Twenty-Seventh Symposium (International) on Combustion/The Combustion Institute, 1998/pp.

1087–1095

EFFECTS OF TURBULENCE ON SPECIES MASS FRACTIONS IN

METHANE/AIR JET FLAMES

R. S. BARLOW and J. H. FRANK1

Combustion Research Facility
Sandia National Laboratories
Livermore, CA 94551-0969, USA

It is important that combustion models capture the effects of turbulent mixing on reaction zone structure
in non-premixed and partially premixed flames. A more complete understanding of the response of species
mass fractions to turbulent mixing is needed to improve predictive capabilities, particularly with regard to
combustion intermediates and minor species. Using the combination of Raman scattering, Rayleigh scat-
tering, and laser-induced fluorescence, simultaneous measurements of CO, OH, H2, and NO are obtained
along with the major species, temperature, and mixture fraction in a series of six piloted methane/air jet
flames. Flame conditions vary from laminar to turbulent with significant localized extinction. Two-photon
laser-induced fluorescence (TPLIF) is used to determine instantaneous CO concentrations, providing an
improvement over Raman scattering measurements of CO in methane flames. Conditional probability
density functions (cpdf ’s) of species mass fractions in the six flames are compared. Significant changes are
observed in the mass fraction cpdf ’s of several species. Results for H2O, CO2, H2, and OH are consistent
with the concept that turbulent transport becomes dominant over molecular diffusion within the range of
Reynolds numbers and axial locations considered in these experiments. The cpdf ’s of CO mass fraction
are broadened in the turbulent flames relative to the laminar flame. However, there is not an increase in
the maximum conditional mean value of the CO mass fraction as suggested by some previously reported
measurements in methane flames. The cpdf ’s of NO mass fraction at a given streamwise location in the
turbulent flames show NO levels decreasing significantly as jet velocity increases.

Introduction levels with increasing Reynolds numbers in a series

The effects of turbulent mixing on reaction zone
structure in non-premixed and partially premixed
flames have important implications for combustion
models, and a more complete understanding of the
response of species mass fractions is needed, par-
ticularly with regard to combustion intermediates
and minor species. Masri et al. [1] reviewed multi-
scalar experiments on piloted- and bluff-body sta-
bilized flames of various fuels. Several studies of
methane flames reported levels of intermediates that
were higher than predicted by steady laminar flame
calculations or turbulent combustion models. CO
levels measured by Raman scattering in piloted
flames of undiluted methane were significantly
above those calculated in laminar flames [2]. Raman/
Rayleigh measurements in bluff-body flames of
methane reported by Masri et al. [3] and Correa et
al. [4] have also shown CO levels higher than laminar
flame calculations and PDF model predictions. Står-
ner et al. [5] studied piloted flames of dilute methane
and reported elevated levels of OH and H2. Barlow
and Chen [6] reported a progressive increase in OH
1Present address: Physical Sciences, Inc., 20 New En-
gland Business Center, Andover, MA 01810, USA
1087
of piloted methane/air jet flames.
Computational studies have been conducted to in-
vestigate mechanisms that might contribute to the
high measured levels of CO, H2, and OH. Mauß et
al. [7] considered the effects of unsteadiness on lam-
inar flames and suggested that high CO concentra-
tions result from an extinction–reignition process.
Chen and Dibble [8] observed that high CO levels
are also produced in perfectly stirred reactor calcu-
lations. Barlow and Chen [6] used laminar flame cal-
culations to show that unsteadiness and differential
diffusion can influence combustion intermediates.
The present investigation of turbulent methane
flame structure uses part of a comprehensive scalar
and velocity data set on piloted methane/air jet
flames that is described on the World Wide Web [9].
Simultaneous measurements of CO, OH, H2, and
NO were obtained along with the major species,
temperature, and mixture fraction. Two-photon la-
ser-induced fluorescence (TPLIF) was used to de-
termine instantaneous CO concentrations, providing
an improvement over Raman scattering measure-
ments of CO. The influence of turbulence on con-
ditional probability density functions (cpdf ’s) of spe-
cies mass fractions is reported for six jet flames
1088 NON-PREMIXED TURBULENT COMBUSTION

