Fuel 358 (2024) 130201

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Fuel
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Spectroscopic investigation of diesel-piloted ammonia spray combustion

Valentin Scharl ∗, Thomas Sattelmayer
Chair of Thermodynamics, Technical University of Munich, Boltzmannstraße 15, 85748 Garching, Germany

ARTICLE INFO ABSTRACT

MSC: This work investigates the flame emissions of diesel-piloted ammonia spray combustion under conditions
00-01 relevant to internal combustion engines. Due to ammonia’s carbon-free structure, its flame emissions differ
99-00 significantly from carbon-containing fuels. This work provides new insights into the combustion process by
Keywords: distinguishing pilot and main fuel combustion by analyzing spectrally resolved flame emission footprints
Ammonia between 275 nm and 750 nm in a rapid compression expansion machine (RCEM). Additional results based
Chemiluminescence on Shadowgraphy (SG), OH*-chemiluminescence (CL), visible natural flame luminosity (NL) imaging, and
Direct-injection
heat release rate (HRR) analysis describe the combustion process in detail. OH*, NH*, NH2 *, as well as
Combustion
broadband CL from NH2 *, NO2 *, and H2 O* contribute to ammonia flame luminosity. The results show that the
Spectroscopy
Dual-fuel combustion process encompasses a pilot ignition phase, a flame transition phase, and an ammonia combustion
phase, during which only ammonia-related flame emissions occur and the main share of heat is released.
Background corrected OH*, NH*, and NH2 * intensities reveal the evolution of individual contributions to the
flame emissions. NH2 *-CL is the main contributor to visible ammonia flame emissions under the conditions
investigated. Therefore, visible flame emissions are a suitable indicator for the flame front during the ammonia
combustion phase.

1. Introduction production by renewable power plants. Among the dual-fuel concepts,

With the background of climate change, ammonia is of interest
as an alternative to fossil fuels. Due to its carbon-free structure, it
offers the potential to reduce greenhouse gas emissions significantly.
Easier storage and higher energy densities provide an advantage for
transportation or mobile applications compared to hydrogen. A possible
option to convert the energy stored in ammonia is using internal com-
bustion engines, which offer a robust and cost-effective way of energy
conversion. Therefore, internal combustion engines could be part of
future energy systems [1]. However, as the combustion characteristics,
physical properties, and chemical reaction pathways differ immensely
from carbon-based fuels, research is necessary to develop internal
combustion engines suitable for using ammonia. As ammonia has a
high auto-ignition temperature, slow laminar burning velocities, high
enthalpy of evaporation and narrow flammability limits, measures to
improve its combustion behavior are commonly used [2]. These include
hydrogen addition [2], ammonia dissociation prior to combustion [3]
and the use of pilot fuel [4]. Furthermore, pure, spark-ignited ammonia
combustion is feasible if compression ratios and fuel preheating are
sufficiently high [4]. Dual-fuel concepts that use conventional fuel
as pilot may also run on the conventional fuel only. This option
decreases the exposure of engine operators to the risk of fluctuating
ammonia availability, e.g., caused by seasonal variability of power
the high-pressure dual-fuel (HPDF) combustion, where both fuels are
injected close to top dead center (TDC), offers the potential to reduce
unburned fuel emissions caused by wall-quenching effects and valve
timing overlap. For this combustion process, the primary fuel burns
mainly diffusively, similar to diesel engines. Comprehensive reviews of
ammonia combustion in ICEs can be found in [5] and [6].
Imaging of the natural flame luminosity (NL) is used in experimental
combustion research to infer important features of combustion pro-
cesses, such as flame front location, ignition time and location, or heat
release rate (HRR) distribution [7,8]. Most investigations target specific
wavelength ranges using bandpass-filtered 2-D imaging techniques.
Therefore, interference between the chemiluminescence (CL) of several
excited species emitting in the investigated band or with other sources
of luminosity, such as soot, distorts the information obtained. For exam-
ple, under high-temperature conditions, OH*-CL is known to interfere
with soot radiation [9,10]. Under low-temperature combustion condi-
tions, OH*-CL interferes with CO2 * and HCO* broadband CL [11,12].
By dispersing flame emissions based on their wavelengths, spectro-
scopic investigations can help distinguish flame emissions’ source. A
detailed overview of the chemiluminescent species present in various
flames is given in [13]

∗ Corresponding author.
E-mail addresses: valentin.scharl@tum.de (V. Scharl), sattelmayer@td.mw.tum.de (T. Sattelmayer).

https://doi.org/10.1016/j.fuel.2023.130201
Received 24 July 2023; Received in revised form 30 September 2023; Accepted 26 October 2023
Available online 3 November 2023
0016-2361/© 2023 The Author(s). Published by Elsevier Ltd. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).
V. Scharl and T. Sattelmayer Fuel 358 (2024) 130201

