3.9 6.

Letter

A Dual-Laser Sensor Based on Off-

Axis Integrated Cavity Output
Spectroscopy and Time-Division
Multiplexing Method

Kunyang Wang, Ligang Shao, Jiajin Chen, Guishi Wang, Kun Liu, Tu Tan, Jiaoxu Mei,
Weidong Chen and Xiaoming Gao

https://doi.org/10.3390/s20216192
 sensors
Letter
A Dual-Laser Sensor Based on Off-Axis Integrated
Cavity Output Spectroscopy and Time-Division
Multiplexing Method
Kunyang Wang 1,2 , Ligang Shao 1 , Jiajin Chen 1 , Guishi Wang 1 , Kun Liu 1 , Tu Tan 1 ,
Jiaoxu Mei 1 , Weidong Chen 3 and Xiaoming Gao 1, *
1 Anhui Institute of Optics and Fine Mechanics, Hefei Institutes of Physical Science, Chinese Academy of
Sciences, Anhui 230031, China; [email protected] (K.W.); [email protected] (L.S.);
[email protected] (J.C.); [email protected] (G.W.); [email protected] (K.L.); [email protected] (T.T.);
[email protected] (J.M.)
2 Science Island Branch of Graduate School, University of Science and Technology of China,
Anhui 230031, China
3 Laboratoire de Physicochimie de l’Atmosphère, Université du Littoral Côte d’Opale, 189A, Av. Maurice
Schumann, 59140 Dunkerque, France; [email protected]
* Correspondence: [email protected]




Received: 19 September 2020; Accepted: 28 October 2020; Published: 30 October 2020


Abstract: In this article, a compact dual-laser sensor based on an off-axis integrated-cavity output
spectroscopy and time-division multiplexing method is reported. A complete dual-channel optical
structure is developed and integrated on an optical cavity, which allows two distributed feedback
(DFB) lasers operating at wavelengths of 1603 nm and 1651 nm to measure the concentration of CO2
and CH4 , simultaneously. Performances of the dual-laser sensor are experimentally evaluated by
using standard air (with a mixture of CO2 and CH4 ). The limit of detection (LoD) is 0.271 ppm and
1.743 ppb at a 20 s for CO2 and CH4 , respectively, and the noise equivalent absorption sensitivities
are 2.68 × 10−10 cm−1 Hz−1/2 and 3.88 × 10−10 cm−1 Hz−1/2 , respectively. Together with a commercial
instrument, the dual-laser sensor is used to measure CO2 and CH4 concentration over 120 h and
verify the regular operation of the sensor for the detection of ambient air. Furthermore, a first-order
exponential moving average algorithm is implemented as an effective digital filtering method to
estimate the gas concentration.

Keywords: OA-ICOS; dual-laser sensor; time-division multiplexing; carbon dioxide; methane

1. Introduction
Off-axis integrated cavity output spectroscopy (OA-ICOS) is a powerful spectroscopy technology
for gas detection owing to advantages including fast response, high sensitivity and stability [1–4].
Briefly, OA-ICOS employs a high-finesse optical cavity as an absorption cell that consists of two
high-reflectivity mirrors (>99.9%), and continuous-wave laser beams that are coupled into the cavity
at an angle and are bounced up to thousands of times to reach a long effective path length, which
delivers sensitivity down to parts per trillion and parts per billion [5–7]. In traditional OA-ICOS
approaches, researchers have generally used single laser sources to measure gas concentration or
isotopes [8–11]. Although these “single-laser-source” OA-ICOS approaches can be applied to most
detection experiments, they still cannot achieve the demand of simultaneous multi-gas measurements,
especially, for a near-infrared narrow linewidth laser, which is one grand challenge for multi-gas
measurement in different wavelength ranges.