TABLE 1 The concentration of CO was measured by Raman

Relative standard deviations of scalars measured in flat scattering and by two-photon laser-induced fluores-
flames and estimated systematic uncertainties cence (TPLIF). Only the CO TPLIF results are in-
cluded here because they are less affected by inter-
Conditions Systematic ferences and have superior signal-to-noise
Scalar r (rms) (mass frac., T) Uncertainty characteristics. A calibration curve for the CO fluo-
rescence measurements was generated following an
T 1% 2140 Ka 3% approach similar to that for the Raman method. This
YN2 2% 0.73, 2140 Ka 3% curve was based on heater data for dilute CO in N2
YH2O 5% 0.12, 2140 Ka 4% at temperatures up to ;900 K and on rich, premixed
YCO2 6% 0.14, 2140 Ka 4% CH4/air flat flame measurements (;1900 K to
YH2 17% 0.003, 2020 Kb 6–12% ;2200 K). The shape of the polynomial through the
YOH 8% 0.0016, 2140 Ka 10% interpolated region was constructed to match ap-
YCO 6% 0.062, 2020 Kb 10–20% proximately the temperature dependence of a Boltz-
YNO 10% 8 ppm, 1760 Kc 10–15% mann fraction calculation (provided by M. Di Rosa,
Sandia). Further description of the CO TPLIF
aPremixed CH /air, f 4 0.96, uncooled (Hencken) method and comparisons of simultaneous CO mea-
4
burner. surements by Raman scattering and TPLIF are re-
bPremixed CH /air, f 4 1.27, uncooled (Hencken) ported elsewhere [13,14].
4
burner. We note here that comparison of measurements
cPremixed CH /O /N , f 4 0.72, cooled (McKenna) in lean and near-stoichiometric methane/air calibra-
4 2 2
burner. tion flames reveals a small but repeatable offset of
roughly 1 2 1015 mol/L in the TPLIF result above
the Raman result. This may be due to photodisso-
having fixed nozzle diameter and increasing jet ve- ciation of vibrationally excited CO2 at flame tem-
locities, corresponding to jet Reynolds numbers peratures [15]. It is not a significant effect for this
from 1,100 (laminar) to 44,800 (turbulent with sig- paper, because the cpdf ’s are for a mixture fractions
nificant localized extinction). Results suggest a interval where the Raman and TPLIF calibrations
strong influence of scalar transport on major and mi- have been matched. However, interference from
nor species. CO2 may be an important consideration for experi-
ments in lean premixed combustion, where lower
CO concentrations must be measured accurately
Experimental Methods
and direct calibration may be difficult.
Most aspects of the flow facility, diagnostic sys- Experimental uncertainties are summarized in Ta-
tems, and calibration procedures have been de- ble 1. Standard deviations of species mass fractions
scribed previously [10,11]. Spontaneous Raman in the calibration flames may be used to estimate
scattering of the beams from two Nd:YAG lasers contributions of photon shot noise and instrument
(532 nm) was used to measure concentrations of the noise to the widths of the cpdf ’s. Estimates of sys-
major species. The Rayleigh scattering signal was tematic uncertainties are based on analysis of the
converted to temperature using a species-weighted calibration methods, repeatability of calibrations,
scattering cross section, based on the Raman mea- considerations of calibration drift, and allowances for
surements. Linear laser-induced fluorescence (LIF) the interpolated calibration curves for CO and H2.
was used to measure OH and NO, and the fluores- With regard to comparison of cpdf ’s, the relative un-
cence signals were corrected on a shot-to-shot basis certainty (not including statistical noise or potential
for variations in Boltzmann fraction and collisional effects of spatial averaging) within each set of mea-
quenching rate. The spatial resolution was roughly surements in the five turbulent flames is estimated
0.75 mm. to be within 52% for the Raman measurements,
Temperature-dependent calibration functions for 55% for OH, 55% for CO, and 510% for NO.
each of the Raman channels were determined from The piloted burner [1] had a main jet diameter of
a series of measurements in flows above an electric d 4 7.2 mm and a pilot diameter of 18.2 mm. The
heater and a flat flame (Hencken) burner. OH mea- jet composition was 25% CH4 and 75% air, by vol-
surements were referenced to a premixed CH4/air ume, which produced a shorter, more robust flame
flat flame, in which the OH number density had than pure methane [1,5] with lower levels of inter-
been measured previously by laser absorption. The ference. The annular pilot burned a mixture of
NO calibration factor was determined by doping a C2H2, H2, air, CO2, and N2 having the same enthalpy
lean premixed CH4/O2/N2 laminar flat flame (Mc- and equilibrium composition as methane/air at 0.77
Kenna burner) with known concentrations of NO. equivalence ratio. A lean pilot was used to reduce
Flame calculations have shown that destruction of the flux of minor species from the pilot. One profile
the seeded NO in this flame is negligible [10,12]. (Flame D, x/d 4 15) was repeated with the pilot
 TURBULENT METHANE/AIR JET FLAMES 1089