The chemiluminescent signature of flames generally depends Table 1

strongly on the fuel used, combustion temperatures and pressures, RCEM specifications and operating parameters. The timings in CAD refer to OP4 at
1000 rpm.
equivalence ratios, and strain rates. Only a few studies investigated
Operating point OP3 OP4
the flame luminosity under engine-relevant temperatures and pressures
for ammonia. Wang et al. [14] used visible flame luminosity to study TDC temperature [K] 865 ± 10 920 ± 10
TDC pressure [bar] 98 ± 2 125 ± 2
pure ammonia spray combustion. They observed a transparent-like,
Effective compression ratio [−] 17.2 20.5
orange-red flame with less intense luminosity than sooting diesel flames 1
Equivalent engine rpm [ min ] ≈920 ≈1000
under similar conditions. Wüthrich et al. [15] used simultaneously Bore diameter [mm] 220
acquired Schlieren and OH*-CL imaging to analyze the combustion of Maximum Stroke [mm] 368.9
homogeneous ammonia mixtures ignited by diesel pilots (low-pressure Fuel injection temperature [K] 293 ± 3
dual-fuel combustion), which allowed a detailed description of pilot Diesel injection duration [μs∕CAD] 520∕1.56
fuel ignition, as well as flame transition to the premixed ammonia Start of diesel injection [μs∕CAD btdc] 2000 ± 50∕6 ± 0.15
charge and subsequent flame propagation. The authors of the study Diesel nozzle diameter [μm] 200
Diesel injection pressure [bar] 2000 ± 20
at hand carried out OH*-CL investigations of ammonia combustion
Injected diesel mass [mg] 5
to analyze the combustion of diesel-piloted ammonia sprays (HPDF
Ammonia injection duration [μs∕CAD] 2700∕8.1
combustion) in a rapid compression expansion machine (RCEM). We
Relative ammonia injection timing [μs∕CAD] +500∕1.5
found the OH*-radiation intensity of the burning ammonia spray to Diameter [μm] 940
be more than an order of magnitude lower than the OH* intensity Injection pressure [bar] 503 ± 10 530 ± 10
emitted by the diesel pilot combustion, although diesel only accounted Ammonia mass [mg] 210
for 5% of the LHV supplied [16,17]. Spectroscopic measurements
of premixed mixtures containing ammonia have been carried out at
atmospheric pressures for CH4 /NH3 /air mixtures by Zhu et al. [18]
and for CH4 /NH3 /H2 /air by Mashruk et al. [19]. The studies detected 2.1. Test rig
NO*, OH*, NH*, CN*, CH*, NH2 * peaks, as well as CO2 *, H2 O* and
NO2 * broadband radiation. A strong reduction in the intensity of all The investigations are conducted in a pneumatically driven RCEM,
peaks (including NH*) except NH2 * was found for increasing ammonia which is optically accessible via a quartz-glass piston. The machine
shares. While the behavior of CH* and CN* can be explained by the simulates single cycles of large-bore engines. Essential specifications
reduced availability of carbon atoms, the decline of NH*-CL intensity and operating parameters are listed in Table 1, and a scheme of the
was attributed to the reduced OH* concentration in ammonia flames, as RCEM driving mechanism, the cylinder head, and the spectroscopy
NH* is mainly produced via the reaction NH2 + OH → NH + H2 O [19]. setup is shown in Fig. 1. This section only outlines the main features of
Under engine-relevant conditions, Ichikawa et al. [20] reported the the RCEM, while a more detailed description can be found in [24].
flame emission profiles obtained from stratified spray injection of Before each experiment, the driving-air bottles are filled with pres-
ammonia and n-hexadecane through a single nozzle. By detecting the surized air. After starting the experiment, the outer piston, which is
NH2 * peaks, they corroborated that the supporting fuel successfully hydraulically coupled to the inner piston, accelerates. As a result, the
induced ammonia combustion. inner working piston accelerates in the opposite direction, which can-
For HPDF combustion, pilot/supporting fuel and ammonia are not cels net momentum and reduces unwanted vibrations. The compression
mixed prior to combustion, which differs from the spectroscopy inves- stroke ends at TDC when a dynamic equilibrium is reached, and the
tigations discussed above. Instead, the two fuel sprays interact within expansion stroke starts. The piston trajectory is determined by driving
the combustion chamber. This interaction is a major influencing factor pressure, flow resistance, and combustion chamber pressure. For the
on the performance of the combustion process [21]. HPDF combustion conditions investigated in this work, the piston motion resembles the
relies on the favorable auto-ignition properties of the pilot fuel, whose motion induced by a crankshaft at 920 or 1000 rpm, depending on the
ignition may fail or be delayed when the mixture formation process operating point. The combustion chamber pressure is measured during
deteriorates by interaction with the less reactive primary fuel [22,23]. the experiment using a Kistler 7061C piezo-electric pressure transducer.
When using ammonia as the main fuel, the unique CL features of the An inductive linear incremental encoder measures the piston position.
ammonia flame (e.g., NH*, NH2 * emissions) may allow us to distinguish Temperature is only measured before the experiment via a thermo-
between the combustion of pilot fuel and ammonia. couple. During the experiment, the temperature is calculated under
This work aims to characterize the natural flame emissions of the assumption of an undisturbed gas core that undergoes isentropic
diesel-piloted ammonia HPDF combustion using spectrally resolved compression. This assumption is valid when flat pistons and large
high-speed CL measurements. The data obtained may serve as a basis on crevice volumes prevent charge motion and roll-up of the boundary
which wavelength ranges to choose for investigating ammonia combus-
layer [25], as in the RCEM employed. Deviations in driving pressure,
tion optically and help interpret the observed luminosity. Furthermore,
initial chamber pressure, and oil temperature lead to deviations in the
we try to take advantage of unique flame emissions of ammonia (NH*,
chamber pressure obtained at TDC. This deviation also causes different
NH2 *) to characterize the flame transition process from pilot to primary
TDC temperatures according to the relations for isentropic compression.
fuel. The work is structured as follows: First, the test rig and the
The deviation in temperature due to different compression ratios is
optical measurement system employed are presented. Then, temporally
superimposed by changes in initial chamber temperature. Furthermore,
and spatially integrated spectra are discussed to reveal which species
the ammonia injector opening timing deviates slightly between indi-
contribute significantly to the observable natural flame emissions. Sub-
vidual experiments, as can be extracted from optical imaging data. In
sequently, time-resolved flame spectra are discussed in context with SG,
OH*-CL, and NL images to characterize the combustion process with a addition, the accuracy with which the injection pressures can be set is
focus on flame transition. Furthermore, NH*, OH*, NH2 *, and broad- limited. Table 1 provides typical ranges of the quantities discussed.
band luminosity intensity evolutions are extracted from the spectra and The thermodynamic model also assumes this isentropic core to
discussed in context to the HRR. The work concludes with a summary calculate HRRs based on chamber pressure and piston position. The
and recommendations regarding future optical investigations. multi-zone model assumes heat loss to occur only in representative
piston crevices. Heat loss model parameters are calibrated using unfired
2. Experimental setup and methods experiments. Therefore, the HRRs presented in this work include the
heat sink due to evaporation of the fuels and effects due to species
This section briefly describes the test rig used, the optical methods conversion. Detailed information on the thermodynamic model is given
employed, and the processing of the spectroscopy results. in [22,23,26].

