Low temperature plasma EPP 5BBB 06 12 2023

Experiments at low temperature

Motion in fast oscillating field
Motion in fast oscillating field
RF trap
Homogeneous electric field Inhomogeneous electric field
RF Ion Trap
RF Ion Trap
Effective potential
22-pole ion trap + +
+ ++ + + +
V
22-pole trap
22-pole trap
TV 22-pole Ion Trap
Ion trap
Ion trap
Experiment
RF trap –Multipole fields

Effective potentials
Actual potential
RF trap
22-pole

Effective potential
RF trap
Photodetachment O- and OH-
Histogram
Molecules
Photodetachment cross section
Molecules
Ion density distribution
Ion temperature
Energy distribution
No colisions
With collisions
 8-pole trap

Effective potential
8-pole trap
8-pole trap
Effective potential
8-pole trap
22-pole trap
Experiment
Radiative decay of ions in ion trap
Molecules
Molecules
22pole trap, reactions at 10 K
Measurement of the rate coefficient Decay curve
Para and ortho hydrogen
Association and clusters
Deuteration is
easy
2000
438
1800 D7 D9 20 s
D5
1600

1400

1200

1000
Counts per filling

800

600

400
D3 D11
200

0,0 2,0 4,0 6,0 8,0 10,0 12,0 14,0 16,0 18,0 20,0 22,0 24,0 26,0 28,0
Mass
Deuteration was not so easy
2000
436-440
D7
1800 D9
1600
D5 1s
2s
5s
1400
10 s
1200 20 s
Counts per filling

1000

800 D11
D13
600

400
D15
D3
200 D17

5,0 10,0 15,0 20,0 25,0 30,0 35,0 40,0

Mass
H-atom source
Energies
 H2 Be=60.80
Energies of H2 and D2 250
B

H2
200

1eV corresponds to ~ 11604K D2 Be=30.429

meV
150

HD Be=45.655 100
100 K

energy
50
D2
j E/meV E/in K 300K 250K 80K 35K low
0

H2 0 0 0 0.128 0.150 0.248 0.25 1/4 0 1 2 3 4 5

j
1 14.7 170.6 0.657 0.694 0.75 0.75 3/4
2 44 510.6 0.117 0.098 0.002 0
3 87 1009.5 0.092 0.055 0 0
4 145 1682.6 0.004 0.0016 0 0
5 215 2494.9 0.001 0.0002 0 0
D2 0 0 0 0.179 0.213 0.552 0.664 2/3
1 7.3 84.71 0.202 0.227 0.329 0.333 1/3 50

2 22 255.29 0.383 0.384 0.114 0.002 H2

40
3 44 510.6 0.115 0.098 0.004 0

meV
4 72 835.5 0.098 0.066 0.0001 0 30

5 108 1253.2 0.015 0.008 0 0

20

D2

energy
HD 0 0 0 1 10

1 11.04 128.1
0

2 33.05 383.4 0 1 2

j
H2 and D2 are taken from O. Wick dissertation
HD is calculated using Be from Herzberg and comparison with H2 from table
 H2 Be=60.80
Energies of H2 and D2 250
B

H2
200

1eV corresponds to ~ 11604K D2 Be=30.429

meV
150

HD Be=45.655 100
100 K

energy
50
D2
j E/meV E/in K 300K 250K 80K 35K low
0

H2 0 0 0 0.128 0.150 0.248 0.25 1/4 0 1 2 3 4 5

j
1 14.7 170.6 0.657 0.694 0.75 0.75 3/4
2 44 510.6 0.117 0.098 0.002 0
3 87 1009.5 0.092 0.055 0 0 1,0
p
p
f3 f3 EXP eH2
4 145 1682.6 0.004 0.0016 0 0 0,8
5 215 2494.9 0.001 0.0002 0 0