Sensors 2020, 20, 6192; doi:10.3390/s20216192 www.mdpi.com/journal/sensors

Sensors 2020, 20, 6192 2 of 11

In recent years, with the gradual development of OA-ICOS [12,13], there have been two main
methods of simultaneous multi-gas detections using dual laser sources: frequency division multiplexing
assisted wavelength modulation spectroscopy (FDM-WMS) and time-division multiplexing assisted
direct absorption spectroscopy (TDM-DAS). Zheng et al. [14] developed a near-infrared CH4 and
C2 H6 OA-ICOS sensor system at parts per billion (ppb) concentration levels by using two distributed
feedback (DFB) lasers and combining FDM-WMS. This dual-gas sensor architecture shows the
advantages of simultaneous C2 H2 /CH4 detection with a single sensor system of reduced size, without
affecting sensitivity and reliability. In addition, there are other advantages of wavelength modulation
spectroscopy technology (WMS) of FDM-WMS, such as, harmonic detection, near-zero background,
zero-absorption baseline and suppression of the 1/f noise [15,16]. However, compared to direct
absorption spectroscopy technology (DAS) of TDM-DAS, the analysis of WMS absorption is more
complex [17]. While, DAS technology has an important position in the field of detection for its relatively
simpler data interpretation and implementation [18,19]. At the same time, DAS technology is also
widely used to investigate the spectroscopic parameters [20,21]. In addition, for “dual-laser-sources”
OA-ICOS sensors based on TDM-DAS, with the need for a single cavity and a single photodetector
and without a hardware lock-in amplifier, the cost of the sensors can be reduced.
In this paper, we set up a compact dual-laser OA-ICOS sensor combining TDM-DAS. The sensor
adopts two narrow linewidth DFB lasers operating at wavelengths of 1603 nm and 1651 nm for
simultaneously measuring the concentration of CO2 and CH4 . A complete dual-channel optical
structure is integrated in the cavity, which allows the sensor to tolerate a very high degree of mechanical
vibration. The sensor performances were evaluated by a standard air (with a mixture of CO2 and
CH4 ). Together with a commercial instrument, the sensor was used to measure ambient CO2 and
CH4 concentrations over 120 h. Furthermore, a first-order exponential moving average (EMA) was
implemented, which provides an effective digital filtering method to estimate the gas concentration.

2. Experimental Design and Methods

2.1. The Dual-Laser OA-ICOS Sensor Setup

A compact optical sub-system was designed for coupling the dual laser beam into an optical cavity
and delivering the output to a photodetector, as exhibited in Figure 1a. A pair of 1”-diameter spherical
mirrors (advanced thin films) with a curvature radius of 1000 mm and a reflectivity R≈ 99.996% were
used to form an optical resonator cavity. The two mirrors were placed co-axially on both sides of
a stainless steel tube, the distance between the mirrors was 28 cm and the inner tube diameter was
20 mm (volume of the tube, 88 cm3 ).
The outside of the optical cavity contains two optical cage systems (30 mm, Thorlabs, Newton,
NJ, USA) by using eight rigid steel rods to mount all optical components along the optical cavity axis.
The right system was an output cage system including a focusing lens with a focal length of 10 mm
and an InGaAs photodiode (Thorlabs, FGA 10) detecting the light transmitted from the optical cavity.
The left system was an input cage system, which allowed the dual-channel lasers to be injected in
the optical cavity, simultaneously. The input cage system mainly contains a cage plate (shown as
“Dual-channel collimator” in Figure 1a) with a circular-cross structure, which allows the lasers to be
placed off-axis. In this way the lasers are coupled “off-axis” into the optical cavity at an angle with
respect to the optical axis of the optical cavity. Two adjustable home-made collimators that provide
the angle of ±5◦ tip/tilt along the optical axis were placed on the left and bottom of the cage plate.
In addition, the positions of the collimators are not fixed, and they can be placed on any side of the
cage plate. Furthermore, the circular-cross structure of the cage plate maximally reduces the physical
squeeze and collision between the two collimators, and allows the collimators to be integrated more
easily. So, this design is very user-friendly and suitable for the dual-laser OA-ICOS sensor.
Sensors 2020, 20, 6192 3 of 11

Figure 1. (a) A designed cavity including integrated light path and dual-channel incident structure.
(b) Schematic diagram of the dual-laser off-axis integrated cavity output spectroscopy (OA-ICOS) sensor.
PS: pressure sensor, FL: focusing lens, PD: photodetector, GF: gas filter, PV1 and PV2: proportional
valve, PT: pressure–temperature.

