Combustion and Flame 235 (2022) 111707

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Combustion and Flame

journal homepage: www.elsevier.com/locate/combustflame

Detailed assessment of the thermochemistry in a side-wall quenching

burner by simultaneous quantitative measurement of CO2 , CO and
temperature using laser diagnostics
Florian Zentgraf a,∗, Pascal Johe a, Matthias Steinhausen b, Christian Hasse b,
Max Greifenstein a, Andrew D. Cutler c, Robert S. Barlow d, Andreas Dreizler a
a
Technical University of Darmstadt, Department of Mechanical Engineering, Reactive Flows and Diagnostics, Otto-Berndt-Str. 3, Darmstadt 64287, Germany
b
Technical University of Darmstadt, Department of Mechanical Engineering, Simulation of Reactive Thermo-Fluid Systems, Otto-Berndt-Str. 2, Darmstadt
64287, Germany
c
The George Washington University, Washington DC, USA
d
Barlow Combustion Research, Livermore, USA

a r t i c l e i n f o a b s t r a c t

Article history: This study focuses on exploring the thermochemistry in flame-wall interaction (FWI) for fully pre-
Received 18 March 2021 mixed side-wall quenching of a laminar, atmospheric-pressure dimethyl ether flame at equivalence ratio
Revised 17 August 2021
 = 0.83 by simultaneous measurement of CO2 and CO mole fractions and gas phase temperature T . The
Accepted 18 August 2021
applied laser diagnostics are dual-pump coherent anti-Stokes Raman spectroscopy (DP-CARS) targeting
Available online 5 September 2021
N2 and CO2 , laser-induced fluorescence of CO and OH, as well as thermographic phosphor thermometry.
Keywords: The extension to DP-CARS to study FWI processes is the first of its kind, previous studies only provided
Flame-wall interaction (CO,T ) measurements. The laser diagnostics are benchmarked and calibrated to an adiabatic test case
Dimethyl ether and assessed in accuracy and precision. Subsequently, the approach is used to measure the thermochem-
Dual-pump CARS istry close to a quenching wall. The nominal flame-to-wall distances from the experiment well match
LIF the numerical simulation data with a marginal offset of 20 μm. Conditioning the thermochemical data
Thermochemistry
with respect to the instantaneous quenching point, named quenching-point conditioning, enables a novel
Differential diffusion effects
tracing of the wall-parallel chemistry evolution across the quenching location. The study provides the
first comparison of experimental three-scalar measurements (CO2 ,CO,T ) with two-dimensional (2D) fully-
resolved chemistry and transport (FCT) simulations. The validation of numerical simulations can now rely
on the three scalars (CO2 ,CO,T ) instead of the two scalars (CO,T ) in past studies. The evaluation reveals
that this novel three-scalar measurement allows highly sensitive probing of the thermochemical states
and is clearly superior to the previously applied two-scalar approach. CO2 is less affected by the quench-
ing wall compared to CO. Differential diffusion effects are experimentally confirmed by comparison to
2D-FCT, with the (CO2 , T ) state space being more sensitive than (CO,T ). As the experimental methodology
proved feasible for laminar operation, a transfer to turbulent cases, where the numerical analysis using
direct numerical simulations (DNS) including FCT is limited, appears promising.
© 2021 The Combustion Institute. Published by Elsevier Inc. All rights reserved.

1. Introduction and motivation
The emerging consequences of human-induced climate change
and stricter legal limits for exhaust emissions demand new ap-
proaches to the energy conversion of carbonaceous fuels by com-
bustion. While it is possible in some areas of society to replace the
use of carbonaceous fuels with other concepts, such as the elec-
trification of urban individual transport, other areas will continue
∗
Corresponding author.
E-mail address: zentgraf@rsm.tu-darmstadt.de (F. Zentgraf).
to depend on the use of high-energy-density chemical energy car-
riers. These include aviation and ground freight using diesel en-
gines, where sustainable synthetic chemical energy carriers, either
e-fuels or fuels derived from biomass, will play an increasing role
in the future [1,2]. Consequently, there is a major fundamental re-
search interest in their combustion characteristics and related pol-
lutants, such as carbon oxides (COx ), nitrogen oxides (NOx ), un-
burned hydrocarbons, aldehydes, and soot. For example, dimethyl
ether (DME, CH3 –O–CH3 ) and oxymethylene ethers (OMEs, CH3 -
O-[CH2 -O]n -CH3 ) are considered to be promising diesel fuel surro-
gates featuring a reduced soot precursor formation [2–4] and a sig-
nificant NOx reduction potential [2]. For its gaseous state at ambi-