fractions f3
p
0,6 f3 EXP nH2
D2 0 0 0 0.179 0.213 0.552 0.664 2/3
1 7.3 84.71 0.202 0.227 0.329 0.333 1/3 0,4
Afterglow Discharge
2 22 255.29 0.383 0.384 0.114 0.002 0,2 o
p
f3 EXP nH2
f3
p
3 44 510.6 0.115 0.098 0.004 0 f3 EXP eH2
0,0
p
4 72 835.5 0.098 0.066 0.0001 0 f2
e
0,8 H2
5 108 1253.2 0.015 0.008 0 0

fractions f2
0,6
HD 0 0 0 1
0,4
1 11.04 128.1
0,2 n
2 33.05 383.4 H2
o
f2
H2 and D2 are taken from O. Wick dissertation 0,0
0 100 200 300
HD is calculated using Be from Herzberg and comparison with H2 from table T (K)
Decay curves
Exothermic reaction
Exothermic reaction
Endothermic reaction
Energies
Temperature dependence
Temperature dependence
k = f ( 0 k1,0 +  1k1,1 ) + (1 − f )( 0 k0,0 +  1k0,1 )
k = f ( 0 k1,0 +  1k1,1 ) + (1 − f )( 0 k0,0 +  1k0,1 )
Part 4B
De Broglie wave length

electrons

e (4K ) ~ 540 A ~ 54 x10 −9 m

e (1eV ) ~ 11.6 A ~ 1.16 x10 −9 m

e (mK ) ~ 3x10 4 A ~ 3x10 −6 m 104A

a0
 Collisions of electrons with atoms

Classical or quantum approach?

Electron:
1eV → v=5.9x107cm s-1
t~a0/v ~10-8/ 5.9x107=2x10-16s
~2A = 2x10-8cm de Broglie
Ar+:
1eV → v=2x105cm s-1
t~a0/v ~10-8/ 2x105~6x10-14s
~ 9x10-11cm de Broglie
 Understanding plasma
Collisions
Classification of collisions ➔ elastic
➔ inelastic

The concept of collision cross-section

dI=-NsIp dx
IP= I0 exp(- sNx)
Hypothetical gas of rigid spheres of cross section s

Slow decrease of interaction potential - Small deviation ….

→ problem with concept of integral cross section

Electronic and ionic impact phenomena

Volume 1 – Collisions of electrons with atoms
H.S.W. Massey and E.H.S.Burhop, Oxford, Clarendon Press, 1969
 Collisions of electrons with atoms – Ramsauer’s method
Lenard 1903
Akesson 1916
Ramsauer 1921

ATENUATION METHOD

dI=-NsIp dx
IP= I0 exp(- sNx)

N
I0(v) IP
Photo cathode
e-
Mono energetic electrons x
IP IP= I0 exp(- sNx)
Cross sections - details
 Frequencies of elastic collisions

dI=-NQIp dx
IP= I0 exp(- QNx)

I0(v) N.x IP

Q(v)
a0=0.53x10-8cm~0.5A
Radius of the first Bohr orbit of H atom

n~nvs
He

Collision Frequencies
Total collision cross sections comparison

Ar
Alkali metals
Ne, He (3eV)

s(v)
(0,3eV)

Ar

-
e (v) (3eV) Cs
Ne
(2eV)
Ar
(0.3eV)
Franck-Condon Principle This is for recombination ??!1
be careful

Franck-Condon Factors

P~<yinitial. yfinal>2.
Interaction of Electrons with Molecular ions
 Electron − molecule collision
calculations using the R-matrix
method
Jonathan Tennyson
Department of Physics and Astronomy
University College London
Dissociation of H2
 Processes: at low impact energies
Elastic scattering
AB + e AB + e
Electronic excitation
AB + e AB* + e
Vibrational excitation
AB(v”=0) + e AB(v’) + e
Rotational excitation
AB(N”) + e AB(N’) + e
Dissociative attachment / Dissociative recombination
AB + e A− + B
A + B−
Impact dissociation
AB + e A+B+e
All go via (AB−)** . Can also look for bound states
 Electron impact dissociation of H2
Important for fusion plasma and astrophysics

Low energy mechanism:

e− + H2(X 1Sg) e− + H2(b 3Su) e− + H + H
R-matrix calculations based on
adiabatic nuclei approximation
extended to dissociation
 Including nuclear motion` (within adiabatic nuclei
approximation) in case of dissociation
• Excess energy of incoming e−
over dissociating energy can be
split between nuclei and outgoing ds(Ein)
e− in any proportion. dEout

• Fixed nuclei excitation energy

changes rapidly with bondlength Determine choice of T-
matrices to be averaged
• Tunnelling effects significant
The energy balance method

D.T. Stibbe and J. Tennyson, New J. Phys., 1, 2.1 (1999).

