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Combustion Imaging JOAKIM BOOD | DIV. OF COMBUSTION PHYSICS, LUND UNIVERSITY CH CH 2 O OH

Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

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Page 1: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

Combustion Imaging JOAKIM BOOD | DIV. OF COMBUSTION PHYSICS, LUND UNIVERSITY

CH CH2O OH

Page 2: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

Combustion processes are very complex The chemistry is extremely complicated…

The most important reaction paths in acetylene oxidation is shown below

Turbulence Chemical reactions

Flow-field equations (Navier-Stokes)

Transport equations for species

Inter- action

then there is also interaction between the chemistry and the turbulent flow

Page 3: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

Outline • Multi-spectral imaging concepts based on spontaneous

flame emission

• Introduction to laser-based combustion diagnostics

• Multi-species imaging with planar laser-induced fluorescence (PLIF)

• Two-dimensional thermometry using PLIF

• High-speed imaging

Page 4: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

Multi-spectral imaging concepts based on spontaneous flame emission

Page 5: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

Spontaneous flame emission (chemiluminescence) Images of Bunsen-type flames having different fuel/air-mixtures

Flame emission spectrum recorded with spectrograph

Spectrum recorded with Ocean Optics HR2000 spectrometer. It is not corrected for the wavelength-dependent variations in sensitivity (i.e. the intensity scale is not calibrated).

Page 6: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

Multi-color imaging of flame emission

Setup Result

This is a line-of-sight imaging technique. Three-dimensional information requires tomographic inversion from multi-projection recordings.

C2 470 nm

OH 308 nm

CH 432 nm

C2H2/O2 flame

Heig

ht a

bove

bur

ner (

1 m

m/d

iv)

Page 7: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

Thermometry in sooty flames

Total signal intensity depends on both soot volume fraction and temperature. We can measure the temperature in a flame if we can detect the emission intensity as a function of wavelength.

How can we measure the temperature in this flame?

Photo: Per-Erik Bengtsson

Page 8: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

0

5E+10

1E+11

1,5E+11

2E+11

2,5E+11

3E+11

3,5E+11

4E+11

4,5E+11

400 800 1200 1600 2000 2400 2800

Wavelength (nm)

Inte

nsity

(W/m

3 )

T=1600KT=2000K

Visible region

Per-Erik Bengtsson

Planck radiation The spectral shape of the emission is temperature dependent

112)( /5

2

−= kThce

hcI λλπλ

mK10898.2 3max ⋅⋅= −Tλ

4TI σ=

Planck´s law

Wien´s displacement law

Stefan-Boltzmanns law:

Photo: Per-Erik Bengtsson

Page 9: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

CCD- Camera 2

CCD-Camera 1

Temperature map

Optical filter λ=400 nm

Optical filter λ=470 nm

The ratio between the emission signals at two wavelengths is temperature dependent.

Still there is a line-of sight limitation!

Temperature imaging using 2-D pyrometry

Page 10: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

Introduction to laser-based combustion diagnostics

Page 11: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

• Nonintrusive

• High spatial resolution (<0.001 mm3)

• High temporal resolution (<10 ns)

• High spectral resolution (~MHz)

• Multiplex (multi-species, multi-point)

Why use lasers in combustion research?

Undisturbed pre- mixed flame

Premixed flame disturbed by a thermocouple

Photos by P.-E. Bengtsson

Photo by H. Bladh

Page 12: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

What can be measured with laser-based combustion diagnostics?

• Temperatures (rotational/vibrational)

• Species concentrations (atoms, molecules, radicals)

• Velocities

• Particle number densities/diameters

• Surface characteristics

Page 13: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

For example • Mie/Rayleigh scattering • Laser-induced fluorescence (LIF) • Laser-induced incandescence (LII) • Laser-induced phosphorescence (LIP) • Raman scattering

Laser Lens

Spectrograph & detector

For example • Coherent anti-Stokes Raman scattering (CARS) • Polarization spectroscopy (PS) • Degenerate four-wave mixing (DFWM) • Stimulated Emission (SE)

Laser techniques used in combustion research

Coherent techniques

Incoherent techniques

Page 14: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

Joakim Bood

Laser-induced fluorescence (LIF) is the most widely used laser diagnostic for combustion studies

Simultaneous OH-LIF and PIV measurements in a turbulent CH4/H2/N2/air flame

Rapid development of lasers and detectors over the last decades has made LIF a very powerful tool in both fundamental and

applied combustion research

125 µsec between images, Image size: 14 × 16 mm

Page 15: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

X

v’

v’’

re’’

De’’

Pote

ntia

l ene

rgy

Internuclear distance

A

v’

X

A

v’’ = 0

v’’ = 1

J’’ = 0 J’’ = 1 J’’ = 2

J’ = 0 J’ = 1 J’ = 2

⇒ fluorescence spectrum

Laser-induced fluorescence - basics

Page 16: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

v’

X

A

v’’ = 0

v’’ = 1

J’’ = 0 J’’ = 1 J’’ = 2

J’ = 0 J’ = 1 J’ = 2

Excitation spectrum Fluorescence spectrum

X

A

v’’ = 0

v’’ = 1

J’’ = 0 J’’ = 1 J’’ = 2

J’ = 0 J’ = 1 J’ = 2

v’

Laser tuned to a specific absorption line and the spectrometer is scanned

Laser is tuned across the various absorption lines and the total fluorescence is monitored

Fluorescence spectrum and excitation spectrum

Fluorescence spectrum

Excitation spectrum

Page 17: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

2-D measurements using planar laser-induced fluorescence (PLIF)

Sheet-forming optics

Side view

View from above

OH-PLIF image

Page 18: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

Multi-species imaging with planar laser-induced fluorescence (PLIF)

Page 19: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

Setup for multi-species imaging

Toluene CH2O OH CH

Exc. (nm) 266 355 309 431

Det. (nm) 275-290 385-500 309±5 431±10

Page 20: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

OH CH CH2O Toluene

20

Multi-species imaging in laminar flame

Page 21: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

Jet speed 120m/s Jet speed 60m/s

Sjöholm et al., Proc. Combust. Inst. 34, 1475-1482 (2013).