https://doi.org/10.1016/j.combustflame.2021.111707
0010-2180/© 2021 The Combustion Institute. Published by Elsevier Inc. All rights reserved.
F. Zentgraf, P. Johe, M. Steinhausen et al.
ent conditions, DME is considered less advantageous compared to
conventional liquid fuels in the transport sector [2]. Nevertheless,
DME is a representative of the partially oxygenated hydrocarbons
that are promising e-fuel pioneers, and it is related to the OMEs in
its chemical structure. Due to its low molecular complexity, DME
is well suited for fundamental research.
A further important topic in applied combustion devices that
is not yet fully explored and understood is the quenching of pre-
mixed flames at cold solid surfaces, called flame-wall interaction
(FWI). FWI is broadly relevant to combustion technologies and en-
vironmental protection because FWI involves non-desirable pro-
cesses, like wall heat loss or incomplete combustion causing pollu-
tants and soot. Especially, for more complex high-molecular-weight
fuels, it is well known that the molecular structure modifies FWI
and particularly the evolution of intermediate hydrocarbons, as for
example demonstrated early by Kiehne et al. [5] for propane or
Hasse et al. [6] for iso-octane. This results in the pressing need to
explore FWI for novel e-fuels, where different intermediate hydro-
carbons are formed and other chemical reaction pathways may be
relevant.
The major challenges in numerical studies on FWI are to predict
the impact of the non-adiabaticity to (1) the chemical progress by
reaction and (2) the convective and especially diffusive transport
in the vicinity of the quenching wall. In fully-resolved chemistry
and transport (FCT) simulations,1 applied for example in Ganter
et al. [7], Efimov et al. [8], Steinhausen et al. [9] for laminar flames
and in Gruber et al. [10], Ahmed et al. [11] for turbulent, generic
FWI configurations, the transport equations of combustion-related
species is solved directly. This approach is very accurate, however,
due to the high computational costs, FCT simulations of turbulent
flames are mostly suitable for generic configurations. Therefore,
it is necessary to reduce the combustion kinetics to enable the
simulation of technical applications. Thereby, chemistry manifolds
combine the accuracy of the FCT simulations with low computa-
tional costs. For FWI, different chemistry manifolds have been de-
veloped including Flamelet-Generated Manifolds (FGM, applied in
Ganter et al. [7], Efimov et al. [8], Steinhausen et al. [9]), Quench-
ing Flamelet-Generated Manifolds (QFM, applied in Efimov et al.
[8], Steinhausen et al. [9]) or Reaction-Diffusion Manifolds (REDIM,
applied in Ganter et al. [7], Steinhausen et al. [9], Straßacker et al.
[12,13]). To enable physical meaningful simulations of complex
combustion devices, it is essential to validate the computational
models employed, both in the DC simulations, as well as the re-
duced chemistry approaches. Thereby, generic experiments play a
crucial role by providing insights into the underlying physics of
FWI.
Experimental studies on two categories of FWI in premixed
flames – head-on quenching (HOQ, flame propagates normal to
wall) and side-wall quenching (SWQ, flame propagates parallel to
wall) – were recently reviewed by Dreizler and Böhm [14]. For an
experimental assessment of FWI, laser diagnostics are considered
most promising to achieve spatially and temporally resolved data
close to a solid surface without altering the local flow and reaction
conditions. Experimental studies on FWI can focus on various as-
pects of heat transfer, fluid mechanics, or chemical reactions rele-
vant to the quenching phenomenon. For example, investigations of
quenching distance [15,16], wall heat flux [15,16], or the interaction
of quenching with the flow field [17–19] are prominent and com-
monly reported. In contrast, the area of detailed near-wall thermo-
chemistry, i.e., the coupling of heat and temperature with chemical
reaction, has previously been covered only occasionally.
In the early 1980s, Clendening et al. [20] used a sponta-
neous Raman-scattering setup to measure profiles of the gas phase
1
also referred to as detailed chemistry (DC) in the cited literature.
2
Combustion and Flame 235 (2022) 111707
temperature and relative hydrocarbon number densities in SWQ.
Saffman [21] applied a comparable setup for temperature and
hydrocarbon mole fractions. However, temperature and species
concentrations were not measured simultaneously. Mokhov et al.
[22] assessed profiles of the gas phase temperatures (by a line re-
versal method using a spectral lamp), OH (absorption and laser-
induced fluorescence, LIF) and CO (by two-photon LIF) number
densities as well as velocities (by laser Doppler anemometry, LDA).
They used a SWQ configuration, but with the quenching wall posi-
tioned fully in the exhaust gas of the burner at equilibrium condi-
tions. Furthermore, it was not stated whether or not the data were
measured simultaneously. Fuyuto et al. [23] performed a compre-
hensive study in a SWQ device measuring two-dimensional distri-
butions of the gas phase temperature (by multi-line NO-LIF ther-
mometry), OH and CH2 O (both by LIF), as well as CO (by two-
photon LIF). However, the data were not measured simultaneously,
and species distributions were qualitative or semi-quantitative.
More recent studies on thermochemistry in FWI simultaneously
quantified the gas phase temperature T by coherent anti-Stokes
Raman spectroscopy (CARS) and the CO mole fraction XCO by two-
photon LIF [16,24,25] in HOQ and SWQ configurations. This en-
abled a shot-to-shot correlation of T to the corresponding XCO .
However, both parameters are influenced by the enthalpy loss at
the quenching wall. An additional major reaction species that is
less prone to the non-adiabaticity of the FWI process would be
desirable, e.g., a product species like CO2 or H2 O. So far and to
the authors best knowledge, the work of Bohlin et al. [26] is the
only experimental multi-parameter study simultaneously probing
six major combustion species (N2 , O2 , H2 , CO, CO2 , and CH4 ) by
application of an ultrabroadband CARS approach for assessing the
thermochemical state during FWI. Thus, for FWI experiments, there
is a further need to explore the thermochemistry quantitatively
and simultaneously beyond (CO,T ) using a complementary diag-
nostical setup.
Recently, the impact of DME fuel in FWI was addressed exper-
imentally by Luo and Liu [27] in a non-premixed HOQ configura-
tion, focusing on soot formation, as well as by Kosaka et al. in pre-
mixed SWQ with scope on thermochemistry by CO and gas phase
temperature [16] and the local heat release rate [28]. A numeri-
cal study on premixed DME combustion in SWQ was presented by
Steinhausen et al. [9]. The sparse treatment of DME as a generic e-
fuel in FWI processes in the literature calls for further fundamental
studies to understand the phenomenological behavior.
The presented experimental approach expands beyond the pre-
vious state-of-the-art on laser diagnostics in FWI. It aims to ad-
dress the open scientific requirements on FWI outlined in the
above paragraphs, namely to (1) extend previous diagnostic ap-
proaches for measuring three scalars simultaneously, (2) gain fur-
ther insight into wall-bounded DME combustion and (3) provide
more comprehensive validation data for CFD. The specific scopes
of this study are:
• Gain more insights into the thermochemical states during FWI
in an atmospheric, fully premixed SWQ configuration. The pre-
vious approach of simultaneously measuring CO and T is ex-
tended by additionally measuring CO2 such that the following
parameters were captured simultaneously: (1) CO2 mole frac-
tion XCO2 , (2) CO mole fraction XCO , (3) gas phase tempera-
ture T , (4) qualitative OH radical distribution. The post-flame
wall temperature is additionally assessed by laser diagnostics
for boundary condition control (for wall temperature reference
at higher wall temperatures). Here, CO2 is selected because, as
a product species, it is expected to be less affected by the en-
thalpy loss through the quenching wall, and its mole fraction
should rise monotonically with progressing reaction. This also
makes CO2 a suitable component of a progress variable defini-
F. Zentgraf, P. Johe, M. Steinhausen et al.
Fig. 1. Schematic side view of the atmospheric SWQ burner facility. Zoomed views of the quenching region outline the relevant field-of-views (FOVs) and the near-wall
measuement locations. Numbers indicate dimensions in millimeters.
tion for reduced chemistry manifolds for both DME [9] and CH4
[7].
• A general assessment of the feasibility, accuracy, and precision
of the combined approach using dual-pump CARS, targeting N2
and CO2 , with CO-LIF to simultaneously measure (CO2 ,CO,T ).
Thus, no parameter variation is performed, and the focus is at
one selected DME/air mixture at  = 0.83, ∼ 60 ◦ C wall tem-
perature with laminar inflow.
• Focus on DME as a relevant fuel from renewable sources, with
main emphasis on its differential diffusion effects in near-wall
combustion, which are already much more pronounced than for
CH4 at atmospheric pressure. As the presented experiments are
limited to atmospheric pressures, more complex features like
low temperature heat release (LTHR) and negative temperature
coefficients (NTC) are beyond the scope of this study.
2. Experimental and numerical approach
In the following four subsections, the burner facility is de-
scribed, the implemented laser diagnostics are outlined in detail
with a brief insight into data processing, the diagnostic methods
are benchmarked to an adiabatic reference case, and the numerical
simulation data used for comparison are documented.
2.1. Burner facility
Measurements were performed within an established side-wall
quenching (SWQ) burner facility [16,19,25,28] shown in Fig. 1. A
fully premixed fuel-air mixture was side-fed to the inlet plenum
of the burner and subsequently guided through a combination of
coarse meshes, fine meshes, and a honeycomb structure to ho-
mogenize the inflow. The mixture then passed through a converg-
ing (Morel) nozzle, resulting in a nearly top-hat velocity profile
at the nozzle exit. An optional turbulence generating grid could
be placed inside the nozzle. Without this grid, the burner oper-
3
Combustion and Flame 235 (2022) 111707
ated under laminar flow conditions. However, for laminar condi-
tions, a remaining unsteadiness of the flame existed that has been
attributed to Helmholtz resonances [25]. The present measure-
ment cases exhibited fluctuation of the quenching point of about
±310 μm (±1σ ) along the wall. These values are consistent with
past measurements [25]. Remaining fluctuations were corrected for
using the instantaneous OH-LIF signal as described in Section 2.2.3.
After exiting the nozzle, a V-shaped flame was stabilized by a ce-
ramic rod (1 mm diameter). One branch of this flame quenched
at a temperature-controlled, stainless steel wall. The wall surface
is curved in the xy-plane (see top view in Fig. 2) with a radius
of 300 mm to allow the laser diagnostics to probe close to the
wall. For orientation, this manuscript labels directions using the
prefixes introduced by the coordinate system in Fig. 1. The y-axis
denotes the wall-normal and z the streamwise direction parallel to
the wall, while x gives the out of plane direction.
The wall was temperature controlled by either flushing
ambient-temperature water or heated thermal oil through the
cooling duct. An air co-flow shielded the central premixed main
flow. The burner was operated at atmospheric conditions. The
Reynolds number of the main flow was maintained at approxi-
mately 5900. This value is based on the hydraulic diameter of the
nozzle exit (approx. 40 × 40 mm2 ) and considers the physical con-
ditions at 20 ◦ C, relevant for the nozzle exit. As the burner was
