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Table of Contents 

Abstract


Introduction



Materials 
Share
and Access Article
Open
Methods

:
Greenhouse Gases Detection Exploiting a Multi-
Help
Results


Conclusions


Wavelength

Author
Interband Cascade Laser Source in Cite
a Contributions
Quartz-Enhanced Photoacoustic Sensor
by Funding


Discuss in
Institutional 1,†

 SciProfiles
Raffaele De Palo (mailto:[email protected])
Review (https://sciprofi
(https://orcid.org/0000-0002-3563-2206),
Board groups/public/1
Nicoletta Ardito 1,†  (mailto:[email protected])
Statement utm_source=mp
(https://orcid.org/0009-0005-9275-4129),
Informed


Andrea Zifarelli 1  (mailto:[email protected])

Consent
(https://orcid.org/0000-0003-1875-4671),
Statement
Angelo Sampaolo 1,2  (mailto:[email protected]),
Data


Marilena Giglio 1,*  (mailto:[email protected])

Availability
(https://orcid.org/0000-0003-2603-7648),
Statement
Pietro Patimisco 1,2  (mailto:[email protected]),

Conflicts
Ezio
of
Ranieri 3  (mailto:[email protected]) (https://orcid.org/0000-
0002-5017-0396),
Interest
Robert
 Weih 4  (mailto:[email protected]),
References
Josephine Nauschütz 4  (mailto:[email protected])
(https://orcid.org/0009-0007-6764-7799),
Oliver König 4  (mailto:[email protected]) and
Vincenzo Spagnolo 1,2  (mailto:[email protected])
(https://orcid.org/0000-0002-4867-8166)

1 PolySense Lab, Dipartimento Interateneo di Fisica, University and

Polytechnic of Bari, Via Amendola 173, 70126 Bari, Italy

2 PolySense Innovations srl, Via Amendola 173, 70126 Bari, Italy
3 Dipartimento di Biologia, Università degli Studi di Bari, Via Orabona 4,

70126 Bari, Italy

4 Nanoplus Advanced Photonics Gerbrunn GmbH, Oberer Kirschberg 4,

97218 Gerbrunn, Germany

* Author to whom correspondence should be addressed.
† These authors contributed equally to this work.
:
Sensors 2025, 25(8), 2442; https://doi.org/10.3390/s25082442
(https://doi.org/10.3390/s25082442)

Submission received: 20 March 2025 / Revised: 8 April 2025 /

Accepted: 9 April 2025 / Published: 12 April 2025

(This article belongs to the Special Issue Recent Trends and Advances in
Laser Spectroscopy and Sensing (
/journal/sensors/special_issues/ls_sensing ))

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Abstract

This study presents the performance of a multi-gas sensor for greenhouse

detection based on quartz-enhanced photoacoustic spectroscopy (QEPAS).
The QEPAS sensor exploits an innovative, compact three-wavelength laser
module as excitation source. The module integrates three interband cascade
laser chips with a beam combining system, all enclosed in a compact metallic
package with sizes of 40 × 52 × 17 mm to generate a single output beam. The
multi-gas QEPAS sensor was tested in a laboratory environment for the
sequential detection of two greenhouse gases, methane (CH4) and carbon
dioxide (CO2), and a precursor greenhouse gas, carbon monoxide (CO). At an
integration time of 100 ms, minimum detection limits of 21 ppb, 363 ppb, and
156 ppb, were estimated for CH4, CO2, and CO detection, respectively, all well
below their natural abundance in air.
Keywords: quartz-enhanced photoacoustic spectroscopy (/search?
q=quartz-enhanced+photoacoustic+spectroscopy); interband cascade
lasers (/search?q=interband+cascade+lasers); greenhouse gases
(/search?q=greenhouse+gases)

