fundamental mechanisms, predictive modeling, and novel … · 2019. 12. 12. · the ohio state...
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Nonequilibrium Thermodynamics Laboratories The Ohio State University
Fundamental Mechanisms, Predictive Modeling,
and Novel Aerospace Applications
of Plasma Assisted Combustion
Overview of research results at OSU
Walter Lempert, Igor Adamovich, J. William Rich, and Jeffrey Sutton
Michael A. Chaszeyka Nonequilibrium Thermodynamics Laboratory
The Ohio State University
MURI 2nd Annual Review Meeting
November 9-10, 2011
Columbus, OH
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Task 1: Low-to-Moderate (T=300-800 K) temperature, spatial and time-
dependent radical species concentration and temperature
measurements in nanosecond pulse plasmas in a variety of fuel-air
mixtures pressures (P=0.1 - 5 atm), and equivalence ratios (υ~0.1-3.0)
Goal: Generate an extensive set of experimental data on radical species
concentrations and temperature rise; elucidate kinetic mechanisms of
low-temperature plasma chemical fuel oxidation and ignition using
kinetic modeling. Bridge the gap between room-temperature data
(low-pressure gas discharges) and high-temperature data (shock tubes)
Thrust 1. Experimental studies of nonequilibrium air-fuel
plasma kinetics using advanced non-intrusive diagnostics
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Test bed: High-temperature nsec pulse discharge
cell for ignition delay and species measurement
Discharge cell placed in a tube furnace (6 inch bore, up to T=12000 C)
Optical access (LIF, TALIF, CARS) on the sides, for species and temperature measurements
Fuels to test in near future: H2, CH4, C2H4, C3H8, methanol & ethanol vapor
Flow Direction
• H2-air at T0= 100-300 C, P=50-150 torr,
ϕ=0.5-1.2
• Flow velocity u=12 cm/sec; residence time
in the discharge ~0.5 sec
• Pulse repetition rate (20 kV peak) ν=10-
40 kHz
60 mm straight angle prism
provides optical access to entire discharge
Nonequilibrium Thermodynamics Laboratories The Ohio State University
10 Hz, 100 msec
Time between pulses: 25 μsec
Laser delay time after last pulse
time
Burst of Pulses
Laser pulse
• Pulser produces a rapid “Burst” of 1-1000 pulses,
typically with 25 – 100 μsec spacing (10 – 40 kHz).
• For laser diagnostics burst is repeated at 10 Hz to
match laser repetition rate.
• Fresh sample of gas with every burst.
High Voltage Nanosecond Pulsed Plasma Generation
80 100 120 140 160 180
-20
-10
0
10
20
Time, nsec
Voltage, kV
H2-air, P=40 torr
experiment
Gaussian fit
40 kHz Burst – 10 Hz Laser Timing
Nonequilibrium Thermodynamics Laboratories The Ohio State University
H2-air at T0= 200 C, P=104 torr,
ν=40 kHz, ϕ=1
Ignition moment defined as beginning of
ignition “footprint”; verified by ICCD images
Spontaneous OH Emission-Based (310 nm)
Ignition Measurements.
Air , T0=25C, P=60 torr, ν=40 kHz
-40 -20 0 20 40 60 80
-20
-15
-10
-5
0
5
10
15
Time, nsec
Voltage, kV
Experiment
Gaussian fit
Peak voltage: ~18 kV, FWHM: ~15 nsec
0 10 20 30 40 50 60 70
Time, sec
-20
-10
0
10
20
Voltage, kVGate 1
(plasma)
Gate 2
(flame)
Nonequilibrium Thermodynamics Laboratories The Ohio State University
YR 1: Ignition delay time reduction
due to plasma-generated radical chemistry
Camera gate for
“last pulse” temperature
Ignition
delay
Use minimum number of pulses in a burst needed for ignition
Measure “last pulse” temperature (by N2 1st Positive emission), T=700 ± 100 K.