designed with a convergent (Morel) nozzle followed by a short
straight section, a nearly flat, laminar velocity profile with thin
boundary layers results that is not yet transitional at the burner
exit. Three sheath thermocouples (type K, 1.5-mm diameter) on
the center line of the wall were used to monitor the temperature
of the quenching wall surface. The tip of each thermocouple was
placed approximately 200 μm to 400 μm below the solid surface.
Calibrated mass flow controllers (Bronkhorst High-Tech B.V.) were
used to define the flow conditions and equivalence ratios. For DME
fuel at  = 0.83 (see operation condition in Table 1) the uncer-
tainty in the equivalence ratio is δ  = 0.01 derived via error prop-
F. Zentgraf, P. Johe, M. Steinhausen et al.
Fig. 2. Schematic of the applied laser diagnostic setup subdivided in a side and front view for the laser beams as well as a top view for the detection arrangement. Numbers
on lenses indicate the focal length in millimeters.
Table 1
Operating conditions of the SWQ burner in this study. Twall expresses the minimum to maximum thermocouple
temperatures during operation, temporal average was 332 K with 2.5 K standard deviation.
fuel  (−) inflow Re (−)
DME 0.83 laminar 5900
agation from the fuel and air flow rate deviations of the calibration.
The entire burner facility was mounted on a computer-controlled
traversing system (x-, y-, z-axes).
To perform the measurements, the entire burner assembly was
moved, while all diagnostics remained fixed. In the zoomed view
in Fig. 1, the fields-of-view (FOV) of the individual laser diagnos-
tics and the domain of the numerical simulation are shown. The
OH-LIF covered a FOV of (y, z ) = (24 mm, 32 mm ), while the
simulation domain featured (y, z ) = (6 mm, 30 mm ). For DP-
CARS and CO-LIF, a 2D field is scanned point by point around the
quenching area as outlined by the sketch on measurement loca-
tions in Fig. 1. For the y-direction, 13 horizontal locations were
acquired (0.1 to 1 mm with 0.1 mm increment and at 1.5, 2 and
4 mm wall-distance). This was done at five different z-locations
centered around the quenching height (the z-location where the
flame quenches). Individual resolutions are given in Section 2.2.
Please note that the coordinate system embedded in Fig. 1 is for
directional purpose only and does not show the origins of these
axes. For data analysis, a relative coordinate system was used with
z = 0 mm placed at the quenching height (individually by condi-
tioning for each recorded sample using simultaneous OH-LIF imag-
ing) and y = 0.1 mm at the nominal wall-closest position.
A comprehensive parameter variation was done during the
measurements using different equivalence ratios, fuels, wall tem-
peratures, and both laminar and turbulent flow cases. For demon-
stration, this study focuses on evaluating the capabilities of the ex-
tended laser diagnostics for assessing the thermochemistry in SWQ
for only one set of operation conditions summarized in Table 1.
The wall temperature range in Table 1 resulted from the thermo-
couples located underneath the wall surface downstream of the
quenching height. A benchmark with the embedded thermographic
phosphor thermometry (TPT) was done for the higher wall temper-
ature cases but not for the cold wall case at ∼ 60 ◦ C (333 K nom-
Combustion and Flame 235 (2022) 111707
ujet (m/s) ucoflow (m/s) Ptherm (kW) Twall (K)
2.2 2.1 6.1 327–338
inal) discussed here. For the higher wall temperature cases, the
thermocouple temperatures (mean ± standard deviation: 626 K ±
6 K) agreed well with TPT measurements (670 K ± 0.7 K). In this
higher wall temperature case, the average TPT result (or measure-
ment) is 44 K higher (∼ 7% in absolute value) than the thermocou-
ple values, which is physical as the TPT is measured at the sur-
face, while the thermocouples are embedded just below the sur-
face. However, the thermocouple measures do sufficiently express
the wall surface temperature within 7% uncertainty and are ex-
pected to accurately report the wall temperature also for the lower
wall temperature case discussed here as temperature gradients are
lower compared to the higher wall temperature case.
2.2. Laser diagnostics
To study the SWQ phenomena, a comprehensive set of laser di-
agnostics was applied. The main features of the laser optical setup
are provided in Fig. 2. In total, four diagnostics were implemented
simultaneously: (1) dual-pump coherent anti-Stokes Raman spec-
troscopy targeting N2 and CO2 , (2) two-photon laser-induced fluo-
rescence of carbon monoxide, (3) planar laser-induced fluorescence
of the hydroxyl radical and (4) thermographic phosphor thermom-
etry. The details of the individual approaches are outlined in the
following.
2.2.1. Dual-pump coherent anti-Stokes Raman spectroscopy
(DP-CARS)
The DP-CARS approach was applied to provide a quantitative
measure of both the gas phase temperature via N2 , as a very ro-
bust temperature indicator in combustion environments, and the
CO2 mole fraction XCO2 . The concept of DP-CARS was introduced
by Lucht [29] to simultaneously measure the spectra of two species
at a time with one detector. In this approach, a narrow-band dye
4
F. Zentgraf, P. Johe, M. Steinhausen et al.
laser was used as one pump laser along with a frequency-doubled
Nd:YAG laser as the second pump laser and a broadband dye laser
as the Stokes laser [29]. For measuring N2 and CO2 using a 607
nm broad-band Stokes laser, N2 (Raman shift around 2330 cm−1 )
was pumped by 532 nm and probed around 560 nm, while CO2
(Raman shift around 1380 cm−1 ) was pumped around 560 nm and
probed by 532 nm [30]. The major advantages of DP-CARS were
that both species are probed exactly at the same time and loca-
tion, as their CARS signals are resulting from the same three laser
beams and the resulting spectra are nearly in the same wavelength
range, allowing them to be imaged on one detector [31]. These
advantages yielded an excellent correlation behavior of the two
measured species, which is of great importance for proper thermo-
chemistry studies. The experimental implementation in this study
followed the outlines of Lucht et al. [31].
Two custom-modified Q-switched, frequency-doubled Nd:YAG
lasers (Spectra-Physics PIV 400, 10 Hz, 5–8 ns pulse width, in
which the PIV-overlap was removed and individual cavities were
split, resulting in two independent lasers at 532 nm) were used
as excitation sources. The first Nd:YAG laser was split into two
beam paths. One part of the beam served as first pump wave-
length at 532 nm and was guided to the DP-CARS overlap optics
directly. The second beam path was used to pump the custom-
built broad-band, modeless Stokes laser (design principle by Ewart
[32]). This laser was operated with a dye mixture of Rhodamine
610 and 640 resulting in a spectral profile centered around 607 nm
having ≈ 8 nm FWHM. The second Nd:YAG laser served as optical
pumping source for a narrow-band dye laser (Radiant Dyes Laser
& Accessories GmbH, NarrowScan) operated with Rhodamine 590
dye at 561.7 nm, serving as second pump wavelength. Note that
561.7 nm is used here instead of 560 nm in Roy et al. [30] or
561 nm in Lucht et al. [31] to achieve a good spectral separa-
tion of the N2 and CO2 . The three individual beams (532, 561.7
and 607 nm) were energy-controlled by combinations of half-wave
plates and polarizing beam splitter cubes and subsequently colli-
mated using telescopes with spherical lenses. The individual beams
passed through delay lines and were overlapped according to their
phase matching conditions (α532 ≈ 2.0◦ , α561 ≈ −1.9◦ , α607 ≈ 2.2◦ ;
angles with respect to the principal beam direction) using a planar
BOXCARS arrangement. Finally, they were guided to the burner fa-
cility and focused to the region of interest (ROI) using a spherical
lens ( f = +300 mm). The average pulse energies in the ROI were
set to ≈ 25 mJ (532 nm, 1% coefficient of variation (CV)), ≈ 24 mJ
(561.7 nm, 3% CV) and ≈ 13 mJ (607 nm, 2% CV), respectively. These
average pulse energy values are reduced by ∼ 15% from those used
by Lucht et al. [31]. The CARS probe volume, i.e. the measurement
resolution, spans about (y, z ) = (67 μm, 54 μm) (1/e2 value
of ICARS ∝ I532 · I561 · I607 intensities on beam monitor) in the cen-
tral plane location at x = 0 mm, while the interaction length in x-
direction is estimated to x = 2.4 mm (1/e2 value of non-resonant
signal in a 100 μm thick glass plate).
The coherent DP-CARS signal at around 496 nm was collected
using another spherical lens ( f = +300 mm) and was split from
the overlapping 561.7 nm radiation by using three lowpass dichroic
mirrors (Thorlabs Inc., DMLP550L, 50% transmission/reflection at
550 nm). While ≈ 90% of the 561.7 nm beam was transmitted
on each mirror, the DP-CARS signal was reflected. Afterwards,
an achromatic half-wave plate (Thorlabs Inc., AHWP10M-600, for
40 0–80 0 nm) was used to optimize the polarization of the DP-
CARS signal with respect to the spectrometer. Two interference
filters were used to remove remaining spectral residuals super-
imposed on the DP-CARS signal: (1) a notch filter at 532 nm
to remove scattered light, (2) a short pass filter (Thorlabs Inc.,
FESH0550, cutoff wavelength 550 nm) to remove the rest of the
transmitted 561.7 nm intensity. A filter wheel was used to op-
tionally put neutral density filters into the signal path (options:
5
Combustion and Flame 235 (2022) 111707
0.5%, 10% transmission or no filter) in case the DP-CARS signal
saturated the detector, e.g., at ambient temperatures. The sig-
nal was focused to the slit of the spectrometer (SPEX Indus-
tries Inc., 1704, 1 m spectrometer, 2400 lines/mm grating) using
a spherical lens ( f = +100 mm). The spectra were recorded us-
ing a cooled, backside-illuminated CCD camera (Princeton Instru-
ments, Pixis 400, 1 ms exposure time). In the horizontal wave-
length direction, all 1340 pixels were used, while in the verti-
cal direction only 25 pixels were used and fully hardware binned
prior to readout. All optics used in the setup had anti-reflective
coatings. For correction purpose, non-resonant DP-CARS spectra
were recorded in pure argon gas. This was done several times
during each measurement day, periodically between operation
points.
The processing flow to derive gas phase temperature and CO2
mole fraction from the DP-CARS raw spectra is outlined in Fig. 3.
Initially, the raw spectra were pre-processed and their intensity
was corrected by a mean background subtraction as well as a
normalization to a mean non-resonant signal. The square root of
the intensity-corrected spectra was taken, and a dispersion cali-
bration was applied to assign the correct wavenumbers to the in-
tensities. For the dispersion calibration, experimental data recorded
in an adiabatic flat-flame burner was fit to a simulated spectrum
under identical conditions by a least square scheme, optimizing
the wavenumber expansion and shift (a linear correction). Sub-
sequently, these spectra were processed by a spectral fitting al-
gorithm [33] with the gas phase temperature, N2 and CO2 mole
fractions as well as the wavenumber shift as free fitting parame-
ters. This procedure was applied to the single-shot spectra directly,
yielding quantitative single-shot gas-phase temperature and CO2
mole fraction.
Due to its lower concentration and quantum mechanical charac-
teristics, the CO2 signal was weaker than the N2 signal at elevated
temperatures approaching the burnt gas. To compensate for a bias
originating from weak CO2 signals, e.g., caused by beam steering,
appropriate post-processing steps were performed. First, an em-
pirical thresholding procedure was applied to judge the CO2 sig-
nal quality from the most prominent CO2 feature at ≈ 2373 cm−1
(i.e., the 000 0–100 0 band of CO2 ). All data with a
spectral fit fea-
turing an absolute baseline to peak difference  ICO2 ≥ 0.6 were