1. Introduction
:
 In 2023, global temperatures reached unprecedented levels, marking it as
the warmest year on record with an increase of 1.45 °C above pre-industrial
levels. The World Meteorological Organization (WMO) has highlighted
concerning trends in key climate indicators, including greenhouse gas (GHG)
concentrations and global temperatures, emphasizing the critical role of
methane (CH4) and carbon dioxide (CO2) in driving global warming [1,2].
Carbon dioxide is the most prevalent anthropogenic GHG, primarily
arising from fossil fuel combustion, vehicle exhaust, industrial processes, and
deforestation [2]. Recent data from NOAA’s Global Monitoring Laboratory
revealed that in 2023, the global average atmospheric CO2 concentration
reached a new record of 419.3 parts per million (ppm), an increase of 2.8 ppm
with respect to the previous year [3].
Methane, despite its low concentration (~1.8 ppm), exerts significant
influence on global climate due to its heat-trapping capability. Over a 100-year
period, it has a global warming potential (GWP) approximately 25 times
greater than CO2 [2,4]. Beyond its climatic effects, methane also contributes to
local air quality degradation as a precursor to ground-level ozone (O3). Major
sources of methane emissions include fossil fuel production (especially natural
gas), vehicle exhaust, and agricultural activities [2,5].
Together with methane and CO2, carbon monoxide (CO) also acts as a
precursor GHG influencing atmospheric chemistry and human health [6].
Originating from incomplete combustion in industrial and vehicular activities,
CO interacts with hydroxyl radicals (OH) in the atmosphere to produce CO2,
thereby increasing its concentration in the atmosphere. Additionally, CO
affects methane concentrations in the atmosphere by competing with CH4 for
OH. The oxidation of methane primarily occurs through its reaction with OH,
leading to the formation of water (H2O) and CO2. This oxidation process is
crucial for reducing methane concentrations in the atmosphere and mitigating
its overall impact as a greenhouse gas. When CO is present in elevated
concentrations, it can significantly decrease the availability of OH, thereby
influencing both the atmospheric lifetime and concentration of methane.
Moreover, CO poses significant health risks even at low levels because it
reduces the ability of hemoglobin to transport oxygen in the blood. The World
:
Health Organization (WHO) advises stringent limits for short-term exposure
(25–35 ppm for one-hour exposure) to mitigate health impacts, highlighting the
dual environmental and public health challenges [7].
The 2023 Annual Report from the United Nations Environment
Programme (UNEP) underscores the urgent need for a global response to the
growing challenges of climate change, loss of biodiversity, and pollution [8]. In
this scenario, a strategic priority is the creation of cost-effective stations for
continuous, accurate, and selective monitoring of greenhouse gases (GHGs)
in the atmosphere, which are also crucial for evaluating the effectiveness of
interventions in achieving the desired outcomes. To address this requirement,
GHGs sensors are continuously developed and improved. Among these,
electrochemical, semiconductor-based, and optical-based sensors have
gained popularity due to their cost-effectiveness and their compact design.
Electrochemical sensors, like the Alphasense CO-A4, achieve MDLs of a few
ppm but face challenges such as short service life and poor selectivity due to
cross-interference with other gases [9]. Semiconductor-based sensors, such
as Figaro Inc.’s TGS 3870-B00, are remarkable for their compactness and
affordability in detecting gases like carbon dioxide and methane [10]. However,
their methane detection range, typically in the thousands of ppm, limits their
suitability for environmental monitoring. NDIR sensors, like the Senseair K30,
offer sensitivity ranging from low ppm to percentage levels, with power
consumption typically between 50 mW and a few watts, depending on the gas
type and configuration. On the other hand, they are not highly selective and