Explicit adiabatic averaging over T-matrices using continuum functions
Need to Calculate:
• Total cross sections, s(Ein)
• Energy differential cross sections, ds(Ein)
dEout
• Angular differential cross sections, ds(Ein)
dq
• Double differential cross sections, d2s(Ein)
dqdEout

Required formulation of the problem

C.S. Trevisan and J. Tennyson, J. Phys. B: At. Mol. Opt. Phys., 34, 2935 (2001)
Collisional dissociation
Collisional dissociation

Dissociation cross section as a function of incoming electron

energy,Ein, and initial vibrational state, v.

Dissociation rate as a function of electron temperature and

initial H2 vibrational level. Note the log rate scale.
Collisional dissociation

Dissociation cross section as a function of incoming electron

energy,Ein, and initial vibrational state, v.

Dissociation rate as a function of electron temperature and

initial H2 vibrational level. Note the log rate scale.
Electron impact dissociation of H2
Effective threshold about 8 eV for H2(v=0)

Thermal rates strongly dependent on initial

H2 vibrational state

For v=0: Excess energy largely converted

to Kinetic Energy of outgoing H atoms
For v > 0: Source of cold H atoms ?
Rotational and vibrational excitation - H3+ + e
 How is o/p-H3+ produced in H2 plasma
o/p-H2+ + o/p-H2→ o/p-H3+ + H

H3+
32.9
3 atomic molecule H3+

n2x

n2y

n1
State specific recombination H3+(v=0)

n2x

3500
n2y

2500

n1
Rotational levels for n2
Absorption spectroscopy H3+(v=0)

overtone band n2=3  0 at 1.4 µm

Rotational and vibrational excitation - H3+ + e
Rotational and vibrational excitation - H3+ + e
Vibrational excitation - H3+ + e
Rotational excitation - H3+ + e

Rotational excitation - H3+ + e Vibrational excitation - H3+ + e

Rotational excitation - calculations
Electron collisional selection rules are found to be consistent
with the CB theory. In particular, dominant transitions are
those for which DJ ≤ 2 and DK = 0.
Rotational excitation - calculations

H3+
Rate coefficients

H3O+
H3+
 Dissociative recombination of NO+
NO+ important ion in ionosphere of Earth
and thermosphere of Venus
Mainly destroyed by
NO+ + e− N +O
Need T-dependent rates for models
Recent storage ring experiments show
unexplained peak at 5 eV
Calculations:
• resonance curves from R-matrix calculation
• nuclear motion with multichannel quantum defect theory
NO+ dissociation recombination: potential energy curves

Spectroscopically determined

R-matrix ab initio

R-matrix calibrated
NO+ dissociation recombination:
Direct and indirect contributions
 NO+ dissociation recombination:
comparison with storage ring experiments

IF Schneider, I Rabadan, L Carata, LH Andersen, A Suzor-Weiner & J Tennyson,

J. Phys. B, 33, 4849 (2000)
 NO+ dissociation recombination:
Temperature dependent rates
Rate coefficient (cm3 s−1)

Experiment
Mostefaoui et al (1999))

Calculation

Electron temperature, Te (K)

 Conclusion
• R-matrix method provides a general method for
treating low-energy electron collisions with
neutrals, ions and radicals
• Results should be reliable for the energies above
100 meV (previous studies of Baluja et al 2001 on
OClO).
• Total elastic and electron impact excitation cross
sections.
• Being extended to intermediate energy and
ionisation.
 Chiara
Natalia Vinci Piccarreta
Jimena Gorfinkiel

Iryna Rozum