2
V. Scharl and T. Sattelmayer
Fig. 1. RCEM driving system and cylinder head: (1) driving-air bottles, (2) driving piston, (3) hydraulic fluid, (4) flow orifice, (5) working piston, (6) combustion chamber,
(7) cylinder head, (8) diesel injector, (9) ammonia injector, (10) UV lens, (11) monochromator, (12) image intensifier, (13) high-speed camera.
Fuel injection is triggered based on the piston position via a Com-
pactRIO field-programmable gate array. Single-hole injectors inject the
fuels on a plane parallel to the flat piston surface to study the interac-
tion between the two sprays in detail. A custom Woodward L’Orange
injector with a 0.94 mm spray hole injects ammonia, while a Bosch
CRI 2.20 injector with a nozzle diameter of 0.2 mm supplies diesel. The
injection pressure of ammonia is 530 bar for the 125 bar TDC pressure
operating point, and the same relative pressure between the ammonia
injector and the chamber is maintained for the lower compression ratio
investigated. In contrast, the diesel injection pressure is kept constant
at 2000 bar, as the change in relative pressure is low. Air-driven high-
pressure pumps (Maximator G400-2 for diesel and Maximator G150-2
with EPDM gaskets for ammonia) supply the two fuels. The ammonia
fuel line features an additional counter-pressure valve that creates a
back-pressure of 15 bar in the leakage stream after the fuel injector.
The increased pressure inhibits fuel evaporation within the injector,
which would deteriorate injector behavior. The injectors were analyzed
in an IAV injection analyzer using calibration fluid. The correspond-
ing injection mass was then derived by assuming that the discharge
coefficient is independent of the fuel used. Coppo et al. [27] showed
that opening and closing behavior of the injector are not affected by
changing the fuel. However, Gaucherand et al. [28] pointed out that
ammonia may show significantly lower injection masses due to intense
cavitation under engine-relevant conditions, particularly when the fuel
is preheated. Therefore, ammonia was injected into the RCEM combus-
tion chamber under non-reacting conditions (i.e., no pilot) to confirm
the determined ammonia injection mass. The resulting concentration
in the chamber was measured using an ABB Advanced Optima Limas
21 HW gas analyzer. The difference in injected masses was small due
to the cold initial fuel temperature and the high combustion chamber
pressure, which reduce cavitation. The angle between the two fuel
sprays and the timing of the two injections can be freely adjusted.
However, in this work, timing and spray angle are fixed at values found
suitable in a previous publication, where a more detailed description of
the injection setup is given [23]. Based on these findings, the spray
interaction angle is set to −7.5◦ , which leads to slightly converging
and strongly interacting sprays. The start of diesel pilot injection is
set to 2 ms BTDC, corresponding to 12 CAD BTDC for 1000 rpm, while
ammonia is injected 0.5 ms after diesel. The work presented in the
paper at hand investigates two different TDC conditions. The less
reactive condition (OP3) features a TDC pressure of 98 bar and a TDC
temperature of 865 K. Soot luminosity is weak for these conditions,
and the CL emissions in the UV and visible range can be investigated
undisturbed. The highly reactive case (OP4) features a TDC pressure
of 125 bar and a temperature of 920 K, which are the most reactive
conditions possible in the RCEM employed. Under these conditions, the
strongly sooting diesel combustion leads to overexposure of the image
intensifier in the visible wavelength range. Therefore, the investigation
considers only spectrally resolved UV emissions for this operating point.
3
Fuel 358 (2024) 130201
Previous studies illustrate the high repeatability of experiments in
the RCEM by showing low variations in pilot fuel ignition delay [22,23]
and repeatable OH* CL intensities [16]. Furthermore, the results pre-
sented in this work rely on clear qualitative trends robust to the small
variations between individual experiments.
2.2. Optical setup
The optical investigations presented in this work rely on three differ-
ent optical setups: Spectrally resolved CL, simultaneous SG and OH*-CL
imaging, and NL imaging. First, the setup for spectrally resolved CL
measurements is presented.
Fig. 1 includes a scheme of the spectroscopy setup. A Cerco UV lens
with a focal length of 100 mm collects light emitted by the combus-
tion event and projects it onto the 10 μm slit of the monochromator.
The SpectraPro 275 spectroscope from Acton Research Corporation is
a Czerny-Turner type monochromator. It allows to change between
different gratings, which feature different densities of grooves per mm
and result in different spectral dispersions. In this work, a grating with
150 grooves per mm is used to resolve the CL in the UV–VIS range
from 275–750 nm with a spectral resolution of 1 nm, while 600 grooves
per mm are used to resolve the UV range from 275 nm to 400 nm with
a higher spectral resolution of 0.25 nm. A Hamamatsu C10880 image
intensifier coupled with Photron Fastcam SAX2 records the spectra at
the outlet of the monochromator. For the less reactive case (OP3), flame
emissions in the UV–VIS range are recorded with 20 000 f ps, while in
the UV range, longer exposure times were necessary, which resulted in
a frame rate of 10 000 f ps. For the highly reactive case (OP4), the soot
luminosity of the pilot fuel prohibits any investigations in the visible
wavelengths. The UV emissions were significantly brighter than in the
less reactive case and were recorded at 20 000 f ps. The resolution of
the spectrally resolved images is 1024 × 632 pixels. Different image
intensifier gains prohibit a comparison of the flame emission intensities
obtained for different combustion cases. Therefore, the results do not
provide absolute intensity values for most cases.
Simultaneous SG and OH*-CL images were obtained using the
double-pass setup shown in Fig. 2. A point source of light is created by
focusing a xenon-arc lamp on a pinhole. The pinhole is placed in the
focus of a large concave mirror redirecting the beams onto a flat mirror
and then into the combustion chamber. The light passes the combustion
event before it is reflected onto the same optical trajectory as before by
a polished stainless steel plate. Therefore, the density gradients in the
combustion chamber deflect the light beams twice. Two beam splitters
redirect the reflected light. For SG imaging, the light is detected directly
via a Photron Fastcam SAX with 20 000 f ps. The flame emissions, which
follow the same optical trajectory, are redirected by a second beam
splitter and filtered with a bandpass filter centered at 307 nm with an
FWHM of 10 nm. The same combination of Hamamatsu C10880 and
Photron Fastcam SAX2 as above is used for detecting the CL. For SG
V. Scharl and T. Sattelmayer
Fig. 2. SG and CL setup: (1) xenon-arc lamp, (2) UV-filter, (3) pin hole, (4) concave
mirror, (5) planar mirror, (6) reflective polished steel plate, (7) beam splitter,