TABLE 2
Flow parameters

Ujet—cold Upilot—burnt Ucoflow

Flame Rejet (m/s) (m/s) (m/s)

A ;1100 2.44 none 0.9

B ;8200 18.2 6.8 0.9
C ;13400 29.7 6.8 0.9
D ;22400 49.6 11.4 0.9
E ;33600 74.4 17.1 0.9
F ;44800 99.2 22.8 0.9

Fig. 2. Scatter plots of measured temperature at x/d 4

5 in the laminar Flame A and at x/d 4 30 in the turbulent
Flames B–F. All 3000–5000 samples from each flame are
included. The line shows results of a strained, opposed-
flow laminar flame calculation with a strain parameter of a
4 50 s11 and is included as a visual guide.

affect flame structure, and the flame behaves as a

Fig. 1. Scatter plots of measured temperature at x/d 4
5 in the laminar Flame A and at x/d 4 15 in the turbulent
Flames B–F. All 3000–5000 samples from each flame are
included, and in Flame A the clusters of points from sepa-
rate locations are apparent. The line shows results of a
strained, opposed-flow laminar flame calculation with a
strain parameter of a 4 50 s11 and is included as a visual
guide.
flow rate reduced by 40% to assess the influence of
the pilot on minor species concentrations, and there
was no significant change in the cpdf ’s.
Results and Discussions
Flame Characteristics
Measurements were obtained in six flames, as
listed in Table 2. At these flow conditions the fuel-
rich premixed chemistry is too slow to significantly
diffusion flame, with a single reaction zone near the
stoichiometric mixture fraction of fs 4 0.351 [5,16].
Profiles were measured at x/d 4 5 and x/d 4 10 in
the laminar flame and at x/d4 15 and x/d 4 30 in
the five turbulent flames. To minimize errors due to
calibration drift, the flames were measured out of
order, wind-tunnel air measurements were acquired
before and after each profile, and the first profile was
repeated at the end of the series. A total of 3000–
5000 samples was collected at four to six radial lo-
cations (more in the laminar case) within each flame
at each streamwise station.
Scatter plots of temperature versus mixture frac-
tion are shown in Figs. 1 and 2. The calculated tem-
perature curve for an opposed-flow laminar flame
with a strain parameter of 50 s11 is included to fa-
cilitate visual comparisons. These scatter plots pro-
vide a qualitative indication of the probability of local
extinction, which is characterized by samples with
strongly depressed temperatures. At x/d 4 15 (Fig.
1) there is no evidence of extinction in Flame B.
Flames C and D have very small probability of local
extinction, and extinction becomes more important
in Flames E and F. At x/d 4 30 (Fig. 2), the scatter
plots for Flames C, D, and E all show low probability
1090 NON-PREMIXED TURBULENT COMBUSTION
Fig. 3. Measured conditional means of temperature and
the mass fractions of CO2, H2O, CO, OH, NO, and H2 in
Flame B at x/d 4 15 (symbols). Lines show results of a
strained, opposed-flow laminar flame calculation with a
strain parameter of a 4 100 s11. This calculation includes
full transport. The mixture fraction intervals used in form-
ing the cpdf’s are indicated for each species.
of extinguished samples, indicating a healthy reig-
nition process. In contrast, Flame F still has high
probability of local extinction at x/d 4 30, and the
characteristic bimodality of the temperature distri-
bution in lean and near-stoichiometric samples [1] is
evident.
The rms fluctuation in temperature near the stoi-
chiometric mixture fraction in the laminar flame is
40–45 K, which is greater than the 20–25 K mea-
sured in the calibration flames. This is attributed to
small variations in the location of the reaction zone,
which do not significantly add to the relative fluc-
tuations in species mass fractions.
Conditional Probability Density Functions
In this section, cpdf ’s of the mass fractions of H2O,
CO2, CO, OH, H2, and NO in the six flames are
compared. For each species, the cpdf is formed from
samples within a mixture fraction interval corre-
sponding to the peak mass fractions of that species.
These intervals are shown in Fig. 3, which includes
conditional means of measured scalars at x/d 4 15
in Flame B. The location of the peaks can change
slightly in these flames. However, small changes in
position or width of the mixture fraction intervals do
not significantly alter the cpdf ’s or conclusions re-
ported here.
There is not sufficient information on scalar gra-
dients in the present flames to quantify the effects
of spatial averaging on the cpdf ’s. However, we note