considered for further analysis, while data with  ICO2 < 0.6 was
excluded (see visualization in Fig. 3). The empirical thresholding
criterion was validated, based on the (CO2 , T ) state space evo-
lution of data from the free branch of the laminar V-stabilized
flame and comparison with the corresponding numerical simula-
tion. This is outlined in the final plot in the DP-CARS processing
flow
 in Fig. 3, where green symbols visualize the excluded  data
( ICO2 < 0.6, 20% of samples) and black symbols ( ICO2 ≥ 0.6,
80% of samples) depict the retained data. From these observations
it is evident that the criterion is effective in removing unphysi-
cal samples from the (CO2 , T ) state space. Note that for the near-
wall data presented in Section 3, only 10% of the samples were
excluded by this procedure, indicating a high quality of the ac-
quired data. Second, an additional calibration was applied to the
data after thresholding. Again, this is done using the known evo-
lution of (CO2 , T ) in the adiabatic reference case. For this purpose,
the CO2 mole fractions of both the simulation and experiment are
curve-fitted over temperature. A calibration coefficient as a func-
tion of temperature can be derived from the fitted polynomials as
CCO2 ,calib (T ) = f itCO2 ,sim (T )/ f itCO2 ,exp (T ). This coefficient is multi-
plied to the experimental CO2 mole fractions using the correspond-
ing temperature for correction towards the simulation values. The
calibration further aided in improving the average accuracy of the
CO2 mole fractions from 9% (not calibrated, see final plot for DP-
CARS in Fig. 3) to 2% (calibrated, see Fig. 4(a) and (f)). This is fur-
ther discussed in Section 2.3.
F. Zentgraf, P. Johe, M. Steinhausen et al.
Fig. 3. Flowchart summarizing the processing methodology for DP-CARS, CO-LIF and OH-LIF.
2.2.2. Two-photon laser-induced fluorescence of carbon monoxide
(CO-LIF)
The CO mole fraction XCO was assessed using two-photon CO-
LIF. The excitation of CO molecules was done within the Hopfield-
Birge bands at 115.05 nm using two-photons at 230.09 nm for the
transition B1  + ←← X 1  + (0, 0 ), while the emission of the transi-
tion B1  + → A1 u (0, 1 ) in the Ångström bands was detected [34].
This scheme is well established in combustion diagnostics and the
implementation of this approach in this study follows the outlines
of [16,24,25,35] for previous FWI investigations.
A Q-switched, frequency-doubled Nd:YAG laser (Spectra-Physics
GCR 4, 10 Hz, 5–7 ns pulse width (FWHM)) was used to pump
a narrow-band dye laser (Sirah Lasertechnik GmbH, PrecisionScan,
2400 lines/mm) operated with Pyridine 1 dye. The fundamen-
6
Combustion and Flame 235 (2022) 111707
tal dye laser emission at 690.27 nm was frequency tripled to
230.09 nm in the UV using a second harmonic and third harmonic
generation stage (i.e., 345.135 nm was mixed with 690.27 nm to
230.09 nm). The fundamental wavelength was continuously mea-
sured by a wavelength meter (HighFinesse GmbH, WS6) and used
to control the grating position of the dye laser. This control loop
guaranteed a constant excitation wavelength at 230.09 nm within
0.025–0.036 cm−1 (difference between maximum and minimum
average wavenumber measured over a measuring day). The UV
beam was guided to the burner facility using high reflectivity di-
electric mirrors. A combination of half-wave plate and Glan-laser
double escape polarizer (Lattice Electro Optics Inc., PCGL-a-BBO-
04) was used to control the energy. The usual average pulse en-
ergy within the ROI was ≈ 0.7–0.9 mJ (5% CV). A fused silica glass
F. Zentgraf, P. Johe, M. Steinhausen et al.
plate (≈ 10 mm thickness) was placed in the beam path to gener-
ate both an energy and beam profile reference. The front side re-
flection was deflected to an energy meter (Coherent Inc., EM USB
J-10MT-10KHZ), where the pulse energy was measured for a shot-
to-shot energy correction. The backside reflection of the glass plate
was guided to a beam monitor (DataRay Inc., WinCam D) equipped
with a UV-converting beam profiler (Star Tech Instruments Inc.,
BSF23). Beam profiles were only measured occasionally to check
location and intensity distribution. Note that the beam profile of
the laser didn’t change during the measurements, but the overall
pulse energy did slightly drop in its average by ∼10–18% over a
measuring day. The beam was focused to the ROI using a spherical
lens ( f = +300 mm) with a beam diameter of (y, z ) = (260 μm,
200 μm) (1/e2 value of Gauss-fitted profiles). Since the applied CO-
LIF is a two-photon process, the probe volume size is not sim-
ply given by this beam diameter but rather determined by the
area with laser intensity In , with the exponent n ≤ 2 considering
the laser fluence dependency, impacted by photo-ionization (here:
n = 1.68). The effective probe volume diameter, i.e., dimensions in
y- and z-direction, corresponding to the laser intensity I1.68 rele-
vant for CO-LIF here is (y, z ) = (140 μm, 140 μm) (1/e2 value
of Gauss-fitted profiles). In x-direction, the probe volume for data
analysis spans 2 mm in length to overlap well with the DP-CARS
probe volume. To finally combine and overlap the CO-LIF beam
with the DP-CARS, a small rectangular mirror (10 × 20 mm2 ) was
placed between the upper (532 and 607 nm) and lower (561.7 nm)
DP-CARS beams directly after their transmission through the focus-
ing lens.
The CO-LIF emission was detected by an intensified relay op-
tic (IRO, LaVision GmbH, low speed IRO) gated at 100 ns to sup-
press background and flame luminosity and recorded using a CCD
camera (LaVision GmbH, Imager E-Lite 1.4M) with 10 ms exposure
time to fully capture the phosphor decay of the IRO and a 4 × 4
hardware binning. The IRO was operated in the linear regime. A
reduced ROI of 70 (horizontal) by 30 (vertical) bins centered at
the CO focus was used, corresponding to 3.5 × 1.5 mm2 (bin size
≈ 50 μm). The signal was collected with a customized imaging op-
tics consisting of an achromatic lens (Qioptiq Photonics GmbH &
Co. KG, G3222670 0 0, f = +160 mm, 80 mm diam.), an interference
filter (Laser Components GmbH, LC-HBP 490/20-75, >95% trans-
mission at 480–500 nm) and an objective lens (Canon, EF 135 mm
f/2L USM, focused to infinity). The entire imaging system was pro-
tected from thermal radiation by a heat shield cooled with a N2 -
flow.
The CO-LIF raw signal was turned into quantitative mole frac-
tions using a well-established calibration procedure [16,24,25].
However, the procedure was advanced for the application in the
current setup and is outlined under CO-LIF in Fig. 3. The quantifi-
cation to CO mole fractions XCO (y, z, i ) was done by
1 T (i ) 1 f itCO,sim (T (i ))
XCO (y, z, i ) = ICO (y, z, i ) · · · · (1)
a + b · E n (i ) T0 W (y, z ) f itCO,exp (T (i ))
       