(8) focusing lens, (9) bandpass filter, (10) image intensifier, (11) and (12) camera.
and OH* imaging, both cameras acquire images at 20 000 f ps. NL images
are captured separately in additional experiments. Due to the light
emitted by the xenon-arc lamp, simultaneous performance of NL and
SG imaging is impossible. As an image intensifier is not necessary for
detecting the bright visible flame luminosity, the setup consists only of
the Photron Fastcam SAX2 and a lens.
2.3. Spectroscopy image processing
The monochromator preserves the spatial coordinate along the
spray axis (vertical), while the incident light disperses on the coor-
dinate perpendicular to the spray axis (horizontal) depending on its
wavelength. Therefore, the horizontal positions of the pixels of the
images taken reflect specific wavelengths, while the vertical positions
of the pixels correspond to a certain height in the combustion chamber.
Before the combustion experiments, light emitted by a mercury-arc
lamp was recorded. This light consists of several distinct spectral lines
specific to mercury-arc lamps. Therefore, specific pixels of the images
taken correspond to certain wavelengths, and a conversion rule from
the wavelength to the pixel scale is derived based on interpolation. Fur-
thermore, the coordinate along the spray axis was calibrated by varying
the position of the mercury-arc lamp within the combustion cham-
ber. A third calibration procedure corrects the wavelength-dependent
sensitivity of the setup employed. This calibration requires a light
source with a continuous emission spectrum. Therefore, a halogen
lamp, whose spectrum is known from the manufacturer, was located
in the combustion chamber, and the light emitted was recorded. A
wavelength-dependent calibration function was derived by comparing
the intensities obtained by the spectroscopy setup to the reference
spectrum. This function corrects the spectra obtained during the exper-
iments. The correction considers the wavelength-dependent sensitivity
of the entire setup, encompassing the quartz-glass piston and lens
transmissivities, as well as the monochromator’s sensitivities and the
image intensifier’s sensitivities.
While significant parts of this work use raw spectra to discuss
the evolution of the dual-fuel combustion process, the results also
discuss the background corrected intensities of OH*, NH*, NH2 *, and
broadband emissions. The background corrected intensities result from
integrating peak areas corresponding to the respective species’ CL
emissions. These peak areas superimpose on a continuous background
of broadband flame emissions. Fig. 3 illustrates the areas considered
for the background corrected OH*, NH*, and NH2 * intensities. The
background radiation is interpolated linearly within the range, in which
each considered species causes a peak in CL emissions to distinguish
between species-specific and background radiation. The spectra were
filtered using a Savitzky-Golay filter in 𝑀𝑎𝑡𝑙𝑎𝑏 to reduce noise and
4
Fuel 358 (2024) 130201
enable reproducible interpolation of the background radiation. The
filter considered 21 interpolation points to approximate fifth-degree
polynomials. In addition, broadband luminosity intensity is consid-
ered, which is obtained by integrating the intensities over the entire
range of investigated wavelengths. While OH* and NH* intensities
are obtained by considering the area of individual peaks, the NH2 *
intensity is obtained by adding the intensity of several of its major
peaks. NH2 * flame emissions consist of a multiple-line system appearing
as a continuous band with superimposed heads [13,29]. Therefore, the
approach followed in this work only detects a fraction of the actual
NH2 * intensity. However, the intensity inferred from the peak areas
can give information on when NH2 * radiation occurs and its relative
intensity. OH* intensities were derived from images obtained using
both gratings. NH* intensities are derived using the higher spectral
dispersion, as the NH* peak was not sufficiently prominent for the
post-processing routine in the images obtained using grating 3. The
broadband radiation can mainly be assigned to CO2 * at shorter wave-
lengths and at longer wavelengths to NO2 *, H2 O*, and NH2 * [13]. For
diesel combustion, soot might occur additionally.
3. Results and discussion
In the first part of this section, temporally and spatially inte-
grated CL signatures of the lower reactivity combustion case with low
soot luminosity are presented to enable a detailed assignment of the
observed flame emissions to individual species. Subsequently, time-
resolved spectra are interpreted with SG, OH*-CL, and NL imaging
to describe the HPDF combustion process in detail. In addition, the
temporal evolution of background corrected OH*, NH*, NH2 *-CL and
broadband luminosity intensity are discussed in context to the HRRs
for two combustion chamber conditions. Three repetitions were carried
out for each case and measurement technique. The HRRs are averaged
over all experiments conducted for the combustion case, while the
spectroscopic data is averaged over the three experiments conducted
for each grating. The 2D imaging data is taken from the cases with the
HRRs most similar to the averaged HRR.
3.1. Integral flame spectra
The integral flame emissions shown in Fig. 4 are obtained by
temporally and spatially integrating the flame emissions. This results
in well-defined spectra suitable for identifying individual peaks and
the corresponding species. While the spatial integration was conducted
over the entire combustion chamber for diesel, the combustion chamber
region starting from 20 mm downstream of the diesel nozzle was
considered for the ammonia spectra shown to exclude the influence of
diesel combustion due to injector dripping. The diesel spectrum was
obtained by temporally integrating up to 900 μs ASOI. In comparison,
the ammonia spectrum was obtained by integrating from 1600 μs to
6000 μs ASOI (of diesel). As diesel is injected before ammonia, diesel
combustion progresses undisturbed at first. Subsequently, the sprays
interact, and both fuels burn simultaneously from approximately 900 μs
to 1600 μs ASOI. This flame transition period is not included in the
analysis conducted in this section and will be discussed in more detail
in the next section. The corresponding HRR and injection mass fluxes
are shown in Fig. 5.
In the following, A-X or B-X refers to the electron state transition,
while (𝑣′ , 𝑣′′ ) refers to the vibrational states of the electrons in their
upper and lower states. The UV range of the ammonia flame spectrum
shown in Fig. 4 a (grating 3, left part) and (c) (grating 2) consists
of the distinct NH* (A-X (0,0)) peak system at 336 nm and the OH*
(A-X (0,0)/(1,1)) peak system at around 308 nm superimposed on
weak broadband radiation. A weak peak visible at 282 nm results from
OH* (A-X(1,0)). Continuous broadband CL is observed for wavelengths
longer than 400 nm (see Fig. 4 a). A possible source for this radiation
is the CL of NO2 *. The approach by Sheehe and Jackson [30] is
V. Scharl and T. Sattelmayer Fuel 358 (2024) 130201