Measure ignition delay after the burst, τplasma
Compare with thermal ignition delay at the same T and P, τthermal
τplasma= 0.5-2.0 msec << τthermal (no ignition at T=700 K, τthermal= 1 msec at T ~ 850 K)
Consistent with measurements in FIW plasmas in shock-preheated mixtures (MIPT)
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Yr 2 Results: Plasma Uniformity and Ignition: H2/Air
(After Last Pulse in Burst)
ICCD Images after burst (Gate: 30μsec)
ICCD Single Pulse Images during burst (Gate: 2μsec)
Pulse #125Pulse #50Pulse #5
Region of Interest
Delay 1.05ms Delay 1.55ms Delay 2.55ms
Delay 0.05ms Delay 0.35ms Delay 0.55~0.95ms
Region of Interest
Emission in center lags by ~0.7ms compared to edge.Delay 4.00ms
Tinit = 500K , P = 80 Torr, 125pulses @ 20 kHz, FID Pulser (~10 nsec) , υ=0.5
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Time Expansion of Images During Ignition0.55 to 0.95 msec AFTER Last Pulse in 125 Pulse Burst
Delay 0.55ms Delay 0.60ms Delay 0.63ms
Delay 0.66ms Delay 0.69ms Delay 0.72ms
Delay 0.75ms Delay 0.78ms Delay 0.95ms
Region of Interest
Ignition is Quite Uniform Spatially
Note: Each Image is an Average of 5 Shots.
Ignition is Extremely Reproducible in Time
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Yr 1: Temperature Measurement by N2 2nd
Positive Emission vs Pulses in Burst
N2(C3Π→B3Π, v′=0→v″=0)
H2-air
Air
Time-Resolved Temperature in H2-air Plasma
Peak Temperature
and OH* emission
are nearly
coincident
Experimental T
is somewhat
lower than
prediction.
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Yr 2: Ignition Delay Measurements: H2/Air(After Last Pulse in Burst)
Hydrogen-air
T= 200C ϕ=1 =40 kHz,
150 Pulses
120 Pulses
115 Pulses
114 Pulses
Using a different pulser (FID) and a new dielectric
(perfluoreastomer) results in higher coupled energy,
fewer number of pulses in burst to achieve ignition.
Measured ignition delay: Extremely good
reproducibility.
Ignition delay vs. burst duration consistent with kinetic
model predictions; quantitative comparison need
accurate “last pulse” temperature measurements and
time-resolved [OH] measurements.
Ignition Threshold
Only one extra pulse makes
a difference between
ignition / no ignition
Last pulse
temperature
difference
predicted by
model ≈2°C
H2-air, ϕ=1
Ignition Delay AFTER Laser Pulse in Burst
Time, sec
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Yr 2: H2 /Air OH (LIF) Number Density Measurements in
Nanosecond Pulsed Discharge vs # Pulses in Burst (CPT Pulser – 25 nsec Pulse Duration)
υ = 1, P = 94 Torr, T = 200 oC.
OH: 40 kHz Burst.
υ = 1, P = 74 Torr, T = 100 oC.
Single Discharge Pulse.
- = Full Reaction Set(Popov – 22 Processes)
… = Reduced Reaction Set
H + O2 + M ↔ HO2 + M (1)
O + HO2 ↔ OH + O2 (2)
OH + H2 ↔ H + H2O (3)
H + HO2 ↔ H2O + O (4)
H + HO2 ↔ OH + OH (5)
H + HO2 ↔ H2 + O2 (6)
O + H2 ↔ H + OH (7)
H + O2 ↔ O + OH (8)
OH + HO2 ↔ H2O + O2 (9)
Modeling Input for Specific
Energy Coupling is the
same for all four cases.
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Yr 2: OH LIF Temperature Diagnostic
Development – A Few Details
EXCITATION at ~283 nm: (1, 0)
COLLECTION at ~310 nm: Full (1,1) & (0,0)
OH X
OHAv’=1
v’=0
v’”=1
v’”=0
b01
A10
b10
Q10
V10
A00
b00
Q00
V01Nu1
Nu2
Nl1
Nl2
Excitation Spectra and Voigt Fits.
Q1(5)
Ф – fluorescence quantum yield
calculation (assumes steady-state
approximation)*
J
A A V A Q
V A Q10 00 10 00 00
10 10 10
Afi: spontaneous emission rate, s-1
Qfi : quenching rate coefficient, s-1
Vfi: V-V Transfer Rate (Assumed 0.58 Q)
Qfi for H2 , H2O, N2, and O2 in the flame
taken from literature – Assumed J-
independent.
A+Q in the plasma: measured directly
(includes small J dependence)!
