Development of an automated diode-laser-based

multicomponent gas sensor

Dirk Richter, David G. Lancaster, and Frank K. Tittel

The implementation and application of a portable fiber-coupled trace-gas sensor for the detection of
several trace gases, including CO2, CH4, and H2CO, are reported. This particular sensor is based on a
cw fiber-amplified near-infrared distributed Bragg reflector diode laser and an external cavity diode
laser that are frequency converted in a periodically poled lithium niobate crystal to the mid-IR spectroscopic fingerprint region 3.3 4.4 m. A continuous absorption spectrum of CH4 and H2CO from 3.37
to 3.70 m with a spectral resolution of 40 MHz 0.0013 cm1 demonstrated the spectral performance
that can be achieved by means of automated wavelength tuning and phase matching with stepper motor
control. Autonomous long-term detection of ambient CO2 and CH4 over a 3- and 7-day period was also
demonstrated. 2000 Optical Society of America
OCIS codes: 190.2620, 300.6340.

1. Introduction

The spectroscopic detection and quantification of numerous trace-gas species has become an important
aspect in many industrial, urban, and environmental
applications. More importantly, there is a need to
selectively detect several different molecular gas species simultaneously by means of a single, tunable,
and portable sensing device capable of high sensitivity and rapid response time.
Characteristic absorption bands of most molecules
can be found in the near-infrared overtone and midinfrared fundamental rovibrational spectral region.
The latter range has the advantage that the spectrum
is less congested and exhibits 20 200 times stronger absorption cross sections. Established techniques for multicomponent gas analysis include
nonlaser-based Fourier-transform infrared spectrometers that can rapidly cover a broad spectrum 1 s
with a typical resolution of 15 GHz.1 For highly
selective 50-MHz absorption spectroscopy of trace
gases, various narrow-linewidth laser sources are
used in the mid-IR, including cw cyrogenically cooled
leadsalt diode lasers2 4 and, more recently, cw and

The authors are with the Rice Quantum Institute, Rice University, Houston, Texas 77251-1892. The e-mail address for F. K.
Tittel is [email protected].
Received 4 January 2000; revised manuscript received 24 May
2000.
0003-693500244444-07$15.000
2000 Optical Society of America
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APPLIED OPTICS Vol. 39, No. 24 20 August 2000

pulsed quantum cascade lasers.5 In the near-IR

spectral region, room-temperature operation of cw
single or multisection distributed feedback InGaAsP
diode lasers can be applied to overtone absorption
spectroscopy.6 An alternative, narrow-linewidth
mid-IR spectroscopic source that has been applied
successfully to trace-gas detection is based on
difference-frequency generation DFG of two near-IR
diode lasers in a nonlinear optical material such as
periodically poled lithium niobate PPLN.79
In this paper we describe the development and
application of an automated mid-IR diode-laserpumped DFG-based trace-gas sensor source that offers wide tunability from 3.3 to 4.4 m and a spectral
selectivity of 40 MHz. A fiber-coupled tunable
near-IR external cavity diode laser ECDL 814 870
nm and a Yb-fiber-amplified distributed Bragg reflector DBR diode-laser 1083 nm are used as DFG
pump sources. The two pump lasers are differencefrequency mixed in a fan-out-type PPLN crystal that
offers high optical conversion efficiency, broad spectral transmission 0.35.3 m, and continuous
quasi-phase matching. This sensor uses extractive,
direct absorption spectroscopy at a reduced pressure
80 Torr in a multiple-pass absorption cell fitted
with astigmatic mirrors 18 or 36 m.10 Several
gases including CH4, CO2, H35,37Cl, H2CO, N2O,
NO2, CH3OH, and C6H6 have been detected to date
within the tuning range of this DFG-based gas sensor. Spectral tuning and quasi-phase matching by
means of stepper motors are controlled by LabView
software operating on a laptop PC and interfaced

Fig. 1. Schematic of an automated DFG multicomponent gas sensor. M1, M2, and M3 are stepper motors for the ECDL, PPLN crystal
stage, and reference gas assembly, respectively. WDM, wavelength division multiplexer; DL, diode laser; CTRL, control.

with serial ports. Furthermore, the fast measurement response time of typically 510 s, including averaging and automated data processing, allows the
real-time monitoring of in situ and remote chemical
and atmospheric trace-gas species.
2. Gas Sensor Configuration