Combining the structure of the portable optical sub-system, the dual-laser OA-ICOS sensor
designed is depicted in Figure 1b. The home-made laser drivers, which integrated with the temperature
controllers and current drivers, were used for driving the lasers. An NI card (National Instruments, NI
6353, Austin, TX, USA), integrated with the analog output (AO) and analog input (AI) functions, was
applied as a function generator and data acquisition card. A radio frequency (RF) white noise source
(Shenzhen Dakofeng Techno logy Co., Ltd., Shenzhen, China, NF-1000, output frequency range of
5 MHz–1.5 GHz) with a power of −20 dBm was used to broaden the laser linewidth [22,23]. Typically,
−
by broadening the laser linewidth wider than the cavity free spectral range (FSR) by injecting white
−
noise to the laser current, the spurious coupling of the longitudinal cavity modes can be reduced,
and the signal-to-noise ratio (SNR) can be increased − [24]. A temperature control box was added
−
to provide a stable working temperature for optical detection. The surrounding air in the box was
heated by a heating plate, a home-made radiator, and two home-made fans. The temperature and
pressure−in the box were controlled and stabilized by a home-made PT card (pressure–temperature
−
card), a temperature −
sensor (Heraeus, M222 PT1000, Hanau, Germany), a pressure sensor (MEAS,
US266-000006-005PA, Hampton, VA, USA) and two proportional valves (Clippard, − −
ET-PM-10-4025,
Cincinnati, OH, USA).
−
2.2. Selection of CO2 and CH4−Absorption Lines
The 1603.2 nm DFB laser (NEL, NLK1L5EAAA, Oslo, Norway) and the 1651 nm DFB laser (NEL,
NLK1U5FAAA) were placed on the “Dual-channel collimator” cage plate and were used to detect the
CO2 and CH4 concentration, respectively. According to the above method, the optical path lengths of
the cavity are 5.5 km (@1603 nm, CO2 ) and 8.5 km (@1651 nm, CH4 ), so three transmission spectra of
438.6 ppm CO2 , 1892.2 ppb CH4 and 2% H2 O in the spectral region from 6238.3 to 6239.2 cm−1 and
6056.8 to 6058 cm−1 , respectively, were simulated using the HITRAN 2016 database. As shown in
Figure 2a, the absorption line located at 6238.78 cm−1 for high-precision detection of CO2 was selected
due to its large absorption strength of 1.75 × 10−23 cm/molecule at a temperature of 296 K. Furthermore,
Sensors 2020, 20, 6192 4 of 11

its absorbance can be up to two orders of magnitude higher than the red line of 2% H2 O (line strength,
1.23 × 10−26 cm/molecule) in the nearby waveband. The CH4 absorption lines (three overlapping
lines) near 6057.09 cm−1 , whose full strength is 3.25 × 10−21 cm/molecule at a temperature of 296 K,
are plotted in Figure 2c. Their distance from the red line of H2 O (wavenumber, 6057.796 cm−1 ) is
0.705 cm−1 . At the same time, the linear relationship between the lasers emitting wavenumber and
driving current is shown in Figure 2b,d, the current range was decided to be 75−110 mA to scan
the CO2 line, and the range was decided to be 44−105 mA to simultaneously scan CH4 lines (three
overlapping lines) and H2 O lines.

0.4
438ppm,CO2,140Torr,5.5km
(a)
2%,H2O,140Torr,5.5km

0.3
Absorbance
-ln(I/I0)

0.008
0.2

0.1

6239.07 6239.10
0.0
110
(b)
6238.78cm-1
Current (mA)

100 91.6mA
Laser

90 6239.89cm-1
79.2mA
80
Emission at 24℃
70
6238.4 6238.6 6238.8 6239.0 6239.2
Wavenumber (cm-1)

0.3
1892ppb,CH4,140Torr,8.5km
2% H2O,140Torr,8.5km
(c)

0.2
-ln(I/I0)