that the cpdf ’s are determined for mixture fraction
intervals corresponding to peak conditional-mean
mass fractions. Thus, spatial averaging across react-
ing samples would tend to reduce the apparent mass
fractions. We find that the cpdf ’s of several species
shifted toward higher mass fractions with increasing
jet velocity, suggesting that spatial averaging does
not have a strong influence on the present results.
The mixture fraction was calculated following the
method of Bilger et al. [18], but with oxygen ex-
cluded from the expression:
2(YC 1 YC,2)/wC ` (YH 1 YH,2)/2wH
f4
2(YC,1 1 YC,2)/wC ` (YH,1 1 YH,2)/2wH
Here, Y’s are elemental mass fractions, w’s are
atomic weights, and subscripts 1 and 2 refer to the
main jet and coflowing air stream, respectively. The
partial premixing of fuel and air leads to boundary
conditions for YO that are relatively close, causing
excessive noise in the mixture fraction if oxygen is
included in the calculation.
Figure 4 includes cpdf ’s from x/d 4 5 and x/d 4
10 in Flame A and from x/d 4 15 in Flames B
through F. The latter location corresponds to the
“neck” region of the turbulent flames, where local
extinction is most probable in the highly strained
cases. The cpdf ’s of YH2O in the turbulent flames
align with those in the laminar jet flame, and the
progression with increasing Reynolds number in-
volves an increase in the population of extinguished
samples without a significant change in YH2O for re-
acted samples. In contrast, the cpdf of YCO2 shows a
progressive decrease in the most probable value of
YCO2. The cpdf of YOH shows a trend similar to that
reported in Ref. [6]. As the Reynolds number in-
creases, the curves broaden and shift toward higher
mass fractions. This trend is clearly present before
local extinction becomes important, and it cannot be
attributed to reignition.
For CO, the main effect of increased turbulence
is a broadening of cpdf ’s relative to Flame A. This
broadening is mainly in the direction of lower mass
fractions, but the trend is less obvious than for OH.
At x/d 4 15 in the turbulent flames, the cpdf ’s of
YH2 display a nonmonotonic response to increasing
Reynolds number. The curve for Flame B is similar
to that from Flame A. YH2 tends to be higher in
Flame C but decreases significantly in Flames E and
F. The cpdf ’s of YNO show mass fractions decreasing
as the Reynolds number increases, and this may be
primarily an effect of residence time.
Figure 5 includes the cpdf ’s from x/d 4 30, which
is roughly two-thirds the Favre-average stoichiomet-
ric flame length (Ls 4 47d) for the turbulent cases.
Here, cpdf ’s of YH2O in Flames B through E are
 TURBULENT METHANE/AIR JET FLAMES 1091

Fig. 4. Conditional pdf’s of the measured mass fractions of H2O, CO2, OH, CO, H2, and NO from x/d 4 5 (A5) and
x/d 4 10 (A10) in the laminar jet flame and from x/d 4 15 in the turbulent flames B–F. Mixture fraction intervals used
in forming the cpdf’s are given in each graph.

nearly identical, with the most probable values of
YH2O being about 10% higher than in Flame A. The
cpdf for Flame F is bimodal, but the portion cor-
responding to reacted samples aligns with the other
turbulent flames. The cpdf ’s of YCO2 in Flames B–E
show a most probable mass fraction about 10% lower
than in Flame A. These differences in major species
are believed to reflect the increasing importance of
turbulent transport relative to molecular diffusion as
Reynolds number and streamwise distance are in-
creased [19]. A similar effect on YH2O and YCO2 is
observed in strained laminar flame calculations [17]
when all diffusivities are set equal to the thermal
diffusivity. This transport effect is also believed to
explain, at least in part, the distinct shift to higher
mass fractions that is seen in the cpdf ’s of YH2 at x/
d 4 30. A comparison of laminar flame calculations
at the same strain rate (a 4 100 s11) shows the peak
mass fraction increasing by ;10% for H2O, decreas-
ing by ;9% for CO2, and increasing by ;60% for
H2 when equal diffusivities are specified instead of
the normal CHEMKIN treatment of transport prop-
erties.
The cpdf ’s of YOH at x/d 4 30 in Flames B–F
continue to show higher mass fractions than in
Flame A. This may also be related to transport ef-
fects, because the specification of equal diffusivities
in the a 4 100 s11 laminar flame calculation causes
1092 NON-PREMIXED TURBULENT COMBUSTION