Fig. 3. Typical CL spectrum of ammonia combustion. Left: UV-range obtained using grating 2, right: UV–VIS spectrum obtained using grating 3. The colored peak areas represent
the background corrected CL intensity of the corresponding species. The peaks are extracted by interpolating the background radiation linearly in the respective wavelength ranges.

Fig. 4. Spatially and temporally integrated flame spectra (OP3). (a) and (b) were obtained using grating 3, while (c) was obtained using the higher spectral dispersion offered by
grating 2. (a) and (c) are obtained by temporal integration ranging from 1600 μs to 6000 μs ASOI, while (b) is obtained by integrating until 900 μs ASOI.

adopted to test whether NO2 * can explain the broadband emissions
observed for the ammonia flame. Therefore, the NO2 * intensity dis-
tribution presented by [31] is compared to the spectrum obtained in
this work (see Fig. 4 a). The NO2 * intensity distribution is fitted to the
ammonia flame emission spectrum so that the NO2 * emissions do not
exceed the ammonia flame emission intensity at any wavelength. As a
result, the NO2 * intensity distribution fits well in a range from 400 nm
to approximately 450 nm. However, the broadband emissions of the
ammonia flame are more intense for wavelengths longer than 450 nm
than to be expected if only NO2 * was contributing to its flame emis-
sions. Therefore, the maximum possible contribution of NO2 * to the
flame luminosity during ammonia combustion is small. The broadband
emissions unaccounted for by NO2 * may be attributed to H2 O* and to
NH2 * [20]. In addition, the NH2 * peaks of the ammonia-alpha band are
superimposed on the broadband spectrum. In addition to the OH* (A-
X (0,0)/(1,1)) peak system, the diesel spectrum recorded during earlier
combustion phases and shown in Fig. 4b shows more intense broadband
radiation in the UV range. This radiation is attributed to HCO (Vaidya’s
hydrocarbon flame bands), HCHO (Emeleus’s cool flame bands), as
well as CO2 * [13,32,33]. A weak CH* peak (A-X (0,0)) is visible at
432 nm. The highly bright sodium D-line at 589 nm results from sodium
impurities in the diesel fuel. An additional peak at approximately
460 nm could not be identified and is thought to result from impurities
in the diesel fuel. Similar to the ammonia case, broadband emissions
at longer wavelengths result from NO2 * and H2 O*. In addition, weak
soot luminosity occurred. The absence of distinct features of diesel
combustion in the ammonia emission spectra clearly shows that the
ammonia combustion phase after 1600 μs ASOI, in which the major part
of heat release occurs (see Fig. 5), is not directly supported by diesel
fuel combustion.
3.2. Temporal and spatial evolution of flame emissions
The temporal evolution of the combustion using SG, OH*-CL and
NL imaging is shown in Fig. 6 for 𝑡 = 700–1600 μs and in Fig. 7 for 𝑡 =
2000–5000 μs. The corresponding temporal evolution of flame spectra
for the same combustion case is shown in Fig. 8. While SG and OH*-CL
images were taken simultaneously, NL and spectroscopy imaging could
only be performed one at a time, which required repeated experiments.
SG contours are overlayed onto the OH*-CL images to enable a detailed