suffer from spectral interference by water [11,12]. Asking for high sensitivity
and specificity, laser-based gas sensing techniques occupy a dominant role in
trace gas detection. These methods also fulfill the requirements for real-time
monitoring thanks to their fast response time [13,14,15,16]. For instance,
Cavity Ring-Down Spectroscopy (CRDS) sensors, such as the Picarro Gas
Concentration Analyzer, offer sensitivity levels down to a few parts-per-billion
(ppb) for methane and carbon monoxide [17,18]. Nevertheless, CRDS
systems require perfect optical alignment, and their high cost, several kilo
euros, along with a bulky form factor, limits their use in environmental
monitoring applications. In this context, Quartz Enhanced Photoacoustic
:
Spectroscopy (QEPAS) stands out as a reliable and robust technique for the
detection of several trace gas species [19,20,21,22,23,24,25]. QEPAS exploits
the principles of photoacoustic spectroscopy, employing a quartz tuning fork
(QTF) as an acoustic transducer [26]. Photoacoustic effect occurs when
periodically modulated light is absorbed by a gas sample. Through non-
radiative relaxation pathways, the modulated absorption is converted into
pressure waves, which can be detected using a transducer. In QEPAS, these
waves are detected by a QTF and converted into an electrical signal through
the piezoelectric effect occurring in the quartz crystal. To enhance the
sensitivity of the QEPAS sensor, the QTF is typically coupled with a pair of
millimeter-size resonator tubes to amplify the pressure waves. The QTF
response is independent of the exciting light source wavelength, making it a
promising candidate for use with multi-wavelength sources. Recently, a
QEPAS sensor for multi-gas detection with a multi-wavelength source
consisting of three commercial Quantum Cascade Lasers (QCLs) within a
single box has been proposed [27]. Three QCLs housed in HHL packages
were mounted into an aluminum box and manually aligned to be collinear,
using free-space optics mounted on standard mechanical supports. The
resulting assembly is bulky, uses a lot of energy, and faces several thermal
management challenges related to the operation of each HHL package.
Additionally, the stability of the beam collinearity is significantly affected by
extra-thermal heating inside the enclosure, especially when three QCLs are
turned on simultaneously. This suggests that, to achieve successful long-term
stability in multi-laser sources, a different technological approach is needed:
instead of assembling multiple laser sources in one box, it involves integrating
various laser chips into a single package. This minimizes the system’s
footprint, which is particularly important in space-constrained environments.
Moreover, the optical assembly required for ensuring the collinearity of
different beams must be integrated in a compact way, avoiding the use of large
mechanical supports. The optical components should be securely fixed to
minimize internal misalignments caused by thermal expansion. To improve
thermal extraction, the use of low-power consumption laser chips becomes
mandatory. Furthermore, from a market perspective, manufacturing and
:
assembling multiple laser chips into a single module can reduce packaging
costs, simplify the alignment process, and streamline production, leading to
lower overall costs compared to using individual laser modules.
In this work, an innovative three-wavelength ICLs module was employed
as a light source for a compact multi-gas QEPAS sensor [28,29,30,31]. The
module offers remarkable compactness and ruggedness, being characterized
by reduced dimensions (~5 cm on the longest side) and a robust design. It
incorporates three distinct ICL chips, which are combined into a single output
beam through a custom-designed integrated beam combining system made of
lenses and dichroic mirrors. The 3λ-module was employed as laser source for
a QEPAS sensor for the sequential detection of direct and precursor GHGs,
namely CH4, CO2, and CO. Using this configuration, a laboratory benchtop
sensor prototype was developed, and the three gases were targeted in a
controlled environment as proof of concept.