(I ) (II ) (III )
with respect to the probed y- and z-location as well as sample
number i. Roman numbering (I) to (IV) summarize individual cor-
rection steps with their impact and parameters explained in the
following. Initially, a pre-processed CO-LIF intensity ICO (y, z, i ) was
derived by

ICO (y, z, i ) = Iraw (x, z, i ) − I¯BG (x, z ) − IBL (i )
z x
from individual raw images Iraw (x, z, i ). An average background
I¯BG (x, z ) was subtracted (recorded between consecutive laser
pulses, flame on) and the resulting signal was integrated in x-
direction, i.e., principal beam direction, within a 2 mm region
Combustion and Flame 235 (2022) 111707
centered around the DP-CARS probe volume. Then, a Gaussian was
fit in z-direction, i.e., orthogonal to the principal beam direction;
the intensity beyond the 1/e2 -bounds was subtracted as baseline
intensity IBL (i ), and the intensity within the 1/e2 -bounds of the
fitted Gaussian was subsequently integrated, ending up in one in-
tegrated intensity value ICO (y, z, i ) for each raw image i. This in-
tegrated intensity was subsequently corrected using Eq. (1) for
shot-to-shot energy fluctuations (I), local density (II), and geomet-
rical influences (III), as previously described by Jainski et al. [25],
and is finally turned into quantitative values using a calibration
polynomial recorded in the free flame branch (IV). Here, the non-
linear energy correction (I) followed a laser energy (E) dependency
∝ E n (i ) with n = 1.68 for the case presented in this study (see
Table 1). It was measured in-situ within the exhaust gas of the V-
shaped flame by varying the laser pulse energy. The value of the
exponent n < 2 confirms the presence of photo-ionization of CO
molecules, that promotes a signal less dependent on the quench-
ing environment, as discussed below. By decreasing the laser en-
ergy, n was chosen above the value in previous studies, like n =
1.24 in Jainski et al. [25], to minimize photolysis-generated CO
from CO2 that could bias the combustion-generated CO2 quan-
tification via DP-CARS. Exponent values n ≈ 2, as achieved using
femtosecond lasers [36], are hardly realizable using the applied
nanosecond approach. The instantaneous temperature values T (i )
from simultaneous DP-CARS divided by a reference temperature
T0 = 300 K were used to correct for the local density (II). A geo-
metric correction (III) considered the influence of the quenching
wall distance on the CO signal (due to reflections of the stainless-
steel wall, the intensity is slightly rising when approaching the
wall). The correction function W (y, z ) was generated by operat-
ing the burner with a fully homogeneous calibration gas mixture
(1% CO, 99% N2 ). For wall-distances of y ≥ 5 mm, W (y, z ) = 1. For
final quantification, a calibration polynomial (IV) was derived by
fitting corrected experimental (CO,T ) data (on T = 50 K incre-
ments) recorded in the free flame branch to a non-adiabatic sim-
ulation (see Section 2.4). This was done in the same manner as
for (CO2 , T ) in DP-CARS above and resulting in a calibration coef-
ficient CCO,calib (T (i )) = f itCO,sim (T (i ))/ f itCO,exp (T (i )) as function of
the instantaneous temperature. Such a calibration procedure cov-
ers influences from varying Boltzmann fractions, quenching envi-
ronment and ionization, as pointed out by Mann et al. [24]. The
different chemical composition between the adiabatic and non-
adiabatic flame branch at a given temperature causes a change
in the quenching rate which impacts the calibration. However, for
the given conditions, the quenching rate Q and the ionization rate
R are in the order of 109 s−1 as estimated with an in-house CO-
LIF simulation code based on [37] with quenching data from [38],
an ionization cross-section of 1017 cm−2 [39] and ∼ 0.3 GW/cm2 as
computed from the pulse energy, pulse duration and area of the
focal spot. For this estimation, a CH4 flame at 0.83 equivalence ra-
tio was simulated as there is no literature data on the quenching
  cross section of DME. Effectively, as R and Q are in the same or-
(IV ) der of magnitude, a change in Q loses its impact on the fluores-
cence quantum yield by approximately a factor of two. This ap-
proach thus allows transferring the calibration to different chemi-
cal environments as long as the temperature is measured simulta-
neously. For even higher fluences, the LIF signal becomes nearly in-
dependent of quenching. This has been more intensively discussed
in Greifenstein et al. [35]. This argument has also been made in
Voigt et al. [40] that in this regime of intensities, the LIF signal be-
(2) comes independent of the composition-dependent quenching even
at higher pressures, with associated higher quenching rates. How-
ever, this increases issues with photolytic production of CO by dis-
sociation of CO2 [36,41]. The used fluence presents a carefully se-
lected compromise between these effects to obtain the best possi-
ble accuracy.
7
F. Zentgraf, P. Johe, M. Steinhausen et al.
2.2.3. Planar laser-induced fluorescence of hydroxyl radical (OH-PLIF)
The hydroxyl radical OH was visualized qualitatively by a pla-
nar LIF (PLIF) setup to determine the flame front position and the
quenching location. In OH, transitions in the A2  − X 2  system
are used for laser excitation and the resulting detection [42]. Past
studies frequently applied the UV radiation of excimer lasers, for
example at 248.45 nm [23] or 291.5 nm/313 nm/268.5 nm [43],
and used various different transitions for exciting OH, while recent
studies on FWI excited the Q1 (6) transition around 283 nm using
the frequency doubled radiation of dye lasers [16,25], to only name
a few. The latter scheme using dye lasers is applied here as the
presented study aims at simply visualizing the qualitative spatial
distribution of OH.
A Q-switched, frequency-doubled Nd:YAG laser (Spectra-Physics
PIV 400, 10 Hz, 5–8 ns pulse width, only one cavity used) was used
for optically pumping a narrow-band dye laser (Sirah Lasertechnik
GmbH, Double Dye, 2400 lines/mm, only one cavity used) operated
with Rhodamine 590 dye. The fundamental wavelength was set to
567.86 nm (in air) and was frequency doubled to 283.93 nm. This
corresponds to an excitation of the Q1 (9) transitions of the OH rad-
ical [44]. A half-wave plate was placed in front of the frequency
conversion unit to control the final pulse energy in the UV, i.e., the
conversion efficiency, while preserving the beam profile. Pulse en-
ergies within the ROI were ≈ 0.3–0.4 mJ (10% CV). The UV beam
was guided to the burner facility by high reflective dielectric mir-
rors. A combination of spherical and cylindrical lenses was used to
form a laser light sheet. First, a Galilean telescope ( f = −100 mm
and f = +200 mm) expanded and collimated the laser beam. Sec-
ond, a cylindrical lens ( f = +500 mm) compressed the expanded
beam to the laser light sheet featuring 220 μm width in the ROI.
To cover both the quenching region and the thermographic phos-
phor coating with this laser sheet, an additional cylindrical lens
( f = −300 mm) was used to further expand the height of the laser
light sheet (approximately 60 mm height in ROI). Note that the ex-
citing laser light sheet was introduced to the ROI inclined (angle of
≈ 40◦ to horizontal) from above the CO-LIF detection system due
to the limited available space near the burner.
The OH-PLIF signal was collected using an objective lens (B.
Halle Nachfl. GmbH, 150 mm, f/2.5) equipped with an interfer-
ence filter (Laser Components, BP300-325, 305–340 nm transmis-
sion). The emission was recorded using an IRO (LaVision GmbH,
low speed IRO) gated at 100 ns combined with a CCD camera (LaV-
ision GmbH, Imager E-Lite 1.4 M) with 10 ms exposure time and a
3 × 3 hardware binning (bin size ≈ 69 μm). Note that the entire
OH detection system was mounted inclined (angle of ≈ 15◦ to hor-
izontal) above the DP-CARS excitation beams.
The processing is outlined under OH-LIF in Fig. 3 and follows
the procedure for flame front and quenching point detection de-
scribed in the work of Jainski [45]. Here, the procedure is refined
for the circumstances of the current study. OH-LIF raw images
were processed by an average background subtraction (recorded
between consecutive laser pulses, flame on), followed by two spa-
tial filtering steps: (1) a filtering in the Fourier-domain to selec-
tively remove a residual striped pattern on the laser light sheet
(most likely due to beam steering); (2) a 5 × 5 moving average fil-
ter to reduce spatial noise. Both filtering procedures enabled a ro-
bust calculation of the two-dimensional gradient magnitude, and
the maximum gradient magnitude value in y-direction for each z-
location was used to identify the flame front position. The quench-
ing point was then approximated from the flame front trace (gra-
dient magnitude normalized to [0; 1] on the trace) at the (y, z ) lo-
cation where the normalized gradient magnitude first exceeded a
value of 0.3, approaching from the post-flame direction. This value
was chosen empirically to provide robust detection of the quench-
ing location in the presented study (see results in Fig. 3 under OH-
LIF). However, for reproduction in future studies, i.e., with a differ-
8
Combustion and Flame 235 (2022) 111707
ent sensitivity in the detection setup, this value may need to be
adapted. Finally, all DP-CARS/CO-LIF data were conditioned to the
instantaneous quenching point by this scheme, to correct for the
remaining unsteadiness of the flame.
2.2.4. Thermographic phosphor thermometry (TPT)
Please note that the benchmark values from TPT were not used
for the low wall temperature case at 60 ◦ C discussed here but for
controlling the higher wall temperature cases only. The values are
not used for correlation with thermochemistry but are used to
control the boundary conditions. Thus, the TPT diagnostic is an
essential part of the simultaneous thermochemistry measurement
setup and is briefly described here for completeness.
A decay-time approach was applied using powder of the ther-
mographic phosphor Gd3 Ga5 O12 :Cr3+ ,Ce3+ (GGG:Cr,Ce), as in a
previous study [16]. The phosphor was airbrush-coated on the
quenching wall in the far post-flame region. For preparation, 1 g
of GGG:Cr,Ce was mixed with 5 ml high-temperature binder (ZYP
Coatings Inc., HPC binder). For excitation of the thermographic
phosphor, the OH-PLIF setup described in the paragraph above
was used. The signal was captured with an objective lens (Nikon,
Nikkor 50 mm, f/1.2) equipped with an interference filter (Edmund
Optics Inc., long-pass 650 nm, #84-759). The luminescence de-
cay was finally recorded by a combination of photomultiplier tube
(PMT, Hamamatsu Photonics, type H11901-20) and digital oscillo-
scope (Tektronix Inc., TDS5034B).
As shown by Kosaka et al. [16], the temperature of the quench-
ing wall can be assumed constant in the post-flame region down-
stream of the quenching point. Thus, TPT measurements in the far
post-flame region appear sufficient for control purpose. The de-
cay time was estimated iteratively using a non-linear least square
scheme, as described in Fuhrmann et al. [46]. The quantification in
terms of temperature was done by an in-situ calibration with an
aluminum block equipped with heating cartridges and thermocou-
ples.
2.2.5. Synchronization and matching of the diagnostics
For simultaneous multi-parameter studies, both temporal and
spatial matching of the systems is essential. All lasers and detec-
tion systems were synchronized using pulse generators (Quantum
Composers Inc., 9520 Series). The individual diagnostics were sep-
arated by 200 ns each to avoid crosstalk (temporal order: CO-LIF,
OH-PLIF, DP-CARS). All recording systems were operated at 20 Hz,
while laser systems were running at 10 Hz only. Thus, every sec-
ond image didn’t capture signal, but was used for the purpose of
background correction. For spatial matching of the diagnostics, a
100 μm reference pinhole was used to overlap both the DP-CARS
probe volume and the UV beam for CO-LIF in the center of the
ROIs (at x = 0 mm). The pinhole was further used as reference for
laser position in the two-dimensional OH-PLIF recordings. For spa-
tial scaling of the CO-LIF and OH-PLIF data, a customized calibra-
tion target was used.
Further important aspects include (1) the procedure to deter-
mine the distance of the matched probe volumes from the wall
and (2) the in-situ monitoring of the probe volume matching of
DP-CARS and CO-LIF during combustion operation. A detailed de-