0.1

0.0
105 6058.79cm-1 (d)
87.6mA
Current (mA)

90

75 6057.79cm-1
55.2mA
60

45
Emission at 18.5℃

6056.6 6056.8 6057.0 6057.2 6057.4 6057.6 6057.8 6058.0

Wavenumber (cm-1)

Figure 2. (a) HITRAN based absorption spectra of CO2 and H2 O (b) Plot of the CO2 laser emission
wavenumber as a function of the laser drive current. (c) HITRAN based absorption spectra of CH4 and
H2 O (d) Plot of the CH4 laser emission wavenumber as a function of the laser drive current.

2.3. Time-Division Multiplexing Method in the Dual-Laser OA-ICOS Sensor

In order to achieve the purpose of simultaneous detection, a time-division multiplexing method
was proposed. Figure 3 (a)
shows the scanning signal of two lasers and time sequence of the system. On a
scan periodicity T, T1 is the scanning range of the laser1 and T2 is the scanning range of the laser2,
which cover the absorption line of CO2 and the absorption line of CH4 , respectively. “T2 +∆T” is a
Laser1 scan
direct current output of laser1 and “T1 +∆T” T1 is a direct current output of laser2, which ensure each

scanning range of the lasers was staggered without interference. In this way, the laser beams can
be simultaneously coupled into the cavity and acquired by the photodetector. Figure 4 depicts the
time-division multiplexing
Laser2method
scan which is used to detect the actual output signals of the photodetector.
T2
ΔT
As shown in Figure 4, the method can be perfectly applied ΔT to the dual-laser OA-ICOS sensor without
the problem of superposition of laser intensity.
T
trigger

Δ
 Wavenumber (cm )

Sensors 2020, 20, 6192 5 of 11

(a)

Laser1 scan
T1

Laser2 scan
T2
ΔT ΔT

T
trigger

Figure 3. The scanning signal of two lasers and time sequence of the time division multiplexing method.
T: periodicity, T1 : CO2 spectral region, T2 : CH4 spectral region, ∆T: dark current of the detector.

Δ
1.2
Output signal

1.0

0.8
Intensity (V)

0.6
CH4
CO2 H2O
0.4

0.2

0.0
0 1000 2000 3000 4000 5000 6000
Number

Figure 4. Plot the actual CO2 and CH4 output signals of the photodetector based on the time division
multiplexing method, where bule dash circle represents the CO2 absorption line, and red dash circle
represents the CH4 absorption line.

2.4. Performance Optimization Using Exponential Moving Average

For the dual-laser OA-ICOS sensor, it is highly desirable to be able to perform real-time
concentration measurements with high precision, while the main factors limiting measurement
precision are the presence of system noises. These noises from practical measurements enable
researchers to use various digital processing methods [25–28] to estimate the gas concentration.
The exponential moving average (EMA) algorithm [29,30], as an effective digital filtering method, can
filter these noises and increase the precision of the OA-ICOS
– sensor.
The EMA can be defined as a linear transformation of raw concentration to a filtered concentration.
Let xt be the raw concentration at time t and x′ t be the filtered concentration at the same time, the
equation can be written as follow:

2 2 ′
 
x′ t = 1 − x′ t−1 + xt (N ≥ 1) (1)
N+1 N+1

where N is length of concentration 2 when N =2 1, the EMA is the identity transformation:

 samples,
1
x′ t = xt . Note that the length of concentration samples
1 (
N is important, 1)
because as a filter parameter, it
 1 1
determines the final filtered concentration of the OA-ICOS sensor. For a small N value, the precision
of the filtered concentration is not high, but the sensor’s response time is shorter to follow real-time
′
Sensors 2020, 20, 6192 6 of 11