2. Materials and Methods

2.1. Three-Wavelength ICL Module
The laser source is a multi-wavelength module, realized by Nanoplus
Advanced Photonics Gerbrunn GmbH, consisting of three ICL chips with
central emission wavelengths of 3.35 µm, 4.23 µm, and 4.57 µm, selected for
detecting CH4, CO2, and CO, respectively. The laser chips are mounted on
aluminum nitride heat spreaders and arranged on sub-mounts within
aluminum housing, which includes Peltier elements for the thermal
management of each laser. The power consumption of each ICL is lower than
0.7 W. A schematic illustration of the module is depicted in Figure 1a.
:
 Figure 1. (a) Schematic of the three wavelength devices; L1, L2, L3, and
L4 are lenses; M1 is a CaF2-substrate based mirror, while M2 and M3 are
YAG-substrate based mirrors. (b) Beam profiles of the laser targeting CH4
(blue), CO2 (red), and CO (green) overlapped in the focal plane of the 3λ-
module.

The module measures 40 × 52 × 17 mm and integrates a beam

combining system consisting of three lenses (L1, L2, and L3) and three
dichroic mirrors (M1, M2, and M3), designed to obtain a single output beam.
Each ICL beam is focused using a dedicated lens that is mounted on the same
sub-mount as the laser chip, ensuring stable thermal performance. The beams
of the different lasers are focused onto the focal plane of the ADM. This is
achieved by first focusing each laser beam to the corresponding path length
using a lens and then combining the beams using dichroic mirrors. A high-
resolution pyrocamera (Pyrocam III, Ophir Spiricon PY-III-C-C) with pixel size
of 0.1 × 0.1 mm was placed at the focal plane of the 3λ-module to analyze the
overlap of three ICL beams. The resulting intensity distribution of the three ICL
beams is shown in Figure 1b. The overall light distribution diameters in both
the x- and y-directions were measured to be 0.8 mm.
2.2. Experimental Setup for Multi-Gas QEPAS Sensor
The 3λ-module was used as a light source in a QEPAS sensor setup
schematically illustrated in Figure 2.
:
 Figure 2. Schematic of the employed 3λ-ICL QEPAS setup; ADM,
acoustic detection module; PC, personal computer.

The Acoustic Detection Module, ADM01, provided by Thorlabs GmbH,

was equipped with two windows (WG70530-E4) with AR coating in the 2–5 µm
range. ADM01 contains a spectrophone, which consists of a T-shaped QTF
acoustically coupled with a pair of millimeter-size resonator tubes arranged on
both sides of the QTF, in an on-beam configuration. Each tube has a length of
12.4 mm, and an internal and external diameter of 1.59 and 1.83 mm,
respectively [32]. The transmitted optical power through the ADM was
monitored by a power meter to refine the optical alignment. The gas handling
system included a gas mixer (MCQ Instruments, Gas Blender 103), mounted
upstream to maintain a gas flow rate of 50 sccm; downstream, a pressure
controller (Alicat, MC3S-200SCCM) and a vacuum pump fixed the operating
pressure at 400 Torr. In these operating conditions, the spectrophone had a
resonance frequency of 𝑓0 = 12,439.4 Hz with a quality factor of 14,650. The
3λ-module QEPAS sensor operated in wavelength modulation with dual-
frequency detection (2f-WM) [33]. A sinusoidal dither at half of the resonance
frequency of the spectrophone, 𝑓 = 𝑓0 /2 , was applied to the ICL current driver
(ITC4002QCL, Benchtop Laser Driver and Temperature Controller, Thorlabs)
together with a low-frequency ramp to scan across the absorption feature. The
:
resulting QTF signal was demodulated at 𝑓0 by a lock-in amplifier (Zurich
Instruments MFI 500 kHz Lock-in Amplifier) with an integration time of 0.1 s
and a roll-off of 12 dB/oct.

3. Results

This section presents the results obtained using the 3λ-module QEPAS
sensor for the in-sequence detection of CH4, CO2, and CO. The performance
of the sensor was evaluated by operating the three ICL chips individually: the
3.35 µm laser chip for the CH4 detection, the 4.23 µm chip for CO2 detection
and the 4.57 µm chip for CO detection. The temperature of the module was
maintained at 15 °C using a temperature controller to regulate the Peltier cell.
For each analyte, the sensor calibration was performed by diluting a certified
mixture in nitrogen (N2) with pure N2 and acquiring QEPAS spectral scans at
different concentrations across the selected absorption feature.
3.1. Direct Greenhouse Gases Detection
3.1.1. Methane Detection
Methane was the first analyte investigated. Its absorption cross-section
was reconstructed using the HITRAN database [34], simulating at 400 Torr a
mixture of 1.8 ppm of CH4 in N2 within the 2988.4–2989.4 cm−1 range, which
corresponds to the spectral dynamic range of the 3.35 µm-chip. In addition,
the absorption cross-section of mixtures of 420 ppm of CO2 in N2, 100 ppb of
CO in N2, and 0.4% of H2O in N2 were also included in the simulation to
evaluate potential spectral interferences with CH4 detection. The simulated
analyte concentrations are equal to the estimated atmospheric abundance of
the target species [3,7,33]. The results are shown in Figure 3.
:
 Figure 3. Absorption cross-section of a mixture of 1.8 ppm of CH4 in N2,
a mixture of 420 ppm of CO2 in N2, a mixture of 100 ppb of CO in N2, and
a mixture of 0.4% of H2O in standard air, simulated with the HITRAN
database within the emission spectral range of the 3.35 µm ICL at 400
Torr and room temperature.