scription of these aspects is given in Appendix A in the supplemen-
tary material, as they are considered extremely helpful for quality
assurance in the laser diagnostic community.
2.3. Experimental validation case
The experimental methodology for thermochemistry quantifica-
tion was validated with an adiabatic reference measurement. Here,
the free flame branch of the rod-stabilized V-flame was used. As
the zone where the free flame branch was probed is 16 to 20.5 mm
F. Zentgraf, P. Johe, M. Steinhausen et al.
Fig. 4. Evaluation of the diagnostical approach on the adiabatic flame branch as reference case. State spaces shown in (a)–(c), corresponding single-shot residua in (d) and
(e), relative accuracy and precision on 50 K temperature increments in (f) and (g). Error bars only displayed in (a) and (b). 4284 individual samples are considered. (For
interpretation of the references to color in this figure legend, the reader is referred to the web version of this article.)
away from the quenching wall in y-direction and heat loss via
radiation is negligible, the assumption of adiabaticity is valid,
and the flame may be represented by the one-dimensional, adia-
batic freely-propagating flame simulation described in Section 2.4.
The results are outlined in Fig. 4(a)–(c) in terms of the state
space, while (d) and (e) show the respective single-shot residua
r between simulation and experiment, giving an absolute mea-
sure for accuracy (μ(r ), light green line) and precision (scat-
ter in residuum). Figure 4(f) and (g) assesses a relative accuracy
(μ(r )/Xi,sim ) and precision (σ (r )/Xi,sim ) within individual tempera-
ture increments of 50 K; μ expresses the average, σ the standard
deviation and Xi,sim the corresponding simulations mole fraction of
species i. According to Fig. 4(a)–(c), after post-processing and cal-
ibration, the experimental data well reproduces the adiabatic sim-
ulation of CO2 , CO, and T in the state space. Please note that the
scatter is highest in the (CO,CO2 ) state space in Fig. 4(c), due to
the superimposed uncertainties in both CO2 and CO (compared to
the lower uncertainty in the temperature). The small gap appar-
ent in the experimental (CO,T ) data in Fig. 4(b) near 20 0 0 K is due
to a skipped measurement location while scanning over the adi-
abatic flame branch and does not affect overall data quality. For
the deduction of CO2 mole fraction from DP-CARS, it is empha-
sized that the values originating directly from the spectral fitting
algorithm already feature a good relative accuracy of ≈ 9% on av-
erage (Fig. 4(f) dark green hollow circles). As a function of tem-
perature, the relative accuracy of CO2 mole fraction is 5–10% up
to 1600 K, increasing to 20% at the highest temperatures. To fur-
ther improve the accuracy, the data were additionally calibrated to
the adiabatic simulation (see Section 2.2). This results in an aver-
age relative accuracy of about 2% that is nearly constant over the
full temperature range (Fig. 4(f) light green filled circles). The av-
erage relative precision of the CO2 mole fraction is roughly 16%,
decreasing somewhat with increasing temperature (Fig. 4(f) blue
crosses). The relative accuracy of the CO mole fraction, after cali-
bration, is ∼2% and approximately constant up to 1700 K (Fig. 4(g)
9
Combustion and Flame 235 (2022) 111707
light green filled circles). This high relative accuracy affirms a good
implementation of the CO calibration polynomial to transform cor-
rected LIF signals to mole fractions. Above 1700 K, the relative ac-
curacy deteriorates to approximately 10%. This is due to the de-
creasing absolute CO concentrations in the progressing oxidation
process. The average residuum (light green line in Fig. 4(e)) is ap-
proximately constant over the entire temperature range and is less
than 0.003 in CO mole fraction above 1700 K. Thus, the absolute
accuracy in terms of the average residuum appears constant, but
the relative accuracy deteriorates as the absolute CO concentration
becomes small. The average relative precision of the CO mole frac-
tion is near 10% (Fig. 4(g) blue crosses) within the temperature
range 750 K < T < 1500 K, where most of the relevant FWI pro-
cesses occur (wall distance: y = 120–320 μm). However, CO pre-
cision degrades at higher temperature due to lower CO signal lev-
els and the higher state-space gradient across the 50 K averaging
bins. The assessment of the gas phase temperature via DP-CARS re-
sults in a relative accuracy of 3% and precision of 4% (not shown
in Fig. 4), estimated from measurements in the fully burned gas
of the free branch. It is considered a conservative assessment to
only use the highest temperature samples for the evaluation of the
temperature quantification, as the nitrogen CARS signal is weak-
est there. Overall, the applied laser diagnostics seem to perform
well in capturing the (CO2 ,CO,T )-thermochemistry of the adiabatic
reference case with both a good accuracy and precision. Thus, it
is assumed that this experimental procedure remains valid for as-
sessing the thermochemical states in the non-adiabatic near-wall
region during flame quenching.
2.4. Numerical simulation benchmark cases
In this study, two numerical flame configurations are used to
complement the experiments: a one-dimensional, adiabatic freely-
propagating flame [47], in the following referred to as the adiabatic
simulation, and a FCT two-dimensional SWQ simulation referred
F. Zentgraf, P. Johe, M. Steinhausen et al.
to as the non-adiabatic simulation. The general setup of the SWQ
simulation (solver, grid, numerics) is described in Steinhausen et al.
[9]. In the present work, a recently developed mechanism [48],
consisting of 31 species and 140 reactions, is used in combination
with a mixture-averaged approach for diffusion [49,50]. To assess
the importance of diffusive transport during FWI, an equal diffusiv-
ity model (unity Lewis number for all species) is shown for com-
parison in the non-adiabatic case, additionally.
3. Results and discussion
This section presents and discusses results of the near-wall
thermochemistry. As mentioned previously, the focus is on a thor-
ough evaluation of one operation condition with DME fuel at  =
0.83, a cold wall (∼ 60 ◦ C) and laminar inflow.
3.1. Evaluation of the nominal wall distance
The nominal wall distance (y-direction) of the measured ex-
perimental data is examined, as the near-wall thermochemistry is
highly sensitive to this parameter. The comparison of experimental
and numerical data in past studies on FWI suggested that there is
an offset in y-direction between the nominal wall distance, where
the measurements are believed to have been taken, and the real
wall distance, where the measured result best agrees with phys-
ical reality. This offset is assumed to originate from multiple in-
fluences: (1) beam steering, (2) a spatial filtering of the laser di-
agnostics due to the finite beam width within the steep gradients
close to the wall, and (3) inaccuracy in defining the wall-closest
nominal position “y = 100 μm”. However, in the present study, the
major error is believed to be due to beam steering, while (2) and
(3) are considered negligible. As the wall closest y-position is set
during thermally steady FWI operation (see Appendix A in the sup-
plementary material for procedure), there should be only marginal
inaccuracy in defining the nominal “y = 100 μm” position. As it is
hardly possible to quantify the instantaneous position error caused
by beam steering from the experimental data, the effect can be
estimated by using the non-adiabatic simulation as benchmark.
Please note that the non-adiabatic simulation is also based on
modeling assumptions, and the use as benchmark may also suf-
fer inaccuracy. However, this approach appears to be a promising
way to give an estimation of the potential positioning error made
by beam steering in the experiment. The approach is outlined in
Fig. 5 using the (CO2 , T ) state space with the experimental data
at y = 100 μm nominal wall distance, but for different z-locations
(heights). The variation of (CO2 , T ) relative to the model arises to
the diagnostics precision as well as beam steering. The simulation
data evaluated at y = 120 μm wall distance (Fig. 5, solid orange
line) appears to fit best to the conditioned average values of the
experiment (Fig. 5, magenta triangles). The conditioned averages
are calculated on equidistant increments, each spanning 0.0025 on
the CO2 mole fraction axis. That conditioning method within the
state-space is named “state-space conditioning” in this manuscript.
This results in an apparent y-offset of 20 μm between experimental
and numerical data, likely to originate from beam steering. In the
following, this 20 μm y-offset is added to the nominal, experimen-
tal wall distance values. Furthermore, it appears that the majority
of experimental scatter is within a ±30 μm range in y-direction
compared to the numerical data (see red and yellow dashed lines
in Fig. 5). This range is seen as a superimposition of beam steer-
ing fluctuation and temperature precision due to spectral noise and
beam profile fluctuation within the DP-CARS probe volume. How-
ever, it is not possible to separate these influences here. In conclu-
sion, it can be stated that experiment and simulation match very
well after applying a small y-offset correction of 20 μm, as em-
10
Combustion and Flame 235 (2022) 111707
Fig. 5. Evaluation of the experimental data at y = 100 μm nominal wall distance,
to estimate an offset to the simulation data. 1983 individual samples are shown
in the scatter. The non-adiabatic simulation is provided with a mixture-averaged
transport approach. Both experiment and simulation contain values from stream-
wise z-positions spanning ±2 mm relative to the quenching height. (For interpre-
tation of the references to color in this figure legend, the reader is referred to the
web version of this article.)
ployed in the following. It is pointed out that evaluating such an
offset correction is only considered beneficial in the state space
rather than in the physical space, as the state space does not suffer
deviations in assessing the quenching location. This issue is further
discussed in the following section.
3.2. Thermochemistry progress with relative streamwise distance to
quenching height
This section discusses the evolution of the thermochemical
states in z-direction for data measured at the wall-closest y-
position of 120 μm. This is initially done for the physical space in
Fig. 6, followed by the corresponding description in the state space
in Fig. 7. The single-shot experimental data within the physical
space in Fig. 6 is described using both a smoothing spline fit (black
line) and averages conditioned with respect to the instantaneous
z-location of the quenching point (color-coded circles). This pro-
cedure is named “quenching-point conditioning” within this study
and calculates corresponding statistics within 100 μm increments
in z-direction after conditioning to the instantaneous z-location of
the quenching point that is set to z = 0 mm. Comparing the fitted
to the quenching-point conditioned averaged experimental data, it
is directly evident that binning or filtering the data with 100 μm
spatial increments in z-direction is not biasing the absolute val-
ues, as the color-coded circles exactly match the fitted black line.
In Fig. 6(a), the average experimental CO2 evolution (black line and
color-coded circles) across the quenching location closely matches
the corresponding simulation trace (red line). In the CO mole frac-
tions shown in Fig. 6(b) a minor deviation between the fitted ex-
perimental data and simulation is observed in both the peak lo-
cation (∼ 140 μm) and the peak value (∼0.007). Similarly, for the
experimental temperature evolution in Fig. 6(c), there are differ-
ences in peak z-location (285 μm) and value (35 K). These minor
differences may occur due to (1) the remaining unsteadiness of the
experimental flame, (2) the assumed boundary conditions in the
simulation (e.g., the inflow profiles). Consequently, visualizing ther-
mochemical data in the physical space is usually considered much
more sensitive than in the state space. Keeping this in mind, the
agreement between experimental results and numerical simulation
is considered excellent. The experiment thus provides an outstand-
ing validation of the simulation. It is emphasized that, apart from
F. Zentgraf, P. Johe, M. Steinhausen et al. Combustion and Flame 235 (2022) 111707