variation. Conversely, the filtered concentration is more efficient in removing shot-to-shot real-time
noises when a large N is used, but the sensor’s response time is longer.
Figure 5a shows the concentration of two standard CH4 gases (1847.2 ppb and 1861.6 ppb) over a
time period of ~40 min, with a measurement interval of 20 s. The concentration inversion method
for determining the concentration has been given in Section 3.2. The blue triangle curve and the red
circular curve represent the filtered concentration of N = 4 and N = 19, respectively. Response time is
determined by the concentration decreasing from 1860.35 ppb to 1848.64 ppb (orange rectangular area),
which is 90% and 10% of the difference between the two concentrations, respectively. Figure 5b shows
the relationship between N versus the standard deviation of the measurement of 1861.6 ppb CH4 gas
(black curve) and the sensor’s response time (blue curve). It can be seen that the standard deviation
decreases exponentially with increased N, and the response time increases linearly with increased N,
meanwhile, for the OA-ICOS sensor, a value of N = 10 (a quarter of the standard deviation of the raw
concentration) was chosen as a compromise between the fast temporal response and the high filtering
efficiency. Note that the different concentrations’ standard deviations and the different response time,
affect the selection of N, thus the experimental conditions were needed to analyze specifically.

1864 800 0.75

(a) Raw data
N=4
(b)
N = 19 700
1860 0.6
1860.35 ppb (90 %)

Standard deviation 1σ (ppb)

600
CH4 concentration (ppb)

Response time (s)

500
1856 0.45

400

1852 0.3
300

200
1848 0.15
1848.64 ppb (10 %) 100

1844 0 0
0 10 20 30 40 0 10 20 30 40
Time (min) N

Figure 5. (a) Plots of the concentration in 1861.6 ppb and 1847.2 ppb CH4 gases, and the two filtering
results calculated by the exponential moving average (EMA) algorithm. (b) Response time (blue) and
standard deviation (black).

3. Results and Discussion

3.1. The Stability of Temperature and Pressure

In the practical atmospheric measurement, ambient air has a large temperature difference between
day and night, such broad temperature changes have a significant impact on the line-strength of the
absorption line. In addition, pressure changes also have a significant impact on the linewidth of the
absorption line. Therefore, for high precision optical detection, it is necessary to ensure a constant
temperature and constant pressure. The data for the target temperature in the cavity stabilized at 318 K
(45 ◦ C) and the target pressure stabilized at 140 Torr; recorded in the room-temperature laboratory, with
a measurement interval of 1s. Over an 18 h period of continuous measurement, without additional
calibration, the standard deviation 1σ was 0.37 mK, the long-term fluctuation value of the temperature
was 3 mK and plotted in Figure 6a. The gas-flow of 100 sccm, controlled by a precision gas flow-meter
(Beijng Sevenstar Flow Co., Ltd. D07-19B, Beijing, China), at the gas-inlet of the sensor by the gas
flow-meter to ensure stable gas. As shown in Figure 6b, the standard deviation 1δ was 0.005 Torr, and
the long-term fluctuation value of the pressure was 0.04 Torr.
Sensors 2020, 20, 6192 7 of 11

318.0020 140.03
(a) (b)
318.0015 Long-term fluctuation：3 mK Long-term fluctuation：0.04 Torr
140.02
318.0010
Temperature (K)

140.01

Pressure (Torr)
318.0005

318.0000
140.00

317.9995
139.99
317.9990

317.9985 139.98
Standard deviation：1δ=0.37 mK Standard deviation：1δ=0.005 Torr
317.9980
139.97
0 3 6 9 12 15 18 0 3 6 9 12 15 18
Time (h) Time (h)

Figure 6. Measurements of temperature (a) and pressure (b) over an 18 h period of continuous measurement.

3.2. Calibration
The dual-laser OA-ICOS sensor was used for the quantitative detections of CO2 and CH4
concentrations. Twelve CO2 samples with a concentration range of 50−1200 ppm were prepared by
a gas mixing system (Environics. Inc, Series 4000) via diluting a standard 2000 ppm CO2 with pure
nitrogen N2 . By using the same gas mixing system, thirteen CH4 samples with a concentration range
of 800−2300 ppb were prepared via diluting a standard 2300 ppb CH4 with pure nitrogen N2 . In order
to ensure that the pressure and temperature in the calibration are consistent with the pressure and
temperature in the practical atmospheric measurement, the target pressure and target temperature in
the optical cavity were also controlled at 140 Torr, and 45 ◦ C, respectively. The X-axis is the peak height
from the spectral fit and the Y-axis is the expected concentration.
Figure 7a shows the evolution of the CO2 concentration with the absorption term (I0 /I − 1), where
I0 is the incident laser intensity, and I is the output intensity of the cavity. A linear fitting equation was
obtained with a correlation coefficient R2 = 0.99939:
I0
 