(*Cathay, et al, Comb &Flame, 2008)
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Hencken Flat-Flame Burner for Temperature Validation
and Absolute OH Number Density Calibration
C2H4
N2
Nitrogen flow
Measurement
Location – 10mm
Above Surface
(Lucht et al. 1997)
PAC B,
Flame B,
PAC
Flame
Flame F,
PAC F,
Flame ΟΗ,PAC ΟΗ,f
f
S
Snn
Q1(5)
Q2(11)
Two Line Temperature (Burner)
(Best-fit Temperature: 2260 K +/- ~125 K)Hencken Burner (1 Bar) Calibration
Burner TOH vs υ
Nonequilibrium Thermodynamics Laboratories The Ohio State University
T0=500 K, P=80 torr, ϕ=0.5
Experiment: 125 pulses (burst duration 6.25 msec)
Model prediction at P=const: 139 pulses (burst duration 6.95 msec)
Model prediction at V=const: 118 pulses (burst duration 5.90 msec)
Estimated pressure overshoot decay time: ~10 msec
Problem: model considerably over predicts peak OH number density
(Measure OH is close to equilibrium whereas model predicts significant super-equilibrium).
Yr 2: H2 /Air OH (LIF) Number Density & T
Measurements vs Time after 125 Pulse Burst @ 20 kHz (FID Pulser – 10 nsec Pulse Duration)
Nonequilibrium Thermodynamics Laboratories The Ohio State University
T0=500 K, P=80 torr, ϕ=0.5
Quenching Model Dependence of OH LIF Temperature
0
500
1000
1500
2000
0 2 4 6 8 10 12
Tem
per
atu
re, K
Time after the last pulse, msec
J-independent
J-dependent
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Yr 2: OH LIF and Emission Temporal Profiles
H2 – Air (FID Pulser)
20 kHz, 125 pulses, phi=0.5 10 kHz, 125 pulses, phi=0.5
20 kHz, 125 pulses, phi=0.4
Key chemiluminescent processes at
low temperature.
H + O + M ↔ OH* + M
OH* + M ↔ OH + M
M = N2, O2, H2, H2O, OH, O, H
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Kinetic modeling of OH* formation
H + O + M ↔ OH* + M
OH* + M ↔ OH + M
M = N2, O2, H2, H2O, OH, O, H
Peak OH predicted to precede peak temperature, peak OH
Nonequilibrium Thermodynamics Laboratories The Ohio State University
YR 2: Effect of O2 (1D) (SDO) on Ignition Delay
in C2H4 – O2 Mixtures (RF side discharge)
*NOTE: O2(1D) yield measurements were taken directly after their formation and also
downstream. The locations of these measurements are marked by:
Test
Cell
Pump
Gas
Out
PMT
NO
2
cyli
nder
H2
fuel
cyli
nder
Syn
thet
ic
air
mix
ture
Pulser
O2(1D) Cell
RF Discharge
Gas In
Synthetic Air Mixtures
20% O2 in Helium
50% O2 in Helium
20% O2 in Argon
-NO2 is used to titrate out possible effects due to O3 and atomic oxygen.
This is done downstream of O2(1D) formation.
NO2 + O → NO + O2
NO + O3 → NO2 + O2
Nonequilibrium Thermodynamics Laboratories The Ohio State University
The Ohio State University Nonequilibrium Thermodynamics Laboratory
O2(a1Δ) IR Emission Spectra
Without NO2 titration With NO2 titration
20% O2/Ar, P=60 Torr
*At these conditions, temperature inferred from O2 b→X spectra is 400K.
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Example Results – OH Emission Traces
(a) Baseline: No O2(a1Δg) (RF
discharge turned off), no NO2
added.
Δt = 17 msec
(b) O2(a1Δg) (RF discharge turned
on) and NO2 added.
Δt = 8 msec
(c) O2(a1Δg) but no NO2
Δt = 15 msec
(d) NO2 but no O2(a1Δg).
Δt = 11 msec
(a)
(c)
(b)
(d)
υ = 0.75 (C2H4), 50% O2-Ar (“Oxidizer),
P=65 Torr, υ = 50 kHz.
Nonequilibrium Thermodynamics Laboratories The Ohio State University
The Whole Story is More Complicated
20% O2 in Argon with stoichiometric (f=1.0) C2H4 fuel.
Suggests:
i. NOx Chemistry is
complicated.
ii. Three body processes
increasingly important as
pressure increases.
iii. Above 65 Torr discharge
becomes somewhat
filamentary.
iv. Energy loading per
molecule likely drops with
increasing pressure.
O TALIF measurements
on-going.