Fig. 6. Evaluation of the experimental data at y = 120 μm wall distance in z-direction in the physical space. 1983 individual samples are shown in the scatter. The ex-
perimental data is described by a smoothing spline fit (black line) and quenching-point conditioned averages calculated for each 100 μm increment on the physical z-axis
(color-coded circles). The non-adiabatic simulation (red line) is provided with a mixture-averaged transport approach. (For interpretation of the references to color in this
figure legend, the reader is referred to the web version of this article.)

Fig. 7. Assessment of the thermochemistry progression in z-direction at y = 120 μm wall distance in the state space with quenching-point conditioning applied. 92 to 152
individual samples are shown in each scatter plot. Adiabatic and non-adiabatic simulations are shown, with both simulations using a mixture-averaged transport model. The
non-adiabatic simulation features values z = ±2 mm relative to the quenching location. The right column (e), (j) and (o) includes additional experimental data at a z = +2 mm
bin location (green scatter points), corresponding to the fully reacted state. (For interpretation of the references to color in this figure legend, the reader is referred to the
web version of this article.)

11
F. Zentgraf, P. Johe, M. Steinhausen et al.
the y-offset correction in Section 3.1, the simulation has not been
adjusted in any way to match the experimental data.
Figure 7 shows the evolution of the thermochemical states in
the individual (CO2 , T ), (CO,T ) and (CO,CO2 ) scatter plots across the
quenching height in z-direction. Each column presents the samples
within a 200-μm bin in the wall-parallel z-direction centered at
the location given at top of the column (e.g., the z = −400 μm bin
in the first column ranges from z = −500 to −300 μm upstream of
the instantaneous quenching height). Negative values indicate loca-
tions upstream and positive values downstream of the quenching
height, which is located at z = 0 μm. As described in Section 2.1,
the flame quenching location fluctuates axially in z-direction. This
unsteadiness is accounted for by evaluating each sample individ-
ually against the instantaneous quenching height determined by
OH-LIF. Due to the unsteadiness, samples scatter across a range in
the thermochemical states because the spatial range for each sub-
plot extends 200 μm in streamwise z-direction. The numerical ref-
erences are sampled over z = ±2 mm range relative to the quench-
ing location. The evolution of thermochemical states is described
in the following.
At (z, y ) = (−400 μm, 120 μm) shown in the first column of
Fig. 7, (CO2 , T ) and (CO,CO2 ) correlations in (a) and (k) are sim-
ilarly reproduced by adiabatic and non-adiabatic simulations be-
cause the differences are small and below the experimental uncer-
tainty. However, the (CO,T ) correlation in Fig. 7(f) is more sensitive,
and non-adiabatic effects are more clearly visible. At (−200 μm,
120 μm) (Fig. 7, second column), the non-adiabaticity becomes
apparent for the (CO2 , T ) scatter in (b), while the (CO,T ) scat-
ter in (g) is clearly following the non-adiabatic simulation. At the
quenching height (z, y ) = (0 μm, 120 μm) (Fig. 7, center column),
both the (CO2 , T ) and (CO,T ) scatter plots in (c) and (h) coincide
with the non-adiabatic simulation. The CO mole fraction is peak-
ing here near the transition from the CO-production branch to
the CO-oxidation branch. Downstream of the quenching height at
the z = +200 and +400 μm locations (Fig. 7, fourth and last col-
umn), both the (CO2 , T ) and (CO,T ) scatter keep on following the
non-adiabatic simulation, while the (CO,T ) in Fig. 7(i) and (j) is
fully on the CO-oxidation branch. At z = +20 0 0 μm distance down-
stream of the quenching height (Fig. 7, included in the last column
with green scatter points), the (CO2 , T ), (CO,T ) and (CO,CO2 ) scatter
plots indicate completed reactions.
From this evolution, a major finding is that upstream of the
quenching location, CO mole fractions are more strongly influenced
by diffusive transport towards the wall than CO2 . This can be ex-
plained by the flame structure. In the reaction zone, CO is formed
first and then followed by its oxidation to CO2 . Compared to CO, up
to approximately z = 200 μm upstream the quenching point, CO2
thus senses the wall less and adiabatic and non-adiabatic (CO2 , T )
correlations coincide up to approximately 750 K. This suggests that
(1) the CO2 is less affected by the quenching process than CO (as
expected) and (2) for premixed near-wall combustion processes
with DME fuel, CO2 is a suitable component of a progress vari-
able composed of different chemical species. The latter applicabil-
ity as progress variable component is facilitated by its monotonic
increase and small gradient over the reaction zone. Furthermore,
it is clearly observed from the (CO,CO2 ) state space in Fig. 7(k)–
(o) that the adiabatic and non-adiabatic behavior (as shown by
the simulation data) are very close to each other across the en-
tire state space. This expected behavior, which is experimentally
confirmed here within the measurement uncertainty, means the
(CO,CO2 ) scatter plot is nearly independent from the wall heat
loss. It is concluded that in the vicinity of the quenching height
(z = 0 μm) and y = 120 μm from the wall, the (CO,CO2 ) correlation
is only influenced marginally by the quenching wall and the influ-
ence is below the experimental uncertainty.
12
Combustion and Flame 235 (2022) 111707
3.3. Thermochemistry progress with wall distance
The evolution of the thermochemical state in the individual
(CO2 , T ), (CO,T ) and (CO,CO2 ) correlations for different wall-normal
y-distances is shown in Fig. 8. Each column presents a differ-
ent wall distance given in the column title. For comparison to
the simulation, adiabatic and non-adiabatic simulations with a
mixture-averaged transport model are presented. Additionally, a
non-adiabatic case with unity Lewis number transport is depicted.
For more detail related to the simulations, see Section 2.4. As
supplement, Fig. 9 summarizes the trend of both the previously
introduced state-space and quenching-point conditioned averages
shown in Fig. 8 with increasing wall distance to enable a direct
comparison (For clarity, only distances y = 120, 320 and 720 μm
are given). For state-space conditioning, the (CO2 , T ) and (CO,CO2 )
scatter view was conditioned by CO2 mole fraction increments
of 0.0025. The (CO,T ) was conditioned by CO mole fraction in-
crements of 0.00125, and the CO-production and CO-oxidation
branches were split and conditioned separately. The state-space
conditioned results are shown with magenta-colored triangles in
Fig. 8 (with only every third marker shown) and in Fig. 9(a)–(c).
This procedure performed well in the past when analyzing (CO,T )
only, but it does not capture the (CO2 , T ) trend approaching com-
pleted reactions. Therefore, this study additionally uses quenching-
based conditioning. As previously demonstrated for the physical
space data in Section 3.2, Fig. 6, the data for each wall distance
y is subdivided into 100 μm wide streamwise z-increments (40
bins ranging from z = −2 to +2 mm) relative to the quenching
height location at z = 0 μm. Quenching-point conditioned averages
of (CO2 ,CO,T ) are calculated for each 100- μm bin in z-direction.
The results are shown with color-coded circles in Fig. 8 (every
marker shown) and in Fig. 9(d)–(f). This procedure is considered
to capture the reaction progress of both CO and CO2 well as it
is directly related to the wall-parallel evolution, i.e., in z-direction,
of the species during reaction. On a first glance it seems that the
quenching-point conditioning procedure underestimates the exper-
imental CO peaks compared to the simulation in Fig. 8(f)–(j), but
as demonstrated in Section 3.2 this does not result from condition-
ing the experimental data but originates from the overall lower ex-
perimental CO peak values in the experiment. Potential reasons for
this deviation are given in Section 3.2. Regarding conditioning, it
is rather noted that state-space conditioning (magenta-colored tri-
angles) leads to increased experimental peak values in the (CO,T ),
as observed in Fig. 8(f)–(i). Despite these values better match to
the simulation, their conditioned average is evidently biased, as
it is exceeding the average experimental CO trace observed in the
physical space in Fig. 6(b). The reason for the biased averages from
state-space conditioning is the separation of oxidation and produc-
tion branch. By separating the data, the mean values are forced
to outlier instead of following the true average. It is concluded
that conditioning in the physical space, i.e., the quenching-point
conditioning, is more robust for filtering errors and the preferred
method.
Major findings from Figs. 8 and 9 are discussed in the following.
Regarding feature (A), it is evident from the (CO2 , T ) thermochem-
istry in Fig. 8(a)–(e) that the non-adiabatic simulation with unity
Lewis number assumption is not capable of capturing the correct
near-wall flame structure prior to quenching. This behavior is not
apparent in the (CO,T ) scatter view in Fig. 8(f)–(j). Thus, it is con-
cluded that (1) differential diffusion effects need to be accounted
for, e.g., by a mixture-averaged transport model for laminar DME
flames; (2) (CO2 , T ) appears to be much more sensitive to differ-
ential diffusion effects than (CO,T ). Consequently, the CO2 aids sig-
nificantly in experimentally identifying the limitation of the unity
Lewis number assumption in FWI.
F. Zentgraf, P. Johe, M. Steinhausen et al. Combustion and Flame 235 (2022) 111707

Fig. 8. Assessment of the thermochemistry evolution for different wall distances. 1565 to 2047 individual samples are shown in each scatter plot. Both experiment and
simulation contain data z = ±2 mm (streamwise direction) relative to the quenching location. Labels (A) to (C) highlight features discussed in the text. (For interpretation of
the references to color in this figure legend, the reader is referred to the web version of this article.)