5
V. Scharl and T. Sattelmayer
Fig. 5. HRR and mass fluxes of the investigated combustion cases featuring a slightly advanced diesel pilot injection (+500 μs).
spatial allocation of the flame zone. To render the weak OH*-CL
during late ammonia combustion visible, the intensities in Fig. 7 are
brightness-corrected by potentiating the initial intensity values ranging
from 0 to 1 with 0.4. The flame emission spectra corresponding to the
timings of the images shown in Fig. 6 and Fig. 7 are shown in Fig. 8.
During diesel ignition, first weak NL is observed at 𝑡 = 700 μs (see
Fig. 6). The flame spectra (see Fig. 8 a) show first broadband CL with
only weak OH* luminosity at 𝑡 = 750 μs, which might hint at a strong
contribution of cool flame ignition chemistry to the flame emissions
observed. However, as experiments are averaged over three repetitions
and the camera’s exposure time was set to 𝑡 = 40 μs, no isolated
spectrum containing only cool flame chemistry was obtained. Subse-
quently, flame emission intensity increases significantly, and peaks,
such as OH*, CH*, and the sodium D-line, become more prominent in
the spectra. At 𝑡 = 850 μs, both, OH*-CL and NL, encompass the entire
diesel spray. Although the ammonia spray starts interacting with the
diesel spray at approximately 𝑡 = 750 μs, no sign of ammonia-specific
flame emissions, such as NH* and NH2 *, can be observed in the spectra
until 𝑡 = 1000 μs.
At 𝑡 = 1000 μs, NH* and NH2 * peaks first emerge on the spectra
(see Fig. 8 b). Simultaneously, OH*-CL decreases, reflected both in the
spectra and the OH*-CL images. The decrease starts at 𝑡 = 1000 μs on
the side, where ammonia interacts with the diesel cloud first (right)
before an intense reduction of the CL in almost the entire spray occurs.
At 𝑡 = 1600 μs, intense OH*-CL is restricted to a small pocket of gases
on the sides of the spray, which most likely contain diesel combustion
products. The emission spectra from 𝑡 = 1000 μs to 𝑡 = 1600 μs show
a decrease in overall intensity. The UV emission intensity drops to
particularly low levels. The emergence of the NH2 * peaks and the
decline of the sodium D-line mark the shift from diesel to ammonia
combustion. The location of both OH*-CL and NL indicates that the
flame does not encompass the ammonia spray tip in this combustion
phase. Instead, the reaction zone location changes only slightly during
the flame transition process, while the ammonia spray penetrates into
the combustion chamber. Therefore, unburned ammonia emissions may
originate in the spray tip region. This behavior is attributed to the
low ignitability of ammonia. In addition, the tip region features the
typical fuel-rich head vortex, which shows particularly poor mixture
formation, resulting in slower evaporation and lower temperatures [34,
35]. Furthermore, the HRR does not increase significantly between 𝑡 =
1000 μs to 𝑡 = 1600 μs, which also indicates slow and limited combustion
of ammonia in this phase. In contrast to recent spectroscopic studies
burning ammonia and a second, carbon-containing fuel [18–20], the
recorded spectra lack CN* peaks (e.g., B-X(0,0) and B-X(1,1) around
388 nm) during the entire combustion event. As CN originates from
interactions between carbon- and nitrogen-containing fuels, the lack of
its flame emissions hints at low rates of inter-species reactions between
ammonia and diesel for the combustion process investigated in this
work. The NH* peak is weak during flame transition and subsequent
6
Fuel 358 (2024) 130201
phases. The low relative intensity of the NH* peak compared to the
diesel background radiation intensity in the respective wavelength
range may prohibit its use as a flame marker for optical combustion
diagnostics.
During later combustion phases, the flame spectra do not show
significant qualitative changes apart from different intensities (see
Fig. 8 c). The UV emissions, in particular OH*-CL, become weaker,
while the peak intensity of visible broadband CL is reached between
𝑡 = 2000 μs and 𝑡 = 3000 μs. Both OH*-CL and NL drift off from the
injector until and after the end of injection at 𝑡 = 3200 μs (see Fig. 7).
Therefore, combustion progresses close to the cylinder wall, and more
air entrains up to the flame front. As a result, average equivalence
ratios become leaner, and combustion temperatures drop. The lack
of flame stabilization of ammonia flames observed can be attributed
to an inhibition of the stabilization mechanism predominant for con-
ventional diesel fuels, as mixing requirements of the fuel/air mixture
with combustion products to undergo auto-ignition are exceptionally
high for ammonia [16,36]. As OH*-CL gradually weakens, it cannot
be detected reliably for later combustion phases, while NL still permits
proper observation of the combustion event.
3.3. Temporal evolution of background corrected intensities of OH*, NH*
and NH2 *
The temporal evolution of background corrected intensities of OH*,
NH2 *, and broadband luminosity in the lower reactivity case OP3 are