Nonequilibrium Thermodynamics Laboratories The Ohio State University
O TALIF with Xenon Optical Calibration*(Doebele Group – U. Duisburg-Essen)
2221o o
o ND Xe2Xe Xe21 o
a Xe XeS 1N g N
S a O F TO
5p6 1S06p’[3/2]2By obtaining ratio of spectrally integrated
O atom TALIF signal to that from
xenon with identical:
i. beam focusing and spatial mode
structure.
ii. collection optics and geometry
iii. spectral filtering
iv. photomultiplier gain
Then relative signal can easily be converted
to absolute O atom number density.
109837
88631
76795
227
1590
1
2
0
Oxygen
3P
= 225.7 nm
Laser
3S° 1
= 844.6 nm
3P 2, 1, 0
O+(4S° )3/2
G-4582
2p 3P 3p 3P
3p 3P 3s 3S
Bamford, et al., 1986
dt)t(IN)T(FGg)h(
agVS)(
)(
ND
0
2
00
2
2
2
21
*(Niemi, et al, 2005,
Grinstead, et al., 2000)
Nonequilibrium Thermodynamics Laboratories The Ohio State University
O atom TALIF Measurements
Nd:YagSHG
THG
1064
Dump
Dye
Laser
BBO
Boxcar
SRS272
PMT
UV
Separator
DELAY LINE
Gas Out
Gas In
Pulser
Quartz Test
Cell
Filters
619nm Mirrors
355nm Mirrors
225nm Mirrors
840nm
Collection lens
355nm Mirror
619nm Transmit
UV focusing lens
Photodiode
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Preliminary Results: Ar/O2 with/without added NO2.
P=40 Torr
~0.07% NO2 by Volume
20% O2
80% Ar
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Preliminary Ar/O2/C2H4 Results
P=40 Torr
Ar/O2 : 4:1
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Oscilloscope
Dye Laser +
Mixer
Pulse
Generator
Q-switched
Nd:Yag Laser
(Second
Harmonic)
Spectral
Filter + Slit
Photodiode
Delay
Generator
PMT
Flow Controller
Burn
er
O Atom TALIF Measurements in Atmospheric Pressure
Pin – to – Plane nsec Pulsed Discharge*
(*w. S. Pendleton, M. Gunderson: USC
Cam Carter: AFRL – Propulsion
Directorate)
Filament dimensions:
~0.25 mm x 0.8 cm.
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Some Results: Fuel/Air – Time After Single Pulse
(No Ignition)
28kV pulse amplitude used for all data, each data point is 3000 shots averaged
1 10 100 1000
1E16
1E17
1E18
Ethylene/Air Mixtures Ethylene phi=0
Ethylene phi=0.25
Ethylene phi=0.5
Ethylene phi=2.4
O a
tom
nu
mb
er
de
nsity (
cm
-3)
Time (s)
10 100 1000
1E16
1E17
1E18 Methane phi=0
Methane phi=0.3
Methane phi=0.6
Methane phi=1.2
O a
tom
num
ber
density (
cm
-3)
Time (s)
Methane/Air Mixtures
The addition of fuel radically alters the discharge afterglow chemistry, even outside the
limits of combustion. Propane/Air was also measured, yielding O atom behavior similar to
methane/air.
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Task 8: Development and validation of a predictive kinetic model of non-
equilibrium plasma fuel oxidation and ignition, using
experimental results of Thrust 1
Goal: Identify key mechanisms, reaction, and rates of plasma chemical
fuel oxidation processes for a wide range of fuels, pressures,
temperatures, and equivalence ratios. This is absolutely essential
to predictive capability of the model.
Thrust 2. Kinetic model development and validation
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Low-temperature hydrogen-air
plasma chemistry kinetic model
• Air plasma model: equations for ground state species (N, N2, O, O2, O3, NO,NO2, N2O), charged species (electrons and ions), and excited species(N2(A
3Σ), N2(B3Π), N2(C
3Π), N2(a'1Σ), O2(a1Δ), O2(b
1Σ), O2(c1Σ), N(2D),
N(2P), O(1D)) produced in the plasma.