From feature (B) in Fig. 8(b)–(e) it is apparent that, for increas-
ing wall distances y, the conditioned traces in the (CO2 , T ) state
space develop a trend, moving away from the mixture-averaged
simulation and toward the Le = 1 simulation. This behavior is ex-
clusively observed downstream of the quenching height (z = 0 μm)
when the progress is approaching the fully reacted state. Al-
ready at y = 220 μm wall distance in Fig. 8(b), there is a minor
bend towards the Le = 1 simulation and back to the simulation
with mixture-averaged transport, when the reaction approaches
the equilibrium. This bend is more pronounced for y = 320 μm
wall distance in Fig. 8(c), but the reaction turns back to the sim-
ulation considering differential diffusion effects. For y = 520 and
720 μm wall distance in (d) and (e), the conditioned thermochem-
ical behavior stays on the Le = 1 case after bending. This effect is
also apparent in the (CO,CO2 ) state space in Fig. 8(l)–(o). It is em-
phasized that for y = 120 to 320 μm wall distance in Fig. 8(a)–(c)
and (k)–(m), the post flame values approach the equilibrium state
of the non-adiabatic simulation with mixture-averaged transport
modeling. This behavior is considered physically consistent. Even-
tually this might also be the case for y = 520 and 720 μm distance
in (d), (e) and (n), (o), if additional downstream post-flame data
were available to fully capture the trend toward the fully reacted
state. The observations are different in the (CO,T ) thermochemistry
in Fig. 8(i) and (j). There, for wall normal distances larger than
y = 520 μm, the Le = 1 approximation is obviously not valid for
the conditioned experimental data in the CO-oxidation branch and
the data coincide still better with the mixture-averaged modeling
(see feature (B) in Fig. 8(i)–(j)). However, for higher temperatures
(>1600 K) it is observed that the differential diffusion effects in
(CO,T ) are not fully covered by the applied mixture-averaged mod-
eling. This is not consistent with the observation made for (CO2 , T ).
Error bars of the CO2 mole fraction are included for several spa-
tial bins used for quenching-point conditioning in Fig. 8(e) and (o)
to outline that there is a pronounced experimental uncertainty in
the CO2 mole fractions when approaching chemical equilibrium.
While the quenching-point conditioned average follows the Le = 1
assumption, the lower values of the error bars can reach to the
simulation with mixture-averaged transport. Thus, an interpreta-
tion of the bending from the simulation considering differential
diffusion effects towards the Le = 1 simulation for increasing wall
distances y needs further investigation. One possible explanation
could be the influence of local transport phenomena (also three-
dimensional, as there is a slight curvature of the wall and flame).
However, this does not confirm that the Le = 1 assumption is cor-
rect in these regions. It is rather supposed that a compensation of
different physical effects may lead to the apparent Le = 1 behavior.

13
F. Zentgraf, P. Johe, M. Steinhausen et al.
Fig. 9. Summary of the conditioned averages for the wall distance variation shown in Fig. 8. (a)–(c): state-space conditioning on defined CO as well as CO2 increments;
(d)-(f): quenching-point conditioning. (symbols equal to top row). (For interpretation of the references to color in this figure legend, the reader is referred to the web version
of this article.)
It is strongly suggested that a transport effect occurs, but it is not
conclusively clarified how best to model transport in the present
configuration.
It is furthermore observed in Fig. 8(c)–(e) that the upper lim-
its in the CO2 mole fractions in the experimental scatter data
exceed the simulation results, especially for increased wall dis-
tances (y > 220 μm). According to simulations performed in Can-
tera 2.4.0 [51] (well-stirred reactor at both constant pressure and
temperature, Stagni-mechanism [48]), the equilibrium mole frac-
tions of CO2 should vary between 0.101 and 0.104 (between 300
and 2100 K). Experimental data exceeding the possible equilibrium
value first appears unphysical but could be due to local diffusion
effects that were not covered in the simulation (e.g., 3D effects).
These phenomena need further investigation using advanced diag-
nostics and 3D numerical simulations to gain a deeper insight into
potential transport phenomena.
In Fig. 9(a), (b) and (d), (e) it is evident that the measured
(CO2 , T ) and (CO,T ) thermochemistry develop clear trends with in-
creasing wall distance y. It is furthermore emphasized in Fig. 9 that
for both the (CO2 , T ) and (CO,T ) thermochemistry the trends of
the conditioned averages are located within the boundaries of the
physically possible state space between the non-adiabatic simula-
tion at y = 120 μm wall distance (dotted blue line) and the adi-
abatic simulation (solid red line). This is true for all wall dis-
tances y and independent of the conditioning method. This fact
creates further confidence that the conditioned averages are accu-
rate. This also implies that the trend experimentally observed for
the (CO,CO2 ) correlation is indeed real. Therefore, deviations from
the simulation data (see feature (C) in Fig. 8(n) and (o)) underline
the possible explanation above that there are further relevant ef-
fects that require a 3D examination.
As already mentioned in the discussion of Fig. 7, it is difficult to
derive detailed statements from the (CO,CO2 ) correlation, as adi-
14
Combustion and Flame 235 (2022) 111707
abatic and non-adiabatic simulation are very close to each other
and the experimental data suffers the superimposed uncertainties
in both CO and CO2 . However, it is further emphasized here that
this correlation features least impact on the experimental ther-
mochemistry data with increasing wall distances y. This is out-
lined in Fig. 9(c) and (f) for both the state-space conditioning on
defined CO as well as CO2 increments in (c) and the quenching-
point conditioning in (f). In contrast to the (CO2 , T ) in Fig. 9(a), (d)
and (CO,T ) correlations in (b), (e), the conditioned averages in the
(CO,CO2 ) state space do not possess clear trends with increasing
wall distance but do overlap within their experimental uncertainty
(see transparent colored areas in Fig. 9(c), where the CO error with
respect to CO2 is shown for y = 120 and 720 μm wall distance).
4. Conclusion and outlook
This study has presented the first application of simultaneous
dual-pump CARS, CO-LIF and OH-LIF in a side-wall quenching en-
vironment to simultaneously measure the three scalars CO2 , CO,
and T as close as 120 μm to the surface of the quenching wall
and to determine the instantaneous quenching height. A compre-
hensive and detailed description of the applied methodology was
provided, including a thorough discussion of accuracy and preci-
sion of the diagnostics. The capabilities of the extended laser diag-
nostics for assessing the thermochemistry in side-wall quenching
for one operation condition (DME fuel,  = 0.83, wall 60 ◦ C, lami-
nar) were demonstrated and validated against an adiabatic laminar
flame reference. The nominal wall distances from the experiment
matched very well to the numerical simulation data with a small
offset of 20 μm. Conditioning the thermochemical data with re-
spect to the instantaneous quenching point enabled a novel trac-
ing of the wall parallel chemistry evolution across the quenching
location. The study showed the first comparison of the experimen-
F. Zentgraf, P. Johe, M. Steinhausen et al.
tal three-scalar data against 2D numerical simulations. The major
findings of this study are:
• The novel three-scalar measurement approach considering
(CO2 ,CO,T ) allows highly sensitive probing of the thermochemi-
cal states and is clearly superior to the previously applied two-
scalar measurement approach measuring (CO,T ) only. Simulta-
neously recording relative OH distribution allows correction for
remaining unsteadiness of the quenching height.
• Conditioning the experimental near-wall thermochemistry data
within 100 μm spaced increments derived from the physi-
cal space, so called “quenching-point conditioning”, appeared
superior to previously conditioning in the state space only,
e.g., to avoid ambiguities on the production and oxidation
branches, respectively. Thus, quenching-point conditioning is
recommended for future experimental flame-wall interaction
(FWI) studies.
• The CO2 mole fraction is less affected by the quenching wall
compared to CO and should serve as a more robust compo-
nent of a progress variable definition in near-wall environments
than CO. Especially, the (CO,CO2 ) correlation is only influenced
marginally by the quenching wall and the influence is below
the experimental uncertainty.
• Differential diffusion effects and their importance for CFD
are experimentally proven by comparison to 2D fully-resolved
chemistry and transport (FCT) simulations using a mixture-
averaged transport and unity Lewis number modeling approach.
The (CO2 , T ) correlation is much more sensitive to differential
diffusion effects than the (CO,T ), even though (CO,T ) increas-
ingly showed differential diffusion impact at higher tempera-
tures and larger wall distances that needs to be considered.
Thus, the CO2 aids significantly in experimentally identifying
the limitation of a unity Lewis number assumption. The over-
all agreement between the 2D simulations assuming mixture-
averaged transport and the experimental results is very good.
However, when approaching chemical equilibrium some devia-
tions in (CO2 , T ) and (CO2 ,CO) remained and their origins need
further investigation.
• The experimental methodology proved feasible for laminar op-
eration and yielded valuable, novel insights. This is an im-
portant prerequisite and appears promising for the subsequent
transfer to turbulent cases where the numerical analysis using
direct numerical simulations (DNS) including FCT is limited.
As an outlook, the analysis described in this study will be
expanded to the experimental data measured for different fuels,
equivalence ratios and wall temperatures to gain a deeper under-
standing of the parameter dependency in FWI processes. Especially
the analysis of the turbulent cases appears of major interest, as nu-
merical simulations can get very complex and expensive when ap-
proaching turbulent conditions featuring higher Reynolds numbers.
Furthermore, for a clarification of the supposed transport phenom-
ena, further investigations by advanced diagnostics, like sponta-
neous Raman scattering, to measure more species should be per-
formed as well as 3D numerical simulations for a deeper insight
into potential transport phenomena.
Declaration of Competing Interests
The authors declare that they have no known competing finan-
cial interests or personal relationships that could have appeared to
influence the work reported in this paper.
Acknowledgments
This project is funded by the Deutsche Forschungsgemeinschaft
(DFG, German Research Foundation) Projektnummer 237267381
15
Combustion and Flame 235 (2022) 111707
TRR 150. Robert S. Barlow is grateful for a related DFG Mercator
Fellowship. The generous financial support is gratefully acknowl-
edged. Andreas Dreizler is grateful for support through the Gott-
fried Wilhelm Leibniz program. Calculations for this research were
conducted on the Lichtenberg high performance computer of the
Technical University of Darmstadt.
Supplementary material
Supplementary material associated with this article can be
found, in the online version, at doi:10.1016/j.combustflame.2021.
111707
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