Multi-species imaging in turbulent flames

OH CH

CH2O CH

CH2O Toluene

OH CH

CH2O CH

CH2O Toluene

Page 22: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

• Tunable (740-790 nm)

• High pulse energy: ~400 mJ @ 776 nm, ~ 70 mJ @ 387 nm, ~10 mJ @ 259 nm

• Long pulse length: ~150 ns • Single mode (~100 MHz linewidth) • Multimode (~ 8 cm-1 linewidth) • Example: 5 mJ single mode at 226 nm!

Strong potential for CH (doubling) and HCO (tripling) PLIF imaging by long pulse and broadband excitation to avoid saturation

Improved sensitivity using Alexandrite laser

1

2

3

4

pumping Lasing

(700-820 nm)

Rapid non-rad. decay

Rapid relax

Alexandrite (BeAl2O4:Cr3+) energy level scheme

Page 23: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

CH visualization

Thanks to long and broad pulse ~ two orders of magn. increased sensitivity compared with conv. Nd:YAG/dye system (~25 mJ)

Co-axial jet flame

Motivation: Intermediate species in NOx formation Flame front marker Approach: Excitation B ← X at ~ 387 nm Emission B → X, A → X at ~430 nm Broadband excitation

Excitation scan over band head CH-PLIF

Li et al., Proc. Comb. Inst. 31, 727 (2007)

Page 24: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

Simultaneous PLIF imaging of CH and OH CH OH

Excitation (nm) ∼387 ∼283

Detection (nm) ∼430 ∼310

CH OH

Page 25: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

Simultaneous CH/CH2O PLIF

Li et al., Combustion and Flame 157, 1087-1096 (2010). 25

Page 26: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

Li et al. Comb. and Flame, 2010

Simultaneous PLIF imaging of CH and CH2O Burner Flames PLIF images (CH anf CH2O)

Page 27: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

Phi=1.0, Ujet = 100 m/s; Ka ~90

Simultaneous imaging of CH, CH2O, and OH in a turbulent flame

Page 28: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

2-D thermometry with PLIF

Page 29: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

LIF thermometry

• Any method that reflects the distribution of population over two or more individual vibrational rotational states can in principle be used for temperature measurement. LIF is such a method.

• LIF thermometry restricted to high temperatures if molecular

radicals are employed. For OH temperatures above 1500 K are needed.

• If atomic species, such as metal atoms, are used, these have to

be seeded into the flame or flow. • If LIF was used for concentration measurements it is definitely

convenient to apply it for thermometry too.

Page 30: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

Two-line LIF thermometry

0

1

2

λ02

λ12 F21

F20

Basic idea: To measure the relative population of two states ⇒ T from Boltzmann expression

Excitation to the same upper state ⇒ F21 and F20 are equally affected by quenching and energy transfer processes

( )C

II

FF

kEETlnln4lnln

20

21

02

12

20

21

01

+++

−=

λλ C non-dimensional system

Dependent calibration constant

Page 31: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

PCylindricaltelescope

CCD-camera

PBurner

Interference filter ND filter

Dye cell

Quartz plate

Quartz plate

Laser systems

Power meter

Two-Line Atomic Fluorescence (TLAF) thermometry

Page 32: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

Ultrafast imaging

Page 33: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

• Conventional video camera Exposure Read out information Store the information

There is an electronic limitation of how fast you can read out and store images

Filming dynamics Operation of a conventional video camera

Page 34: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

We need some kind of trick to separate the images

Speeding up the image recordings Multiple exposures

Page 35: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

• Coding strategy Each image has a unique code The code is a stripe pattern The final photo consists of

multiple coded images

Image coding Tagging each frame with a periodic modulation

Page 36: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

Identifying coded images The images are separated in the Fourier domain

Page 37: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

Now let us demonstrate this on ultrafast dynamics.

FRAME Frequency Recognition Algorithm for Multiple Exposures

Page 38: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

• Experimental details Four coded “read pulses” are arranged in a pulse train. One “pump pulse” is visualized by the “read pulses”. The part of the “read pulses” that intersects with the

“pump pulse” is detected by the camera.

A. Ehn et al., Light: Science & Applications (2017) 6, e17045; doi: 10.1038/lsa.2017.45

Experimental design

Page 39: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

0 ps 20 ps

Experimental results Identifying movie frames

Page 40: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

Raw data Extracted film frames Movie

A record high frame rate of 5 THz has been demonstrated. Higher frame rates can be reached with shorter laser pulses. Independent of wavelengths of the laser and detected signals. Can also be used for instantaneous 3D imaging Applicable for studies of dynamical processes in physics,

chemistry and biology over a wide range of time scales.

Experimental results Reaching frame rates of 5 THz

A. Ehn et al., Light: Science & Applications (2017) 6, e17045; doi: 10.1038/lsa.2017.45

Page 41: Applied Molecular Spectroscopy - Atomic Physics · • LIF thermometry restricted to high temperatures if molecular radicals are employed. For OH temperatures above 1500 K are needed

Thanks for your attention!

For further information contact

[email protected]