• Two-term expansion Boltzmann equation for plasma electrons
• Fuel-air plasma: model combined with H2-air chemistry model by Popov (22reactions), supplemented with H2 dissociation by electron impact and inreactions with electronically excited nitrogen
• Peak E/N chosen to match coupled pulse energy to value predicted by OSUnanosecond pulse discharge model (Phys. Plasmas, 2009)
• CxHy-air model previously validated by comparing with experiments inethylene-air plasmas (time-resolved O atom number density, temperature)
• H2-air validation: model predictions compared to the experimental data ofThrust 1 (ignition delay time, time-resolved OH number density, andtemperature in H2-air plasmas)
• Reduced plasma chemistry kinetic mechanism is identified; effect of radicalson ignition delay time is demonstrated
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Reduced mechanism: dominant radical generation
processes and chemical reactions in H2-air plasma
Key radical generation processes
N2 + e- → N2(A3Σ, B3Π, C3Π, a'1Σ) + e-
N2(C3Π, B3Π, a'1Σ) + M → N2(A
3Σ) + M
N2(A3Σ) + O2 → N2 + O + O
N2(A3Σ) + H2 → N2 + H + H
O2 + e- → O(3P) + O(3P,1D) + e-
H2 + e- → H + H + e-
O(1D) + H2 → H + OH
H2-O2 reduced reaction mechanism
H + O2 + M = HO2 + M
O + HO2 = OH + O2
OH + H2 = H + H2O
O + H2 = H + OH
H + HO2 = H2O + O
H + HO2 = OH + OH
H + HO2 = H2 + O2
H + O2 = O + OH
OH + HO2 = H2O + O2
Model predicts significant significant additional energy release from fuel
species reacting with radicals produced by the plasma (O, H, and OH)
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Model predictions for full and reduced reaction sets
(H2-air f=1, P=40 Torr – CFT Pulser – NO Oven)
0 5 10 15 20 25 30
300
600
900
1200
0 200 400 600 800 1000 1200
Time, msec
Number of pulses
T, K
H2-air, P=40 torr
f=1
model, full set
model, reduced set
Temperature predicted by
full and reduced kinetic models
Full mechanism
0 5 10 15 20 25 30
1.0E-6
1.0E-5
1.0E-4
1.0E-3
1.0E-2
1.0E-1
1.0E+0
Time, sec
Species mole fractions
H2
O
H2O
OH
H
HO2
0 5 10 15 20 25 30
1.0E-6
1.0E-5
1.0E-4
1.0E-3
1.0E-2
1.0E-1
1.0E+0
Time, sec
Species mole fractions
H2
O
H2O
OH
H
HO2
Reduced mechanism
Data Unobtainable Between 500
and 600 Pulses (Beam Steering?)
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Effect of O and H generation by the pulsed
discharge on ignition delay
• Reduced reaction sets with and
without plasma chemical O and H
atom generation processes
• Ignition is NOT predicted in absence
of generation of O and H atoms by
nanosecond discharge, for the same
discharge input power
0 5 10 15 20 25 30 35
300
600
900
1200
0 200 400 600 800 1000 1200
Time, msec
Number of pulses
T, K
f=1
full set
no O and H generationby plasma
(H2-air υ = 1, P = 40 Torr)
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Thrust 3. Experimental and modeling studies
of fundamental nonequilibrium discharge processes
Task 10: Characterization and modeling of nsec pulse discharges
Goal: Prediction of E/N and electron density in the plasma, individual
pulse energy coupled to the plasma, and their scaling with
pressure, temperature, pulse waveform, and mixture
composition
Nonequilibrium Thermodynamics Laboratories The Ohio State University
CARS Measurements of Vibrational Energy Loading
and Relaxation in Pulser-Sustainer Discharge of Mach 5
Wind Tunnel.
Simplified Schematic Illustrating Discharge, CARS Measurement
Location, and Relaxing Gas Injection Point.
Pulser Electrodes: 4 x 4 x 0.5 (gap) cm (dielectric barrier).
Sustainer Electrodes: 4 x 1 x 4 (gap) cm (copper).
Pulser Repetition Rate: 100 kHz (~5 nsec duration, 20 kV).
DC Sustainer: ~1-4.5 kV (~1 Amps maximum)
Flow velocity in plenum ~40 m/sec (~.4 msec residence time in discharge).