χCO2 = 1396.86098 − 24.45397 × −1 (2)
I

1200
(a) Measure data
2400
(b) Measure data
Linear fitting Linear fitting
2200

1000 2000
CO2 Concentration (ppm)

CH4 Concentration (ppb)

1800
800

1600
600
1400

400 1200

1000
200
800
0
0.0 0.2 0.4 0.6 0.8 0.135 0.18 0.225 0.27 0.315 0.36 0.405
Peak Height Peak Height

Figure 7. Correlation between CO2 (a) and CH4 (b) concentration and peak height (I0 /I − 1) of absorption
spectra (from spectral fit). −
Sensors 2020, 20, 6192 8 of 11

Figure 7b shows the evolution of the CH4 concentration with the absorption term (I0 /I − 1).
A linear fitting equation was obtained with a correlation coefficient R2 = 0.99989:

I0
 
χCH4 = 61.41737 + 5468.19325 × −1 (3)
I

3.3. Long-Term Stability

With a measurement interval of ~20s, spectra of the synthesized air sample (with a mixture of
438.6 ppm CO2 and 1992.2 ppb CH4 ) were recorded for ~18 h to evaluate the measurement precision
linked to the fluctuation in the measured concentration. The long-term fluctuation range in the CO2
concentration was 437.84–439.49 ppm during the whole measurement procedure. In order to further
improve the measurement precision, the data of the concentration was processed in real-time using the
EMA algorithm. The long-term fluctuation range of CO2 -EMA reached 438.35–438.97 ppm, plotted in
Figure 8a. Similarly, the long-term fluctuation range in the CH4 concentration was 1986.89–1998.08 ppb,
and down to 1990.72–1994.58 ppb by using the EMA algorithm, as plotted in Figure 8c. Furthermore,
the raw long-term 1δ of CO2 and CH4 was 0.278 ppm and 1.794 ppb and the EMA long-term 1δ of CO2
and CH4 was 0.107 ppm and 0.733 ppb, as shown in Table 1.

(a)
CH4 Concentration (ppb)
CO2 Concentration (ppm)

440.3 Raw data

EMA data 2000
(c) Raw data
EMA data
439.6
1996
438.9
1992
438.2

437.5 1988

1984
0 3 6 9 12 15 18 0 3 6 9 12 15 18
Time (h) Time (h)
Allan deviation
(d)
Allan Deviation (ppm)

Allan deviation
(b)
Allan Deviation (ppb)

0.271ppm@20s 1.743ppb@20s

0.1

0.047ppm@1240s 0.224ppb@1660s
10 100 1000 10 100 1000
Time (s) Time (s)

Figure 8. (a) The long-term concentration measurement of CO2 and its EMA algorithm result. (b) Allan
deviation analysis of the CO2 data. (c) The long-term concentration measurement of CH4 and its EMA
algorithm result. (d) Allan deviation analysis of the CH4 data.

Table 1. The long-term 1δ of CO2 and CH4.