Fig. 5. Conditional pdf’s of the measured mass fractions of H2O, CO2, OH, CO, H2, and NO from x/d 4 5 (A5) and
x/d 4 10 (A10) in the laminar jet flame and from x/d 4 30 in the turbulent flames B–F. Mixture fraction intervals used
in forming the cpdf’s are given in each graph.

a 25% increase in peak YOH. However, interpretation
is complicated by the fact that the most probable
values of YOH in the cpdf ’s for Flame A are lower
than predicted for full-transport laminar flames. It is
possible that radiative loss and the convective history
of radical recombination contribute to the observed
reduction in OH levels relative to the adiabatic op-
posed-flow calculation. The cpdf ’s of CO in Flames
B–E are broader than in Flame A but are centered
at roughly the same mass fraction. The results for
YNO in the turbulent flames show decreasing mass
fractions with increasing Reynolds numbers. Resi-
dence time may be the main effect here. However,
it is difficult to discern the relative importance of
convective residence time, local scalar dissipation,
transport effects, and various branches of the NO
production and reburn chemistry. The prediction of
these NO results will be an interesting challenge for
combustion models.
Returning to the results at x/d 4 15 (Fig. 4), the
response of the cpdf ’s of all species to increasing
Reynolds numbers appears to be consistent with the
combined (and sometimes offsetting) effects of in-
creases in scalar dissipation and increases in the rela-
tive importance of turbulent transport. Laminar
flame calculations show that the peak mass fractions
of H2O, CO2, H2, and NO decrease with increasing
scalar dissipation or strain rate, whereas the peak
values of CO and OH are relatively insensitive to
strain rate. When diffusivities are set equal in the
 TURBULENT METHANE/AIR JET FLAMES
laminar calculations (the analog of turbulent trans-
port being dominant), the peak mass fractions of
OH, H2, and NO increase significantly, whereas
those of H2O and CO increase modestly, and that of
CO2 decreases. For CO2, the effects of increased
turbulent transport and increased scalar dissipation
are additive, contributing to the progression ob-
served in Fig. 4. At x/d 4 15 these effects tend to
offset each other for H2O, H2, and CO. Unsteadi-
ness may also contribute to the measured trends, but
computational studies [6,7] have required unusual
scenarios of unsteady strain to produce significant
changes in species mass fractions.
Conclusions
These experiments provide a detailed character-
ization of the effects of turbulence on species mass
fractions in piloted methane jet flames. Results show
significant changes in the cpdf ’s of some species as
the jet Reynolds number is increased from the lam-
inar regime through a series of turbulent flames. The
following conclusions are drawn:
1. Conditional pdf’s of OH show a distinct broad-
ening and shift toward higher mass fractions as
the Reynolds number is increased. This trend is
consistent with previous experiments in similar
flames.
2. Results for H2O, CO2, H2, and OH all appear to
reflect a shift in importance from molecular dif-
fusion to turbulent transport within the range of
flow conditions and streamwise locations consid-
ered.
3. Mass fractions of CO in the turbulent flames are
not significantly higher than those measured in a
laminar jet flame. Rather, YCO in the highly
strained neck region of the piloted turbulent
flames (x/d 4 15) tends to be lower than in the
laminar jet flame.
4. NO mass fractions tend to decrease with increas-
ing Reynolds numbers. However, it is difficult to
discern the relative importance of local scalar dis-
sipation, convective residence time, transport ef-
fects, and the various branches of the NO pro-
duction and reburn chemistry in establishing this
measured trend.
Acknowledgments
This research was supported by the United States De-
partment of Energy, Office of Basic Energy Sciences. The
contributions of G. Fiechtner and C. Carter to the devel-
opment of the CO LIF system are gratefully acknowl-
edged.
1093
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1. Masri, A. R., Dibble, R. W., and Barlow, R. S., Prog.
Energy Combust. Sci. 22:307–362 (1996).
2. Chen, J.-Y., Kollmann, W., and Dibble, R. W., Com-
bust. Sci. Technol. 64:315–346 (1989).
3. Masri, A. R., Dibble, R. W., and Barlow, R. S., in
Twenty-Fourth Symposium (International) on Com-