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Nitrogen, P=650 torr, ν=100 kHz, no DC electrodes
Nitrogen, P=350 torr,
ν=100 kHz, no DC electrodes
0.3 seconds after start (pulse # 30,000)
Pulse energy 5.2 mJ/pulse
Average discharge power 520 W (100 kHz)
Nitrogen, P=300 torr, ν=100 kHz, no DC electrodes
Flow into the page
Pulsed electrodes
Sustainer DC electrodes
(removable)
Alumina ceramic plates
Repetitive nsec pulse discharge
sustained in a high-pressure N2 flow
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Schematic of Psec CARS diagnostic*:
for N2 Rotational and Vibrational Temperature
Ekspla Nd:YAG laser
- 10 Hz, ~150 psec pulses
- 125 mJ per pulse max @ 532 nm
Modeless Psec Dye Laser
- Broadband ~602-608 nm FWHM
-~ 7% conversion efficiency
Spectral Resolution ~0.5 cm-1
Nd:YAGDelay Path
Wind Tunnel
Flow
¾ m
Spectrometer Camera
R 473nm / T 532-
607nm Dichroic
Mirrors
Broadband
Dye Laser
250mm
Lenses
476nm Band pass Filter
100mm Lens
Beam Dump
532 nm “Pump / Probe”
607 nm “Stokes”
R 532nm
/ T
607nm
Dichroic
Mirror
Relay Lens
Magnification
System
Unstable Resonator Spatially
Enhanced Detection (USED) CARS
Spatial Resolution ~1-2 mm.
(* Patterned after S. Roy, et al.)
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Portable, broadband psec CARS diagnostic system
Spectrometer
Dye Laser
YAG Power
Supply
Dye Laser in operation
(view from opposite
angle)
Computer
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Single Shot Precision ~ 20 K (2σ) at T = 300 K,
P = 370 Torr
Trot = 316.7 K 300 K single shot spectrum,
P = 300 Torr N2.
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Psec CARS spectra: N2(X,v) populationsNsec pulse discharge vs. pulser / DC sustainer discharge
Nitrogen, P=300 Torr
TV ~760 K, Trot =~380 K
Discharge Average Power = 520 W
Significant vibrational disequilibrium in a nsec pulse discharge without DC sustainer
as measured in “afterglow” ~2 msec downstream from discharge section.
20 shot average
20 shot average
(Averaging helps with dye laser spectral fluctuations).
Nonequilibrium Thermodynamics Laboratories The Ohio State University
How Can the Pulsed Discharge Alone Excite
N2 Vibration?
20 kV/ 0.5 cm / 300 Torr
~ 300 Td
Tvib = 760 K Corresponds to v=1 fraction ~0.012,
corresponding to 3.5 meV/molecule.
ΔTRot/Trans = 80 K corresponding to 23.9 meV/molecule
If all energy goes to rot, trans, or vib then ~13% of total
discharge power loads vibration!
Measured energy loading is 28.4 meV/molecule as compared
to 27.4 meV into rot/trans/vib from CARS spectra.
(1 Td = 10-17 V-cm2)
4: N2 vibration
5: N2 electronic states
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Air, P=100 torr, Upeak=25 kV, 1 cm gap
Top: 50 FWHM pulse, Bottom: 5 FWHM pulse
(~15-25% of Energy Coupled at LOW (<50 Td) – Pulse Duration Dependent
Prediction of Energy Coupling by Nsec Pulsed
Discharge Model
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Some Pulser – Sustainer Spectra
Sustainer VPS = 4.5 kV (E/n ~ 10 Td), 300 Torr pure N2
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Some Preliminary Results from S. Pendleton
Filamentary Discharge: N2 CARS
N2 (v=1) is present in discharge afterglow from ~10-200 us with Tv > 1500 K.
Rotational temperature analysis still underway on these measurements.
E/n ~ 200 Td at tip (~2x increase due to field concentration near tip)
473.0 473.5 474.0 474.5 475.0 475.5 476.0
105
106
Inte
nsity (
a.u
.)
Wavelength (nm)
v=0
v=1
N2 CARS Signal Intensity
Note: Streamer diameter ~0.25
mm whereas USED CARS
obtained from ~1-2 mm x 50
micron cylindrical volume
element.
Hence most of v=0 signal
originates outside of filament!
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Sub-Nsec Electric Field Measurement by
CARS-like Four Wave Mixing
“E-Field CARS” is a 4 wave mixing process.
The typical CARS probe beam is replaced by an external electric field, which is at essentially zero frequency. This creates an IR “CARS” signal at the vibrational-rotational transition Q(1) (v=0, J=1 → v=1, J=1) frequency.
The physical origin of this signal is the dipole induced by the external field.
Energy Level Diagram
for E-Field CARS
ωS
ωp
IR CARS
ωAS
ωp
For “Psec” E-Field CARS the temporal resolution can be limited by
the decay time of the coherence (<~200 psec @ 100 Torr for H2).