shown in Fig. 9 a. The data is derived from the spectra obtained using
grating 3 according to the abovementioned procedure. Furthermore,
each intensity is normalized with its highest value. OH* and broadband
luminosity rise sharply after diesel ignition at 𝑡 ≈ 750 μs, with broad-
band luminosity reaching its first peak slightly earlier. Both intensities
start declining almost immediately, as pilot injection ends at 𝑡 = 520 μs,
and no new diesel fuel is supplied to the reaction zone. At 𝑡 ≈ 900 μs,
NH2 * intensity increases as ammonia starts reacting. Starting from 𝑡 ≈
1600 μs, broadband luminosity and NH2 * intensity correlate strongly,
indicating that the flame luminosity results from ammonia combustion
only. Therefore, the background corrected intensities corroborate the
findings inferred from the raw spectra above: After a short pure pilot
combustion phase, the flame transition occurs in which both fuels con-
tribute to combustion. However, the heat release during this transition
phase is low (see Fig. 5). The main part of combustion and heat release
is entirely attributed to the combustion of the ammonia spray.
Furthermore, the strong correlation between NH2 * peak intensity
and broadband luminosity suggests that a major part of the ammonia
flame emissions result from NH2 * under the conditions investigated.
The correlation is particularly strong for the time interval between
𝑡 ≈ 1600 μs and 𝑡 ≈ 3300 μs. Afterwards, broadband luminosity intensity
increases relative to the NH2 * intensity, which indicates the increasing
importance of other flame emissions, such as NO2 *-CL. The conversion
V. Scharl and T. Sattelmayer
Fig. 6. SG (top), OH*-CL with overlayed SG contours (middle) and NL (bottom) imaging obtained at OP3 (865 k, 98 bar). The left section contains images taken during pilot ignition
(𝑡 = 700–850 μs ASOI), while the right section contains images taken during the flame transition from diesel to ammonia (𝑡 = 1000–1600 μs ASOI). The combustion phases are also
indicated via the HRRs at the top.
of ammonia to NH2 via hydrogen abstraction is generally the first step
of most ammonia oxidation mechanisms [37], NH2 will mainly occur
close to the flame front. Therefore, the NL of the ammonia spray flame
observed is a suitable indicator for the flame front during a significant
part of the ammonia combustion phase. The findings align with a
recent study on visible ammonia flame emissions from atmospheric
burner flames: Weng et al. [29] found that NH2 * radiation is the main
source of CL at the flame front for fuel-rich and fuel-lean flames. In the
post-flame zone, NH2 * is the main contributor to flame emissions for
fuel-rich flames, while NO2 * radiation is the most important contribu-
tor for fuel-lean conditions. Equivalence ratios are non-uniform in the
spray combustion case investigated and subject to temporal and spatial
variations. However, the general trend as combustion progresses and
the lift-off length increases is a shift from conditions that show more
NH2 * radiation (high equivalence ratios, smaller amount of gas in post-
flame zone) to conditions that show more NO2 *-CL (lower equivalence
ratios, more gas in post-flame zone). In full engines, the pressure and
temperature rise due to combustion usually leads to ongoing reactions
in the burned charge, for example, caused by shifts in the chemical
7
Fuel 358 (2024) 130201
equilibrium. Owing to the low fuel mass supplied by the single-hole
injectors, this pressure rise due to combustion is low in the RCEM.
Therefore, practical engines may show more intense afterglow in the
burned zone.
The background corrected OH* and NH* intensities of both oper-
ating points investigated are shown in Fig. 9 b. The intensities are
obtained by analyzing the UV spectra obtained using the higher spectral
dispersion offered by grating 2, as sooting diesel pilot combustion at
OP4 permitted the investigation of longer wavelengths. As different im-
age intensifier gains prohibit the direct comparability of the intensities
of the two operating points compared, the intensities (OH* and NH*)
are normalized with the highest value of OH*-intensity occurring for
the respective operating point. Due to more reactive conditions, the
pilot ignition delay is shorter for OP4, which results in an earlier onset
of OH*-CL and heat release (see Fig. 5). The HRR of OP4 shows a more
prolonged delay between pilot combustion and ammonia combustion
due to the earlier pilot ignition. While the shape of OH*-CL intensity is
similar for both cases, the absolute OH* intensity was much higher for
OP4 due to higher temperatures. Higher combustion temperatures in
V. Scharl and T. Sattelmayer Fuel 358 (2024) 130201

Fig. 7. SG (top), OH*-CL with overlayed SG contours (middle) and NL (bottom) imaging obtained at OP3 (865 k, 98 bar). OH* intensities are 𝛾-corrected (𝛾 = 0.4). The images are
taken during the main fuel combustion phase, in which ammonia is burning (𝑡 = 2000–5000 μs ASOI). The combustion phases are also indicated via the HRRs at the top.