The gas sensor developed for field operation utilizes

both a fiber-pigtailed, widely tunable 25-mW ECDL
operating at a center wavelength of 842 28 nm and
a fiber-pigtailed 50-mW DBR diode laser operating at
a 1083-nm wavelength see Fig. 1. Continuous,
mode-hop-free tuning of the Littman-type ECDL is
selected by simultaneous rotation and translational
movement of the internal feedback mirror about a
pivot point with respect to the grating by means of a
linear translation stage.11 This linear translation
stage was modified to implement a stepper motor and
was operated by use of a compact computercontrolled driver. The fiber-coupled output power of
15 mW from the DBR diode laser was amplified to
600 mW by a side-pumped Yb fiber amplifier using a
2-W diode laser at 975 nm.12,13 Both ECDL and amplified DBR diode-laser fiber-coupled beams pass
through polarization controllers before being combined by use of a four-port fiber coupler. Two percent of the combined beam power was connected to a

second fiber coupler, separating the pump and signal

beams. Either optical fiber arm can be connected to
a wavemeter for absolute frequency calibration. For
convenience, the ECDL beam was monitored continuously with the wavemeter precision: 0.01 cm1
at 1 m to provide absolute frequency tuning
information by a general-purpose interface bus
GPIB Personal Computer Memory Card International Association PCMCIA interface. Alternatively, a solid etalon in combination with a silicon
photodiode could be used as a relative wavelength
tuning reference.14 The other 98% are terminated
in an 8-deg angle-polished fiber connector and
mounted onto a ruggedized DFG conversion stage.
This stage contains the optical elements and optomechanical mounts that are pertinent to achieve widely
tunable DFG, including a fiber port, imaging lens,
PPLN crystal, and a CaF2 lens. We imaged the collinear pump beams from the fiber tip into the
temperature-controlled antireflection-coated PPLN
crystal using an f 10-mm achromatic lens. A kinematic optical mount with vertical translation and
tilt is used to align the crystal to the beam propagation axis. This mount is also controlled by a steppermotor-driven linear translation stage to provide the
optimal quasi-phase-matching grating period. The
dialing position is computed from an experimentally
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4445

Fig. 2. Diagram of the electronic control and data-acquisition system for the DFG-based multicomponent gas sensor. DAQ, data
acquisition; TEC, thermoelectric cooler.

recorded phase-matching function. Both the singlemode fiber-launched pump and the signal beams possess Gaussian beam profiles, and when mixed in a
19-mm-long PPLN crystal they produce a diffractionlimited mid-IR DFG beam of 2.9-W power at
3.5-m wavelength.8 The DFG beam is then collimated by use of an f 50-mm CaF2 lens, passing
through a Ge filter to block the unconverted pump
beams and directed to a multipass cell physical
length, 30 cm; actual path length, 18 or 36 m.10
The sensor operated with a typical sensitivity of 2
104 limited by the occurrence of etalon effects introduced by the optical elements. For convenient identification and tracking specific absorption line center
positions within the scan width, up to five individual
reference gas cells L 5 cm can be rotated into the
DFG beam path by a stepper-motor-driven assembly.
The sensor is also operated and controlled with a
LabView software code running on the laptop PC.
Figure 2 shows the electronic diagram of the gas
sensor. Both stepper motor controllers are interfaced to the laptop PC by a universal serial bus port.
A 16-bit PCMCIA data-acquisition card is used to
acquire the absorption signal synchronized to a trigger signal, the gas sampling pressure, and temperature. The card also controls a shutter through a
digital transistortransistor logic line for background
light subtraction that is necessary for an absolute
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APPLIED OPTICS Vol. 39, No. 24 20 August 2000

spectroscopic absorption measurement. The entire

sensor, including both optical and electronic elements, is packaged into a suitcase with outside dimensions of 61 cm 53 cm 20 cm. An additional
small suitcase 30 cm 25 cm 14 cm contains a
diaphragm pump and a mass-flow controller that are
used for extractive gas sampling at reduced pressure
for optimum spectral selectivity and sensitivity.
3. Wavelength Tuning and Quasi-Phase-Matching
Characteristics

The wavelength tuning curve for the Littman-type

external cavity pump laser as a function of the stepper motor rotation dial position is shown in Fig. 3.
A miniature coupler from the stepper motor shaft to
the ECDL tuning screw was used. This coupler permitted angular, radial, and lateral misalignment of
the stepper motor shaft and therefore suppressed
stress to the ECDL tuning mechanism. The stepper
motor resolution was 13600 steps per revolution and
provided an experimentally measured linear ECDL
frequency tuning rate of 0.018 cm1step. The frequency tuning was superimposed by a sinusoidallike
modulation, corresponding to a peak deviation of 0.15
cm1 as can be seen from the inset of Fig. 3. This
inset also shows a residual backlash of 225 15 steps
inherent to the ECDL device used in this research.
Continuous quasi-phase matching over the entire

Fig. 3. ECDL frequency tuning characteristic with stepper motor

control.

tuning range of the sensor is achieved by use of a

PPLN crystal with a fan-out grating structure.15 In
this configuration the grating period continuously increases from 22.4 to 23.3 m over a 1-cm-wide crystal. Plotted in Fig. 4 is the relative crystal position
versus the DFG wavelength for two temperatures,
26 C and 44 C. The PPLN crystal temperature
can be set to match the available grating periods with
the ECDL wavelength tuning range, which for this
sensor is 44 C. For comparison, a multichannel
PPLN crystal common channel period spacing of 0.1
m requires a temperature adjustment to optimally
phase match intermediate wavelengths. For example, for a pumpsignalidler wavelength combination, which requires a grating period that lies
between two nominal PPLN crystal channel grating
periods of 0.1-m difference, a temperature adjustment of 15 C is necessary.8,16 The measured
PPLN phase-matching bandwidth is 28 cm1 Fig. 4.