(Roy, Appl. Phys. Lett 97, 2010)
E
IR IR Pump Stokes External
CARS CARS Pump Stokes Pump
ExternalIR IR
CARS CARS Pump
IR PumpCARS
External
IR CARS
E E E E
E E E E
EE*
E E
I IE
I
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Generation of H2 Stokes Beam Using High
Pressure Stimulated Raman Shifting Cell.
Raman shifted Stokes beam required for CARS.
Stokes beam created in a high pressure Raman
cell.
532nm Pump beam used in Stimulated Raman
Scattering thus creating a Stokes beam with
λ=683nm.
Data taken for different input energies with
different pressures.0
1
2
3
4
5
6
7
8
9
10
0 5 10 15 20 25 30
Ou
tpu
t E
ner
gy
(m
J)
Input Pump Energy (mJ)
8 bar H2 in Raman Cell
A.S.
Probe
Stokes
0
1
2
3
4
5
6
7
0 5 10 15 20 25
Ou
tpu
t E
ner
gy
(m
J)
Input Pump Energy (mJ)
11 Bar H2 in Raman Cell
Anti-Stokes
Stokes
Pump
0
1
2
3
4
5
6
7
8
9
0 5 10 15 20 25 30
Ou
tpu
t E
ner
gy
(m
J)
Input Energy (mJ)
5 bar H2 in Raman Cell
A.S.
Probe
Stokes
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Some Recent Results - 760 Torr H2 Scope Traces(DC sub-Breakdown Field)
Signal vs Field Strength (100 Torr)
Electric Field (V/cm)
0 500 1000 1500 2000 2500 3000 3500 4000
Sq
rt (
IR*P
um
p/C
AR
S)
0.1
0.2
0.3
0.4
0.5
0.6
0.7
(*Roy, Appl. Phys. Lett 97, 2010)
τCoh vs P*
-6 -4 -2 0 2 4 6
x 10-7
0.006
0.008
0.01
0.012
0.014
0.016
0.018
0.02
-6 -4 -2 0 2 4 6
x 10-7
6
6.5
7
7.5
8
8.5
9x 10
-3
-1 -0.5 0 0.5 1 1.5 2
x 10-7
0
0.005
0.01
0.015
0.02
0.025
0.03
0.035
0.04
0.045
0.05
-1 -0.5 0 0.5 1 1.5 2
x 10-7
0
0.05
0.1
0.15
0.2
0.25
-1 -0.5 0 0.5 1 1.5 2
x 10-7
0
0.1
0.2
0.3
0.4
0.5
0.6
0.7
0.8
0.9
1
-1 -0.5 0 0.5 1 1.5 2
x 10-7
0
0.2
0.4
0.6
0.8
1
1.2
1.4
-1 -0.5 0 0.5 1 1.5 2
x 10-7
0
0.2
0.4
0.6
0.8
1
1.2
1.4
-6 -4 -2 0 2 4 6
x 10-7
0.006
0.008
0.01
0.012
0.014
0.016
0.018
0.02
360 V/cm
4 Averages
-1 -0.5 0 0.5 1 1.5 2
x 10-7
0
0.05
0.1
0.15
0.2
0.25
1780 V/cm
4 Averages3570 V/cm
4 Averages
~ 10 mJ @532 – 8 Bar Raman Cell
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Raw IR nsec N2 E-Field Data*
(Electric field measured between two plane electrodes
in atmospheric air - 625 Torr in Albuquerque, NM)
75 mJ Pump / 35 mJ Stokes
(* w. S. Kearney and E. Barnat, SNL – Albuquerque)
Nonequilibrium Thermodynamics Laboratories The Ohio State University
IR/CARS Signal Ratio vs External Field
(Nsec N2)
SQRT (IR/CARS) vs External DC Field
External Field (kV/cm)
0 2 4 6 8 10
Sq
rt (
IR/C
AR
S)
(au
)
0.0
0.1
0.2
0.3
0.4
0.5
2
CARS CARS Pump Stokes Pump
IR IR Pump Stokes External
ExternalIR IR
CARS CARS Pump
ExternalIR IR
CARS CARS Pump
E E E E
E E E E
EE*
E E
EI*
I E
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Thrust 4. Studies of diffusion and transport of active
species in representative 2-D reacting flow geometries
Task 12: Ignition and flameholding in nonequilibrium plasma cavity flows
at low static temperatures
Goal: Determine viable approaches to flameholding in high-speed flows
using low-temperature plasmas. We simply cannot process the
entire flow with the plasma.