The simulation reveals an absorption feature of water vapor at 2988.62

cm−1, which is sufficiently distant from the CH4 triplet, characterized by three
distinct peaks at 2988.82 cm−1, 2988.98 cm−1, and 2989.08 cm−1, all with
similar cross-sections.
The response of the 3λ-ICL QEPAS sensor for CH4 detection was
evaluated by turning on the 3.35 µm chip. Starting from a certified
concentration of 50 ppm of CH4 in N2, different mixtures were generated with
methane concentrations in the range 10–50 ppm in N2. Figure 4a reports the
CH4 QEPAS spectral scans acquired in the full spectral range of the 3.35 µm
chip at different methane concentrations.
:
 Figure 4. (a) QEPAS spectral scans measured for different
concentrations of CH4 in N2 as a function of ICL injection current; (b)
QEPAS signal of the most intense CH4 feature as a function of gas
concentration (black squares) and the corresponding best linear fit (red
solid line).

The acquired QEPAS spectral scan matches the CH4 simulation in Figure
3 with the strongest absorption feature observed at an ICL current of 97.5 mA,
corresponding to a laser emission at 2988.82 cm−1, with an optical power of
20 mW. For each spectral scan, the peak value of this intense feature was
extracted and plotted as a function of the CH4 concentration, as shown in
Figure 4b. A linear fit of the experimental data points was performed to obtain
the sensor calibration curve for methane, depicted as a red solid line in Figure
4b, with an R-squared value higher than 0.999. The sensor sensitivity was
estimated from the slope of the best fit, resulting in 7.70 ± 0.11 mV/ppm. A 1-σ
noise level of 0.16 mV was measured by flowing N2 through the ADM, while
the laser current was fixed at 97.5 mA. The minimum detection limit (MDL)
was calculated as the concentration corresponding to a signal-to-noise ratio of
1. For CH4, an MDL of 21 ppb was estimated with a 0.1 s lock-in integration
time, well below its natural atmospheric concentration.
3.1.2. Carbon Dioxide Detection
The absorption cross-section of carbon dioxide was reconstructed using
the HITRAN database for a mixture of 420 ppm of CO2 in N2 within the
spectral range of 4.23 µm chip, from 2363.3 to 2364.8 cm−1, at 400 Torr. As
before, the results of simulation are reported in Figure 5 together with the
:
simulations of a mixture of 1.8 ppm of CH4 in N2, a mixture of 100 ppb CO in
N2, and a mixture of 0.4% H2O in N2, in the same spectral range.

Figure 5. Absorption cross-section of a mixture of 420 ppm of CO2 in N2,

a mixture of 1.8 ppm of CH4 in N2, a mixture of 100 ppb of CO in N2, and
a mixture of 0.4% of H2O in standard air, simulated with the HITRAN
database at 400 Torr and room temperature.

A well-isolated CO2 absorption feature located at 2364.1 cm−1 can be

detected by the 4.23 µm chip at an injection current of 125.8 mA and with an
optical power of 1.4 mW, completely free from interference by the other two
gases. The CO2 2f-spectral scans were measured with the 4.23 µm ICL chip
with different mixtures of CO2 in the range of 250–1000 (tel:250–1000) ppm in
N2. The acquired CO2 2f-spectral scans are shown in Figure 6a.
:
 Figure 6. (a) QEPAS spectral scans measured for different concentration
of CO2 in N2 and pure N2; (b) QEPAS signal of the absorption feature,
targeted at an injection current of 125.8 mA for the 4.23 µm ICL, as a
function of the CO2 concentration (black squares) with the corresponding
best linear fit (red solid line).