bustion, The Combustion Institute, Pittsburgh, 1992,
pp. 317–324.
4. Correa, S. M., Gulati, A., and Pope, S. B., in Twenty-
Fifth Symposium (International) on Combustion, The
Combustion Institute, Pittsburgh, 1994, pp. 1167–
1173.
5. Stårner, S. H., Bilger, R. W., Dibble, R. W., and Bar-
low, R. S., Combust. Sci. Technol. 70:111–133 (1990);
Combust. Sci. Technol. 72:255–269 (1990).
6. Barlow, R. S. and Chen, J.-Y., in Twenty-Fourth Sym-
posium (International) on Combustion, The Combus-
tion Institute, Pittsburgh, 1992, pp. 231–237.
7. Mauß, F., Keller, D., and Peters, N., in Twenty-Third
Symposium (International) on Combustion, The Com-
bustion Institute, Pittsburgh, 1990, pp. 693–698.
8. Chen, J.-Y. and Dibble, R. W., Combust. Sci. Technol.
84:45–50 (1991).
9. www.ca.sandia.gov/tdf/Workshop.html.
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G. J., and Barlow, R. S., Combust. Flame 105:499–510
(1996).
11. Barlow, R S., Fiechtner, G. J., and Chen, J.-Y., in
Twenty-Sixth Symposium (International) on Combus-
tion, The Combustion Institute, Pittsburgh, 1996, pp.
2199–2205.
12. Reisel, J. R., Carter, C. D., and Laurendeau, N. M.,
Combust. Sci. Technol. 91:271–295 (1993).
13. Frank, J. H. and Barlow, R. S., in Twenty-Seventh
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bustion Institute, Pittsburgh, 1998, pp. 759–766.
14. Barlow, R. S., Frank, J. H., and Fiechtner, G. J., “Com-
parison of CO Measurements by Raman Scattering
and Two-Photon LIF in Laminar and Turbulent Meth-
ane Flames,” paper WSS/CI 98S-19 (1998).
15. Nefedov, A. P., Sinel’shchikov, V. A., Usachev, A. D.,
and Zobnin, A. V., Appl. Opt., in press.
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Brown, T. M., and Pitz, R. W., in Twenty-Sixth Sym-
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tion Institute, Pittsburgh, PA, 1996, pp. 1121–1128.
17. Chen, J.-Y., personal communication of results of op-
posed-flow laminar flame calculations using the Sandia
code and the Miller-Bowman (1989) mechanism, with
boundary conditions matching the present jet and cof-
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18. Bilger, R. W., Stårner, S. H., and Kee, R. J., Combust.
Flame 80:135–149 (1990).
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(1995).
1094 NON-PREMIXED TURBULENT COMBUSTION
COMMENTS
George Kosàly, University of Washington, USA. It ap-
pears to me that the effects you are showing can be some-
what better understood via the Damköhler number than
via the Reynolds number.
Author’s Reply. It is correct that several trends in the
data can be best explained in terms of an appropriately
defined Damköhler number. The increasing probability of
localized extinction in this series of flames, as shown in
Figs. 1 and 2, is an obvious example of the turbulent mixing
rates becoming too fast for the chemical reaction rates (de-
creasing Damköhler number). The trends in NO mass frac-
tion are believed to be mainly influenced by the ratio of
the thermal NO formation time scale to the convective res-
idence time in each flame, which is also a Damköhler num-
ber effect. The decrease in OH mass fraction between x/d
4 5 and x/d 4 10 in the laminar flame A may be correlated
with a Damköhler number formed from the time scale of
the three-body radical recombination reactions and the
convective time between these measurement locations. A
difficulty in describing these effects is that there is not a
unique definition of the Damköhler number that can be
associated with all the different trends in the experiment.
The Reynolds number is used in this paper partly as a con-
venience because it may be defined simply, and the extra
words required to define multiple flow and chemical time
scales are avoided. However, the main conclusion of this
paper is that the evolution in the relative importance of
turbulent transport vs. molecular diffusion is of central im-
portance in understanding the measured trends in the con-
ditional PDFs of species mass fractions. This evolution is
most appropriately described in terms of Reynolds number
rather than Damköhler number. The cold jet exit Reynolds
number may be less appropriate than a local turbulence
Reynolds number or some other definition, but it is used
here for simplicity.
● Second, the measurement uncertainty in mixture fraction
Normand M. Laurendeau, Purdue University, USA. Be-
cause the effective probe volume would be smaller for CO,