Fig. 5. Measured absorption spectra of formaldehyde and methane over 270 cm1 centered at 2850 cm1. Estimated total pressure was 50 Torr 8% CH4 and 0.65% H2CO; absorption path
length was 5 cm.

This value can be compared with a theoretically computed phase-matching bandwidth of 12.5 cm1 at 3.6
m for normal-incidence nondiverging pump beams.
Similar to the ECDL stepper motor interface, a miniature joint coupling was used to connect to the PPLN
crystal linear translation stage Vernier set screw,
0.5-mm linear translation per revolution. In addition, a 48-pitch, 1:1 Miter gear was implemented to
realize a compact stepper motor arrangement with no
noticeable loss of precision.
The simultaneous computer control of wavelength
tuning and quasi-phase matching allows multispecies gas measurements within the instrument tuning
range from 3.3 to 4.4 m. For example, Fig. 5 shows
a continuous absorption spectra of methane CH4
and formaldehyde H2CO acquired over a 270-cm1-

Fig. 4. Continuous quasi-phase matching with a fan-out grating-type PPLN crystal.

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Fig. 6. Comparison of the relative frequency drift for a steppermotor-controlled and free-running ECDL operation as a function of
time.
Fig. 7. Ambient CO2 laboratory sampling over a 42-h time period.

wide tuning range from 2700 cm1 3.70 m to 2970

cm1 3.37 m with a DFG linewidth resolution of 40
MHz. We performed the measurement using a
5-cm-long reference gas cell containing 8% of CH4
and 0.65% of H2CO with an estimated total pressure
of 50 Torr. A 200-Hz current modulation of the DBR
diode laser provided an effective scanning width of
0.33 cm1. The ECDL was tuned consecutively by
an eight-step 0.15-cm1 increment to take into
account the above-mentioned sinusoidal offset. Absolute wavelength accuracy was provided by a
wavemeter. Each spectrum was averaged over five
scans 25 ms and subtracted by a five-scan average
dark voltage measurement to obtain absolute transmission. The recorded spectroscopic data files that
include an absorption scan, dark voltage scan, and
corresponding wavelength log were automatically
processed with a LabView software-programmed algorithm to connect the acquired spectra indicated by
the dashed circles in the inset of Fig. 5 and to remove
redundant data points of consecutive data scans.
Furthermore, a polynomial-fit algorithm can be applied to improve the baseline overlap of two consecutive scans.
Automated compensation of wavelength drift that
is due to temperature changes is a further advantage
of our using stepper-motor-controlled wavelength
tuning and quasi-phase matching. Critical components that are susceptible to temperature fluctuations include detector amplifier, diode-laser drivers,
temperature controllers, and, most significantly, the
wavelength stability of the ECDL. Figure 6 shows
an example of automated wavelength drift compensation by means of the two stepper motors. For this
measurement the absorption peak location of a CO2
transition line at 4.2 m was monitored after the
DFG-based gas sensor was moved from an outdoor to
an indoor environment with an ambient temperature
difference of 5 C. At the beginning of the measurement the absorption line was centered within the
absorption scan width of 0.32 cm1. We programmed the LabView software to compensate for
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APPLIED OPTICS Vol. 39, No. 24 20 August 2000

the drift of the absorption by appropriately wavelength tuning the ECDL if the peak location was
outside the programmed maximum and minimum
boundary conditions. For comparison, the total
wavelength drift that can occur if the gas sensor system is not actively controlled is also shown in Fig. 6.
4. Spectroscopic Evaluation of the
Difference-Frequency Generation-Based Gas Sensor