For each spectral scan, the peak values were extracted and plotted as a
function of the CO2 concentrations in Figure 6b. The linear fit yields a
detection sensitivity of 0.44 ± 0.01 mV/ppm based on the linear regression of
data points. With a measured 1-σ noise level of 0.16 mV, estimated as
previously described, and an MDL of 363 ppb for CO2 detection, well below its
natural concentration, was estimated at 0.1 s lock-in integration time.
3.2. Precursor Greenhouse Gas Detection: Carbon Monoxide
The QEPAS sensor calibration for carbon monoxide was performed
employing the same method and procedure as the direct greenhouse gases.
The absorption cross-section of carbon monoxide was simulated with the
HITRAN database within the spectral emission of the 4.57 µm chip, from
2189.6 to 2190.4 cm−1. To evaluate potential spectral interferences, a mixture
of 100 ppb of CO in N2, a mixture of 1.8 ppm of CH4 in N2, a mixture of 420
ppm of CO2 in N2, and a mixture of 0.4% H2O in N2 were also included in the
simulation reported in Figure 7.
:
 Figure 7. Absorption cross-section of a mixture of 100 ppb of CO in N2, a
mixture of 1.8 ppm of CH4 in N2, a mixture of 420 ppm of CO2 in N2, and
a mixture of 0.4% of H2O in standard air, simulated with the HITRAN
database at 400 Torr and room temperature, within the 4.56 µm ICL
spectral range.

The isolated CO absorption feature located at 2190 cm−1, free from

interference by the other analytes, has been reconstructed using the 4.57 µm
ICL chip at an injection current of 144.7 mA with an optical power of 8.4 mW.
Different 2f-spectral scans of CO measured at different CO concentrations in
N2 are plotted in Figure 8a.

Figure 8. (a) QEPAS spectral scans measured for different

concentrations of CO in N2 and pure N2; (b) QEPAS signal of the most
intense feature as a function of the CO concentration (black squares) and
the corresponding best linear fit (red solid line).

The calibration curve was obtained by plotting the peak values of the
spectral scans as a function of the CO concentration, as shown in Figure 8b.
The error bars represent the standard deviation of the QEPAS signal,
evaluated as previously described. From the best linear fit, a sensitivity of 1.15
± 0.05 mV/ppm was determined. With a 1-σ noise level of 0.17 mV, the MDL
was estimated to be 148 ppb at a lock-in integration time of 0.1 s, which is
below the WHO one-hour average safe limit.
3.3. Long-Term Stability of the Sensor
:
 To assess the stability of the sensor and estimate the 1-σ noise as a
function of the lock-in integration time, an Allan–Werle deviation analysis of
the 3λ-ICL QEPAS sensor was performed. This analysis involved
simultaneously activating all three ICL chips at their respective current values,
which correspond to the peak values extracted from spectral scans for
calibration. Measurements were taken over a seven-hour acquisition period at
0.1 s lock-in integration time, with N2 flowing in the ADM01 at 400 Torr and a
gas flow rate of 50 sccm. The results of the Allan–Werle analysis are
presented in Figure 9.

Figure 9. Allan–Werle deviation for the 3λ-ICL QEPAS noise level as a

function of the integration time.