Raw Long-Term 1δ EMA Long-Term 1δ

CO2 0.278 ppm 0.107 ppm
CH4 1.794 ppb 0.733 ppb

The stability and the detection limits of the dual-laser OA-ICOS sensor can conveniently be Allan
deviation. The Allan figure can provide information about an optimum averaging time and a limit of
detection (LoD) [31]. Thus, Allan deviation analysis was implemented on the raw data of CO2 and
CH4 to characterize the stability, as plotted in a log–log scale versus the averaging time in Figure 8b,d,
respectively. The LoD of 0.271 ppm for a 20 s averaging time, and a minimum LoD of 0.047 ppm for
an optimum averaging time of 1240 s were obtained based on the analysis of the CO2 concentration.
Similarly, For the CH4 concentration, a LoD of 1.743 ppb for a 20s averaging time and a minimum LoD
of 0.224 ppb for an optimum averaging time of 1660 s were obtained. Using the method described by
Baer et al. [32], the detection bandwidths of CO2 and CH4 were 2.65 Hz (fcavity_CO2 =8.5 kHz, 3200
sweeps averaged) and 1.75 Hz (fcavity_CH4 =5.6 kHz, 3200 sweeps averaged), respectively. Noise
equivalent absorption sensitivities (NEAS) of the CO2 and CH4 for a 20 s averaging time were 2.68 ×
10−10 cm−1 Hz−1/2 and 3.88 × 10−10 cm−1 Hz−1/2 , respectively.
Sensors 2020, 20, 6192 9 of 11

3.4. Detection of Ambient Air with the Dual-Laser OA-ICOS Sensor

Figure 9 depicts the performance of the dual-laser OA-ICOS sensor that is demonstrated with gas
concentration measurements in ambient air. A commercial instrument (Thermo Scientific model 5900)
was applied to ambient air measurements as well for side-by-side intercomparison. This instrument
mainly uses meteorological chromatography technology to detect methane and non-methane total
hydrocarbons, so unfortunately, it is impossible to compare the results of carbon dioxide detection.
The entire measurements were performed over a time period of ~120 h with a measurement interval
of ~120 s. Furthermore, these two instruments were used in a designated meteorological station
located in Zibo City, Shandong Province, China. The black solid line represents the CH4 concentration
result detected by the commercial instrument, and the red solid line represents the CH4 concentration
detected by the dual-laser sensor. The measurement trends of the two instruments are well consistent
for the 120 h measurement time. It is proved that the dual-laser sensor has a practical engineering
value for the ambient air measurement of gas concentration.
CO2 Concentration (ppm)

480 (a) The dual-laser sensor

456

432

408

384

360
2800
(b)
CH4 Concentration (ppb)

Thermo model 5900

2600 The dual-laser sensor

2400

2200

2000

1800

1600
0 20 40 60 80 100 120
Time (h)

Figure 9. (a) The ambient air measurement of carbon dioxide over 120 h. (b) The ambient air
measurement of methane over 120 h.

4. Conclusions
A compact dual-laser sensor based on OA-ICOS and the time-division multiplexing method was
developed in this article. A complete dual-channel optical structure was developed and integrated in
the cavity, which allows two DFB lasers operating at wavelengths of 1603 nm and 1651 nm to measure
the concentration of CO2 and CH4 , simultaneously. The sensor performances were evaluated by a
standard air (with a mixture of CO2 and CH4 ). A limit of detection (LoD) was 0.271 ppm and 1.743 ppb
at a 20 s, for CO2 and CH4 , respectively, and the noise equivalent absorption sensitivity was 2.68 ×
10−10 cm−1 Hz−1/2 and 3.88 × 10−10 cm−1 Hz−1/2 , respectively. Together with a commercial instrument,
the sensor was used to measure the CO2 and CH4 concentration over 120 h and verify the regular
operation
− − of the
− sensor for the− detection
− −of ambient air. Furthermore, the first-order exponential

moving average algorithm is implemented to provide an effective digital filtering method to estimate
the gas concentration.

Author Contributions: Conceptualization, K.W. and L.S.; methodology, K.W. and K.L.; software, K.W.; validation,
J.C.; formal analysis, K.W. and G.W.; investigation, K.W. and G.W.; resources, T.T. and J.M.; data curation, K.W.
and G.W.; writing—original draft preparation, K.W.; writing—review and editing, W.C.; visualization, K.W.;
supervision, X.G.; project administration, X.G.; funding acquisition, X.G. and K.L. All authors have read and
agreed to the published version of the manuscript.
Sensors 2020, 20, 6192 10 of 11

Funding: National Key Research and Development Program of China (2016YFC0303900 and 2017YFC0209700);
National Natural Science Foundation of China (NSFC) (41730103).
Conflicts of Interest: The authors declare no conflict of interest.

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