The DFG-based gas sensor was used in several longterm tests. In a first test, the sensor was tuned to a
CO2 line at 2385.77 cm1 4.2 m and monitored the
CO2 concentration in ambient laboratory air continuously at reduced pressure of 80 Torr for a 3-day
period as depicted in Fig. 7. The rovibrational CO2
absorption lines at 4.2 m have a frequency spacing
of 0.7 cm1 21 GHz. In this case, it is advantageous to perform spectroscopic absorption measurements of CO2 at a reduced sampling pressure to avoid
a zero baseline offset. The CO2 concentration increases and decreases rapidly, respectively, at times
with and without human activity in the laboratory as
shown in Fig. 7. The dynamic detection range at
this CO2 absorption line is 0.52200 parts per million
ppm 100% absorption at a pressure of 80 Torr for
an 18-m optical absorption path-length-configured
multipass cell and a residual optical noise of 2
104. After 2 h into the CO2 sampling test, human
breath was briefly sampled and caused a sharp increase to CO2 levels of more than 2200 ppm, saturating the absorption signal. However, it is possible to
tune the DFG wavelength to a weaker CO2 transition
to measure higher concentrations or to lower frequencies to access a stronger CO2 transition at 4.2 m
when low CO2 concentrations are measured. The
DFG-based gas sensor measured higher ambient
background levels than the atmospheric concentrations measured by the National Oceanic and Atmospheric Administration.17 This may be due to the
fact that the CO2 and other gas species concentration
levels tend to be higher in urban areas such as Houston, Texas.

Fig. 8. Continuous detection of ambient CH4 for a 7-day period.

In another long-term test, the DFG sensor was

tuned to a methane absorption line at 3028.751 cm1
3.3 m to monitor ambient air continuously for a
7-day period. The DFG-based gas sensor was located in an air-conditioned laboratory environment
with the sensor being located close to an airconditioner ventilation inlet. For this test, the multipass cell was aligned to a 36-m optical path
configuration for increased detection sensitivity.

Approximately 20 min into the test, the DFG-based

gas sensor was set to acquire a dark voltage before
and after each absorption scan and to compute an
average absorption value. This effectively reduces
the noise present in a CH4 measurement evident in
Fig. 8. Furthermore, one can see that the methane
concentration peaks around midnight and increased
to over 5000 parts per billion ppb after heavy rain
storms. These methane trends were confirmed to be
real by an intercomparison with another fibercoupled DFG-based gas sensor.18 At the bottom of
Fig. 8 the corresponding DFG output power signal is
plotted. A general drift of 0.03%h with a 1.3% standard deviation is measured, except of a few incidents
when a cooling fan attached to the Yb fiber amplifier
housing stopped operation. This effectively changed
the temperature-dependent pump diode wavelength
which resulted in a shift to a weaker absorption crosssection region of the Yb-doped fiber amplifier and led
to a reduced amplifier gain.
A second CH4 sensor, described in Ref. 18, was set
up in close vicinity and operated at the same DFG
wavelength and measured ambient laboratory air
with a 36-m open path-length multipass cell at atmospheric pressure. Figure 9 shows the superimposed
CH4 concentration measurements versus time plots
of the two independently operating DFG-based tracegas sensors over a 4-day period. Both sensors fol-

Fig. 9. Intercomparison of long-term CH4 concentration measurements by two independent DFG-based gas sensors indicating both CH4
concentrations and deviation in parts per billion.
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4449

lowed the same profile and measured the CH4

concentration with an average difference of 50 ppb
standard deviation, which is well within the accuracy of both instruments 5%. For calibration of the
DFG-based gas sensors, a calibrated gas mixture was
flown through the multipass cells.8 Using LabView
software, we first processed the absorption scans to
obtain a flat baseline, and then we fitted the absorption signal to a Lorentzian line-shape function using
a nonlinear least-squares LevenbergMarquardt fit.8
The obtained spectroscopic parameters also agree
with the HITRAN19 database. Furthermore, the
good agreement between atmospheric and low sampling pressure 88 Torr measurements indicates a
high spectral purity of the two DFG-based gas sensors and confirms the applicability of a Lorentzian
line-shape function.
5. Summary

We reported the development and application of a

portable, compact, widely tunable mid-IR DFG-based
gas sensor that can be operated automatically with
stepper motor wavelength tuning and continuous
PPLN quasi-phase matching. Fiber optics and
fiber-coupled diode-laser pump sources make such a
device suitable for nonlaboratory use of gas sensing
applications. Long-term monitoring of CO2 and
CH4 and the acquisition of a continuous CH4 and
H2CO absorption spectra over 270 cm1 further demonstrates the key advantages of this DFG-based gas
sensor, including robust long-term maintenance-free
operation and wide tunability for multicomponent
gas detection with high sensitivity, selectivity, and
real-time response.
To achieve better sensitivity, more power is required to apply advanced detection techniques such
as dual-beam detection to effectively cancel out the
occurrence of optical etalon effects.20 Potentially,
the same sensor architecture also can be used to access the second atmospheric window from 6 to 16 m
with orientation-patterned epitaxial-grown quasiphase-matched GaAs crystal for optical frequency
conversion.21
The authors acknowledge D. P. Leleux Rice University for the support and help in implementing the
stepper motor control hardware and software. Financial support was provided by NASA, the Texas
Advanced Technology Program, the Welch Foundation, the National Science Foundation, and the Gulf
Coast Hazardous Substance Research Center.
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