The noise level decreases with the integration time following the expected
trend of ~1/√t. This indicates the predominance of QTF thermal noise as the
noise source. For integration times exceeding 600 s, the noise performance
begins to degrade due to slow mechanical vibrations, which become
increasingly relevant over longer periods. With a lock-in integration time of 10
s, the 1-σ noise of the 3λ-ICL QEPAS signal can be reduced to 0.06 mV, thus
achieving an MDL of 8 ppb, 136 ppb, and 55 ppb for CH4, CO2, and CO
:
detection, respectively.
3.4. Gas Mixtures Detection and Analysis
The multi-gas detection capabilities of the QEPAS sensor were further
validated by performing measurements on three different gaseous samples
which were synthetically generated in laboratory environment with the
following mixing ratios:
Mix #1: 500 ppm CO2, 12.5 ppm CH4, 250 ppm CO, in N2;
Mix #2: 250 ppm CO2, 25 ppm CH4, 250 ppm CO, in N2;
Mix #3: 250 ppm CO2, 12.5 ppm CH4, 500 ppm CO, in N2.
The 2f-spectral scans of the analytes were obtained by sequentially
activating the three laser chips, with the sensor operating under the same
experimental conditions employed for the calibration phase. Each scan was
acquired with a lock-in integration time of 100 ms, and the results are shown in
Figure 10.

Figure 10. 2f-QEPAS Spectral Scans of CO2, CH4, and CO in Gas

Mixtures #1, #2, and #3. From left to right: spectral responses for CO2,
CH4, and CO. The breakpoints in the spectra represent the time interval
of approximately 10 s required for sequential detection between each
laser.
:
 The QEPAS signals obtained for each analyte in the multi-gas mixtures
closely match the corresponding single-gas signals measured during the
sensor calibration (Figure 4, Figure 6 and Figure 8). No significant signal
distortion or interference was detected, confirming that the presence of
additional gas components in the mixtures had no impact on the spectral
response.
For each spectral scan, the peak value was extracted and converted into
a concentration using the calibration curves derived in the previous section.
Table 1 summarizes the expected and estimated concentrations for each
analyte, along with the associated signals and the relative differences between
expected and estimated values.

Table 1. Expected and estimated concentrations for each analyte in the

three mixtures, with associated signals and relative difference.

The errors associated with the expected concentrations were calculated

by combining the expanded uncertainties of the certified gas cylinders
concentrations provided by the manufacturer (4% at 3-σ) and the gas mixer
setpoint accuracy (1% at 1-σ). Signal fluctuation was determined as the 1-σ
standard deviation from a 10 min acquisition while flushing the gas mixture
through the sensor. This value was incorporated into the error propagation,
along with the sensitivity uncertainty, to compute the total error in the
estimated concentrations. For all mixtures, the analytes expected and
estimated concentrations are comparable within the relative uncertainty
intervals, demonstrating the sensor’s reliability.

4. Conclusions

In this work, a novel three-wavelength ICL module was employed as a

:
light source for a multi-gas QEPAS sensor. The module integrates three chips
with emission wavelengths of 3.35 µm, 4.23 µm, and 4.57 µm, properly
selected for detecting CH4, CO2 and CO, respectively. The three beams were
combined to generate a single focused output using an integrated beam
combining system housed within a compact module, with overall sizes of 40 ×
52 × 17 mm. The QEPAS sensor was calibrated in a laboratory environment
for sequential detection of CH4, CO2, and CO, achieving a sensitivity of 7.70
mV/ppm, 0.44 mV/ppm, and 1.09 mV/ppm, respectively. The measured 1-σ
noise levels were 0.160 mV for CH4, 0.16 mV for CO2, and 0.17 mV for CO
detection, resulting in estimated MDLs of 21 ppb, 363 ppb, and 148 ppb,
respectively, at an integration time of 0.1 s, which, respectively, reduces to 8
ppb, 136 ppb, and 55 ppb for 10 s integration time.
To assess the impact of drift in the quartz tuning fork’s parameters on the
long-term stability of the QEPAS sensor, its resonance frequency and quality
factor were periodically monitored throughout the experiment. No significant
variations were observed, confirming that drift had a negligible effect on the
overall sensor performance.
The compact design of the 3λ-ICL module ensures reliable performance in
a small form factor, making it an ideal source for a QEPAS sensor for real-time
and multi-gas detection of GHGs and their GHG precursor CO. Considering
the characteristics of the developed multi-gas sensor (compactness, versatility,
detection limits, etc.), it represents a promising solution for urban air quality
monitoring. Offering a cost-effective solution at a few thousand euros, it
addresses a critical gap in gas detection technologies for long-term
monitoring, with potential for significant cost reductions through large-scale
production of the custom laser source. Finally, its efficient thermal
management and compact size facilitate integration into mobile platforms,
such as drones.