OP4 result from higher air temperature and from higher equivalence 4. Summary and conclusions
ratios due to less premixing, which results from the shorter ignition
delay. A slightly earlier onset of NH* emissions for OP3 can be at-
We investigated the flame emissions of diesel-piloted ammonia
tributed to earlier interaction between ammonia and diesel due to
sprays in an RCEM. For this purpose, two single-hole injectors were
ammonia’s faster penetration at lower charge air densities, as is ap-
employed. The pilot injector provided a small diesel fuel injection (5%
parent from well-known spray penetration correlations (e.g., [38,39]).
of total LHV supplied) followed by the ammonia main injection from
As a result of the earlier interaction, ammonia also ignites earlier.
the second injector. Spectrally resolved CL, SG, OH*-CL, NL imaging,
NH*-CL intensity is lower for OP4 relative to OH* intensity, which
and HRR analysis were employed to obtain profound insights into the
results from the more intense OH*-CL mentioned above. Both NH*
combustion process.
intensities peak twice, directly after ammonia ignition and before the
Based on spatially and temporally integrated spectra, as well as
peak HRR. While the second peak is expected based on ammonia
temporally resolved spectra, three phases of the HPDF combustion
combustion intensity, the first peak is thought to result from increased
process were identified:
NH production as entrained diesel combustion products lead to higher
combustion temperatures [40]. Furthermore, the high OH concentra- • First, diesel pilot ignition and combustion lead to a peak in HRRs.
tion produced during diesel combustion increases NH concentration via The flame emissions were typical for diesel flames featuring
the reaction NH2 + OH → NH + H2 O [19]. As expected, temperature, OH*, CH*, the sodium D-line, UV-broadband luminosity (HCO*,
pressure, equivalence ratio, and strain rate variations prohibit any HCOH*, CO2 *), as well as visible broadband luminosity (H2 O*,
direct correlation between HRR and CL intensity. NO2 * and soot).

8
V. Scharl and T. Sattelmayer
Fig. 8. Spatially integrated flame emission spectra at different times during diesel pilot ignition (a), flame transition from diesel to ammonia (b) and ammonia combustion (c) at
OP3.
Fig. 9. Temporal evolution of normalized background corrected CL intensities. (a):
HRRs and mass fluxes to facilitate the allocation of flame emissions to the combustion
phases (see Fig. 5), (b): OH* and NH2 *, as well as broadband luminosity for the less
reactive operating point (OP3). (c): OH* and NH* for the less reactive operating point
(OP3) and the highly reactive operating point (OP4).
• After interaction with the ammonia spray, the flame transition
started, during which flame emissions from NH3 and diesel com-
bustion were observed. HRRs only started to increase slowly.
Although both fuels burned simultaneously, CN*-CL was not de-
tected.
• The major share of heat release was found to occur during the
ammonia-only combustion phase, in which OH*, NH*, NH2 * and
broadband luminosity at visible wavelengths (NO2 *, H2 O*, NH2 *)
were observed. NO2 * provided a minor contribution to the overall
broadband flame emission intensity.
9
Fuel 358 (2024) 130201
OH*-CL and NL showed a strong spatial correlation. However, OH*-
CL dropped during ammonia combustion until it could not be detected
reliably anymore. We also found that the ammonia spray first pene-
trates through the diesel products without being ignited at its tip during
the flame transition phase, which constitutes a possible mechanism for
unburned ammonia emissions.
The peak areas of NH*, OH*, and NH2 * were extracted from the
emissions spectra to discuss their evolution. A strong correlation be-
tween NH2 * peak intensities and broadband CL intensity during the
ammonia combustion phase suggested that most ammonia flame emis-
sions originated from NH2 *-CL. Additional background radiation during
late ammonia combustion originated from NO2 *-CL in lean post-flame
zones. Increasing combustion chamber temperature and pressure leads
to an earlier onset of diesel combustion. However, the first occur-
rence of ammonia-specific flame emissions did not change significantly,
indicating the high importance of spray interaction for the onset of
ammonia combustion.
Apart from improving the understanding of the HPDF combustion
process, the insights obtained in this study will help choose suitable
methods for future optical investigations of diesel-piloted ammonia
combustion. For cases with low soot formation, we suggest focusing on
wavelengths that capture NH2 *-CL, as they offer a strong signal, which
mainly originates from the flame front during ammonia combustion.
Although UV flame emissions are much stronger during pilot com-
bustion, cases with strongly sooting diesel combustion might require
observing wavelengths in the UV range. The best option available is
the observation of established OH*-CL wavelengths (around 308 nm),
as they offer the strongest absolute and relative signal during ammonia
combustion. Observing the wavelengths relevant for NH*-CL (around
336 nm) is not recommended, as diesel UV broadband emissions are
strong relative to the intensity of the narrow NH* peak in this range.
Nomenclature
Abbreviations
ASOI after start of injection
btdc before top dead center
CAD crank angle degree
CL chemiluminescence
V. Scharl and T. Sattelmayer Fuel 358 (2024) 130201

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