N2O NO2
N2O5
-6 -7 -8
NO3
59
74%
O + O2 + M O3 + M
6%: O3 + OH HO2 + O2
60
41%: NO + O3 NO2 + O2
8%: N* + O2 NO + O*
30%: O + NO2 NO + O2
61
40%: NO + O3 NO2 + O2
62
63
Ns
heavy computation
Nr For example 40 species/700 reactions (air) one-dimensional, RF excitation 12 GB, Dual Opteron 250
64
R R n j = r + r kl n j kl (eq-26)
S jl =
n klr
sensitivity coefficient
R S jl = n j (jl) matrix
R klr
(eq-27)
(l1) matrix
low computational load perturbation around equilibrium state sensitivity dominant reaction path
H. Rabitz et al, Ann. Rev. Phys. Chem. 34, 419 (1983)
65
R11 L R1Ns O M lj = M R N r 1 L R Ns N r
normalized
reaction
(eq-28)
medium computational load directly evaluating reaction rate need of finding typical conditions
66
67
5.1 Introduction
Loughborough, UK
68
total momentum conservation: ( uui ) = p ( 0 ) g total energy conservation: mass conservation of air: perfect gas law:
69
neutral gas heat and mass transfer model gas temperature gas velocity gas component
background gas density mobility and diffusion coefficients for electrons/ions diffusion coefficients for neutrals reaction rate coefficients (including elastic energy loss) flux of species
70
(eq-34)
E N N i N N
(eq-6)
m j n j u j q j n j E p j (m j n j u j u j ) t j =i , e
71
(eq-35)
chemical reactions
external electrical power P = qe e E + qi i E (=Joule heating) source terms for EEE source terms for IEE
Se = qe e E Qe-N Qe-i
elastic collision
(~ 0)
72
f pls =
RF
RF
qi ni Edt ,
Qpls =
RF
RF
qi ni E dt
73
74
N2 density
c
75
mole fraction of N 2
N2 rich
10
He channel
0 -20
-10
10
20
30
40
50
He rich
76
He channel 0
pressure: 1 atm
ni 1 (ri ) + = Si t r r
(mass continuity)
77
nN2
Ez
0
Given electric field (not self-consistent!) Ez = 3105 V/m 400 ns 0 125 s (8 kHz)
reaction rate:
E=
Er + Ez
Poissons eq.
given
k = f (E)
78
79
80
200
400
time [ns]
600
800
1000
10 10
29
10 10
29
28
28
reaction rate [m s ]
10 10 10 10 10
27
reaction rate [m s ]
-3 -1
-3 -1
10 10 10 10 10
27
26
N2 e
26
25
25
24
24
23
23
0.0
0.5
1.0 r [mm]
1.5
2.0
0.0
0.5
1.0 r [mm]
1.5
2.0
81
inner diameter: 3 mm
82
+ + B2 u X 2 g
OH N2 N2
+
3 S , P, D 2 S , P
He He
He O
intensity
N2
N2
He
500 600 700
He
800
300
400
wavelength [nm]
N2+(B) He*, He2* (40%) kPen He2+ (75%) kchg Emission rate = kem ~ kPen+ kchg (kem >> kPen, kchg) kem N2+(X) kex kem
3SPD
2P 2S
Emission rate = kem ~ kex (kem >> kex) ~ kiz (kiz ~ kex)
83
r z 0
1.0
20 mm
40 mm
OES
0.8
Model
normalized intensity
-1
0 r [mm]
84
0.3 m/s
1.0 m/s
4 radial position
4 radial position
5 mm Killing pattern
J.Goree, et al, J. Phys. D. 39, 3479 (2006) and IEEE Trans.Plasma Sci. 34, 1317 (2006) (Images courtesy of Prof. John Goree)
85
(momentum conservation)
86
N2 (1atm)
glass plate 5 mm
87
1 mm
88
89
electrons
1019
He*
-0.5
1018 1017
1017
1016
-1 0.5 0 z [mm]
He2+ 1018
N2+
-0.5
1017 1016
1017 1.5 2 0 0.5 1 r [mm] 1.5 1016 2
-1
0.5
1 r [mm]
90
N2 e He gap: 3 mm
0 z [mm]
He
-0.5
-1 0
0.5
1 r [mm]
1.5 [1023
2 m-3s-1] 1
4 mm
0.2
0.4
0.6
0.8
91
off-axis
nair/nHe>10-3 S. mutans
off-axis
(2mm gap)
nair/nHe<10-5 S. mutans
92
20
He2+ O+
N+,N2+
density [m ]
-3
10 10 10 10 10
20
density [m ]
-3
10 10 10 10
19
H2O+,H+,OH+
19
18
18
17
NO+
17
16
16
0.0
0.2
0.4
0.6
0.8
1.0
0.0
0.5
1.0
1.5
2.0
r [mm]
r [mm]
93
20
N,N*,N2*
He*,He2* O,O*,O2*
density [m ]
-3
10 10 10 10 10
20
density [m ]
-3
10 10 10 10
19
19
18
H,OH,H2
18
NO H,OH,H2
17
17
16
16
0.0
0.2
0.4
0.6
0.8
1.0
0.0
0.5
1.0
1.5
2.0
r [mm]
r [mm]
94
OH
NO
95
flux [10 m s ]
-2 -1
10 8 6 4 2 0
19
N2
O2
12
flux [10 m s ]
-2 -1
10 8 6 4 2 0
19
e H N OH H2O N + 2 NO
+
O2
O2
96
3. HPEM: solver for low pressure plasma processing reactors (ICP, RIE, ECR, etc) developed and managed by CPSEG in U. Michigan (http://uigelz.eecs.umich.edu/)
97
5. ANSYS Fluent: general fluid dynamics solver applicable to low pressure CVD simulation ANSYS Inc. (http://www.ansys.com/)
6. COMSOL Multiphysics: FE (finite element) solver ~20 pre-defined application modules from fluid dynamics to mechanics plasma module included in the latest version 4.1 Comsol, Inc. (http://www.comsol.com/)
98
8. XPDP1, XPDP2, XPDS1: particle-in-cell (PIC) solver freeware developed and managed by PTSG group in UC Berkeley (http://ptsg.eecs.berkeley.edu/) 9. VORPAL, OOPIC Pro: PIC solver Tech-X corp. (http://www.txcorp.com/)
10. LSP Suite: 2-D and 3-D PIC solver Alliant Techsystems Inc. (http://www.mrcwdc.com/LSP/)
99
Notation
cp: specific heat [J kg1 K1] R: S: t: T: reaction rate [m3s1] sensitivity coefficient time [s] temperature [K]
D : diffusion coefficient [m2s1] e: electron charge (=1.601019) [C] Eth: ionization/excitation energy [eV] fpls: body force from plasmas [kg m s2] g: J: h: gravity (= 9.81) [m s2] current density [A m2] grid size [m]
kinel: reaction rate coefficient [s1, m3s1, m6s1 ] kel: elastic collision rate coefficient [m3 s1] kb: m: n: p: Boltzmann constant (=1.381023) [J K1] mass [kg] density [m3] pressure [Pa]
Qpls: heating from plasmas [W m3] Qe-N: collisional energy loss [W m3] Q: viscous heat dissipation [W m3]
100
Notation-2
: mean electron energy [eV] 0 : vacuum permittivity (=8.851012)
[CV1m1] E: electric field [V m1] : flux [m2s1] n: unit surface vector [-] : stress tensor [Pa] u: neutral gas velocity [m s1]
m: momentum transfer collision frequency [s1] : electron energy relaxation frequency [s1]