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Cavity injection flow ignition and flameholding:
experimental setup
• Static pressure P=150-200 torr (0.2-0.26 atm), flow velocity u=30-200 m/sec
• Plasma produced in the cavity by repetitively pulsed nsec discharge, U=25 kV, ν=40 kHz
• Fuel (ethylene or hydrogen) injected (a) into flow upstream of the cavity; (b) into the
cavity downstream of high voltage electrode
• Ignition detection: OH emission; plasma and flame development: ICCD emission
imaging and high frame rate NO PLIF imaging; temperature: N2 emission spectroscopy;
burned fuel fraction: FTIR absorption spectra (in premixed flows)
Cavity L/D=3
Air
Flow
Fuel injection
Air Flow
Nonequilibrium Thermodynamics Laboratories The Ohio State University
ICCD images of plasma and flame
in H2- air flows (injection into the cavity)
P=150 torr, u=60 m/sec, ν=40 kHz, υglobal =
Pulse# 180
#240 to #241
Pulse# 140
Pulse# 200
Pulse# 240
#200 to #201
#160 to #161
#140 to #141
Optical access windows
To
vacuum
system
High voltage
electrode block
Ceramic platesPressure tap
Fuel injection ports
Main flow
Nonequilibrium Thermodynamics Laboratories The Ohio State University
280 Hz frame rate schlieren images of injection flow5% precooled He injected into cavity, main flow is air
Transient injection (several msec after injection valve opens)
Injection jet penetration into cavity ~ 1 cm
Near steady state injection 220 ms after injection valve opens, global ϕ=0.05
He injection
Camera field of view
Main Flow Direction
u=150 m/sec
P=150 torr
Nonequilibrium Thermodynamics Laboratories The Ohio State University
10 kHz frame rate NO PLIF images of injection flow5% NO-He mixture injected into cavity, main flow is air
Transient injection (several msec after injection valve opens)
Injection flow directed upstream, toward HV electrode
Steady state, global ϕ=0.042 ([NO]~3∙1015 cm3)
Injection flow mixed with air flow in the entire cavity
NO-He injection
Camera field of view
Main Flow Direction
u=150 m/sec
P=200 torr
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Air and H2-air plasma temperatures
Ignition and flameholding vs. flow velocity (P=150 torr)
• Air plasma temperature does not exceed T=1500 C
• H2-air plasma/flame temperature after ignition T=600-8500 C
• Ignition and stable flame detected in the entire velocity range tested,
up to u=140 m/sec, global equivalence ratio range ϕ=0.03-0.13
• At u≥90 m/sec, flameholding achieved at global ϕ=0.05-0.1
Open symbols: ignition
Closed symbols: flameholding
0
100
200
300
400
500
600
700
800
900
40 60 80 100 120 140 160
Velocity (m/s)
Air
Hydrogen-Air
Temperature (°C)
60
70
80
90
100
110
120
130
140
150
160
0 0.03 0.06 0.09 0.12 0.15
Global equivalence ratio
Velocity (m/sec)
No ignition Ignition
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Air and H2-air plasma temperatures
Ignition and flameholding vs. flow velocity (P=200 torr)
• Air plasma temperature does not exceed T=1500 C
• H2-air plasma/flame temperature after ignition T=600-9000 C
• Ignition and stable flame detected in the entire velocity range tested,
up to u=190 m/sec, global equivalence ratio range ϕ=0.01-0.09
• At u≥80 m/sec, flameholding achieved at global ϕ=0.02-0.04
Open symbols: ignition
Closed symbols: flameholding
60
80
100
120
140
160
180
200
220
0 0.02 0.04 0.06 0.08 0.1
Global equivalance ratio
Velocity (m/sec)
No ignition Ignition
0
100
200
300
400
500
600
700
800
900
60 80 100 120 140 160 180 200
Velocity (m/sec)
Air
Hydrogen-Air
Temperature (°C)
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Ongoing work: scaling down cavity size,
using flush mounted electrodes
• Reducing cavity length and depth while keeping L/D same, L/D=3
• Using non-metal test section (nylon plastic lined with alumina ceramic plates)
• Extending nsec pulse discharge cavity ignition to Mach 2 flows
Optical access windows
To
vacuum
system
High voltage
electrode block
Ceramic platesPressure tap
Fuel injection ports
Main flow
Nonequilibrium Thermodynamics Laboratories The Ohio State University
Questions??