might this explain the good agreement between your CO
measurements and laminar flame predictions near the peak
of your CO vs. mixture fraction plot as compared to other
such plots that you report? In particular, for the OH and
NO mixture-fraction plots, how much of the observed de-
pression at the peak might be related to probe effects?
Author’s Reply. The experimental data in Fig. 3 that you
refer to are from flame B, which has a relatively low Reyn-
olds number and might best be described as having an un-
steady laminar reaction zone. Consequently, the reaction
zone is typically not far from being normal to the laser
beams. While the beam diameter for CO LIF is smaller
than for the other measurements, the imaged length of the
probe volume along the axis of the beams is the same for
all measurements (roughly 0.75 mm). Therefore, the ef-
fective spatial resolution is about the same for all measure-
ments in flame B. The laminar flame calculation at a 4
100 s11 in Fig. 3 was selected because it yielded reasonably
good agreement with the measured temperature and major
species. These calculated curves are plotted mainly as vi-
sual aids to help show the widths of the peaks relative to
the mixture fraction intervals used for the conditional
PDFs for each species. The very close agreement on CO
is gratifying but should not be assigned significance beyond
the fact that agreement is within the estimated experimen-
tal uncertainty. The close agreement near the NO peak is
fortuitous. OH and NO have the narrowest peaks in the
mixture-fraction plots and are the most likely species to
suffer from spatial averaging effects. However, such effects
are difficult to estimate in flames B–F without information
on instantaneous scalar gradients. As noted in the paper,
the CPDFs for YH2O, YH2, and YOH show increasing mass
fractions with increasing jet velocity, which is opposite to
the trend one would expect if spatial averaging was signifi-
cant. There is some spatial averaging in these measure-
ments, but the qualitative conclusions of this paper do not
appear to be sensitive to this potential source of error.
●
Mohy S. Mansour, Cairo University, Egypt. The scatter
plots in flames D, E, and F show different trends at the
lean and rich side of the reaction zone. How do you explain
these differences? Does mixing play an important role at
the lean side while extinction is more dominant at the rich
side?
Author’s Reply. Two experimental details should be con-
sider when interpreting scatter plots in Figs. 1 and 2. First,
the data are from 4 or 5 radial locations in each flame, and
the PDF of mixture fraction may be different for each
flame. This can have some influence on visual impressions.
is roughly 4 B15% of the local value (standard deviation),
and this causes the apparent spreading or blooming of the
scatter plots on the rich side even when there is no extinc-
tion. Beyond these experimental artifacts, there is a clear
trend that temperature samples on the rich side drop pro-
gressively below the calculated laminar flame curve as the
jet velocity is increased for flames D, E, and F. This trend
is apparent at both streamwise locations, and it is believed
to result from the extinction/mixing/reignition process that
becomes progressively more important in these flames.
When there is localized extinction, some mixing occurs
with little or no reaction, and fluid elements move from
being close to the fully reacted envelope toward the inte-
rior of the temperature vs. mixture fraction domain.
Information on the original fuel-side boundary condition
becomes lost in this process. When reaction is re-estab-
lished near the stoichiometric mixture fraction, these
mixed interior elements become the boundary conditions
 TURBULENT METHANE/AIR JET FLAMES 1095

for the reacting layer. This phenomenon must also affect
the lean side, and there is some indication of this in the
scatter plots for flame F. However, on the lean side, the
coflowing air provides an ever-present source of fluid at the
original air-side conditions, so one still finds samples near
the trajectory marked by the laminar flame calculation. Ex-
tinction and reignition are relevant near the stoichiometric
condition, while mixing is active on both rich and lean
sides. It is the constraints on the mixing process that lead
to the foregoing trend in the scatter plots.