Author Contributions

Conceptualization, A.Z., M.G. and P.P.; methodology, N.A., A.Z., A.S., J.N.
and E.R.; investigation, N.A., A.Z., R.D.P., M.G., J.N. and O.K.; resources,
P.P., R.W. and J.N.; data curation, A.Z., N.A. and R.D.P.; writing—original draft
:
preparation, A.Z., N.A. and P.P.; writing—review and editing, All authors;
supervision, P.P., R.W. and V.S.; funding acquisition, P.P., R.W. and V.S. All
authors have read and agreed to the published version of the manuscript.

Funding

Authors from University and Polytechnic of Bari acknowledge funding

from the European Union’s Horizon 2020 research and innovation program
under grant agreement No. 101016956 PASSEPARTOUT, in the context of the
Photonics Public–Private Partnership, project MUR—Dipartimenti di
Eccellenza 2023–2027—Quantum Sensing and Modelling for One-Health
(QuaSiModO), PNRR MUR project PE0000023-NQSTI and from PNRR MUR
project PE0000021-NEST. Marilena Giglio acknowledges funding from the
PRIN 2022 PNNR, ImPACT-AI project P2022C338Z.

Institutional Review Board Statement

Not applicable.

Informed Consent Statement

Not applicable.

Data Availability Statement

Data are available on demand.

Conflicts of Interest

Author Angelo Sampaolo, Pietro Patimisco, and Vincenzo Spagnolo were

employed by the PolySense Innovations srl company. Author Robert Weih,
Josephine Nauschütz, and Oliver König were employed by the Nanoplus
Advanced Photonics Gerbrunn GmbH company. The remaining authors
declare that the research was conducted in the absence of any commercial or
financial relationships that could be construed as a potential conflict of interest.
:
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MDPI and ACS Style

De Palo, R.; Ardito, N.; Zifarelli, A.; Sampaolo, A.; Giglio, M.; Patimisco, P.;
Ranieri, E.; Weih, R.; Nauschütz, J.; König, O.; et al. Greenhouse Gases
Detection Exploiting a Multi-Wavelength Interband Cascade Laser Source in a
Quartz-Enhanced Photoacoustic Sensor. Sensors 2025, 25, 2442.
https://doi.org/10.3390/s25082442
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AMA Style
De Palo R, Ardito N, Zifarelli A, Sampaolo A, Giglio M, Patimisco P, Ranieri E,
Weih R, Nauschütz J, König O, et al. Greenhouse Gases Detection Exploiting
a Multi-Wavelength Interband Cascade Laser Source in a Quartz-Enhanced
Photoacoustic Sensor. Sensors. 2025; 25(8):2442.
https://doi.org/10.3390/s25082442

Chicago/Turabian Style
De Palo, Raffaele, Nicoletta Ardito, Andrea Zifarelli, Angelo Sampaolo,
Marilena Giglio, Pietro Patimisco, Ezio Ranieri, Robert Weih, Josephine
Nauschütz, Oliver König, and et al. 2025. "Greenhouse Gases Detection
Exploiting a Multi-Wavelength Interband Cascade Laser Source in a Quartz-
Enhanced Photoacoustic Sensor" Sensors 25, no. 8: 2442.
https://doi.org/10.3390/s25082442

APA Style
De Palo, R., Ardito, N., Zifarelli, A., Sampaolo, A., Giglio, M., Patimisco, P.,
Ranieri, E., Weih, R., Nauschütz, J., König, O., & Spagnolo, V. (2025).
Greenhouse Gases Detection Exploiting a Multi-Wavelength Interband
Cascade Laser Source in a Quartz-Enhanced Photoacoustic Sensor. Sensors,
25(8), 2442. https://doi.org/10.3390/s25082442

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