of 20
Atmos. Meas. Tech., 9, 3527–3546, 2016
www.atmos-meas-tech.net/9/3527/2016/
doi:10.5194/amt-9-3527-2016
© Author(s) 2016. CC Attribution 3.0 License.
Assessment of errors and biases in retrievals of X
CO
2
, X
CH
4
, X
CO
,
and X
N
2
O
from a 0.5 cm
1
resolution solar-viewing spectrometer
Jacob K. Hedelius
1
, Camille Viatte
2
, Debra Wunch
2,a
, Coleen M. Roehl
2
, Geoffrey C. Toon
3,2
, Jia Chen
4,b
,
Taylor Jones
4
, Steven C. Wofsy
4
, Jonathan E. Franklin
5,c
, Harrison Parker
6
, Manvendra K. Dubey
6
, and
Paul O. Wennberg
2
1
Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA, USA
2
Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA, USA
3
Jet Propulsion Laboratory, California Institute of Technology, Pasadena, CA, USA
4
School of Engineering and Applied Sciences and Department of Earth and Planetary Sciences,
Harvard University, Cambridge, MA, USA
5
Department of Physics & Atmospheric Science, Dalhousie University, Halifax, Nova Scotia, Canada
6
Earth and Environmental Sciences, Los Alamos National Laboratory, Los Alamos, NM, USA
a
now at: Department of Physics, University of Toronto, Toronto, Ontario, Canada
b
now at: Electrical and Computer Engineering, Technische Universität München, Munich, Germany
c
now at: School of Engineering and Applied Sciences and Department of Earth and Planetary Sciences,
Harvard University, Cambridge, MA, USA
Correspondence to:
Jacob K. Hedelius (jhedeliu@caltech.edu)
Received: 5 February 2016 – Published in Atmos. Meas. Tech. Discuss.: 4 March 2016
Revised: 24 June 2016 – Accepted: 28 June 2016 – Published: 3 August 2016
Abstract.
Bruker
EM27/SUN instruments are commer-
cial mobile solar-viewing near-IR spectrometers. They show
promise for expanding the global density of atmospheric col-
umn measurements of greenhouse gases and are being mar-
keted for such applications. They have been shown to mea-
sure the same variations of atmospheric gases within a day as
the high-resolution spectrometers of the Total Carbon Col-
umn Observing Network (TCCON). However, there is little
known about the long-term precision and uncertainty budgets
of EM27/SUN measurements. In this study, which includes
a comparison of 186 measurement days spanning 11 months,
we note that atmospheric variations of X
gas
within a single
day are well captured by these low-resolution instruments,
but over several months, the measurements drift noticeably.
We present comparisons between EM27/SUN instruments
and the TCCON using GGG as the retrieval algorithm. In ad-
dition, we perform several tests to evaluate the robustness of
the performance and determine the largest sources of errors
from these spectrometers. We include comparisons of X
CO
2
,
X
CH
4
, X
CO
, and X
N
2
O
. Specifically we note EM27/SUN bi-
ases for January 2015 of 0.03, 0.75,
0.12, and 2.43 % for
X
CO
2
, X
CH
4
, X
CO
, and X
N
2
O
respectively, with 1
σ
running
precisions of 0.08 and 0.06 % for X
CO
2
and X
CH
4
from mea-
surements in Pasadena. We also identify significant error
caused by nonlinear sensitivity when using an extended spec-
tral range detector used to measure CO and N
2
O.
1 Introduction
Measurements of atmospheric mixing ratios of greenhouse
gases (GHGs), including CO
2
and CH
4
, are needed to aid
in estimating fluxes and flux changes, and to ensure inter-
national treaties to reduce emissions are fulfilled. The To-
tal Carbon Column Observing Network (TCCON) makes
daytime column measurements of these gases. The Orbit-
ing Carbon Observatory2 (OCO-2) and Greenhouse Gases
Observing Satellite (GOSAT) missions enable column GHG
measurements with global coverage. These GHG monitoring
satellites make measurements at one time of day and, there-
fore, lack the temporal resolution that a dedicated ground site
provides.
Published by Copernicus Publications on behalf of the European Geosciences Union.
3528
J. K. Hedelius et al.: Assessment of errors in Xgas from a 0.5 cm
1
spectrometer
Due to cost, lack of infrastructure, and stringent network
requirements, there are limited ground sites on a global scale;
e.g., there are no TCCON sites currently in operation in con-
tinental Africa, South America, or central Asia (Wunch et al.,
2015), and there currently is no urban area with more than
one TCCON site. Cheaper, portable, solar-viewing Fourier
transform spectrometers (FTSs) can make contributions in
these settings provided they have long-term precision. The
Bruker Optics
EM27/SUN, with the “SUN” indicating a
built-in solar tracker, is a transportable FTS that may supple-
ment global GHG measurements made by current networks
(Gisi et al., 2012). This unit is small and stable enough to eas-
ily be transported for field campaign measurements, includ-
ing measurements at multiple locations in 1 day. Column-
averaged dry-air mole fractions (DMFs) of gases (X
gas
)
are
retrieved from the EM27/SUN measurement, like the TC-
CON. X
gas
is calculated from (Wunch et al., 2010):
X
gas
=
column
gas
column
dry air
=
0
.
2095
column
gas
column
O
2
,
(1)
where the 0.2095 factor is the fraction of dry air that is oxy-
gen.
Retrieved X
gas
has been compared with a co-located TC-
CON site in Karlsruhe, Germany, in past work for 26 days
of X
CO
2
retrievals from one EM27/SUN instrument (Gisi et
al., 2012), and 6 days of both X
CO
2
and X
CH
4
retrievals from
five EM27/SUN instruments (Frey et al., 2015).
Operators of these instruments have different end goals
to better understand the carbon cycle. X
CO
2
and X
CH
4
re-
trievals from these instruments have been compared with
satellite measurements in areas without a TCCON site (Klap-
penbach et al., 2015) as well as with satellite measurements
in highly polluted areas (Shiomi et al., 2015). Emission
flux estimates from the Berlin area (< 30
×
30 km
2
)
were
made by combining upwind/downwind measurements from
five spectrometers and were compared with a simulation
(Hase et al., 2015). Chen et al. (2016) have assessed gra-
dient strengths around a large dairy farm (
100 000 cows)
in Chino, California (< 12
×
12 km
2
)
, using measurements
from upwind/downwind spectrometers. Weather Research
and Forecast Large-Eddy Simulations (WRF-LES, 4 km res-
olution) were used in combination with four simultaneous
measurements to estimate fluxes from specific grid boxes in
a subregion of the Chino dairy farm area, which is within a
larger urban area (Viatte et al., 2016).
The column measurements used in these studies provide
some advantages over in situ measurements, including less
sensitivity to vertical exchange, surface dynamics, and small-
scale emissions (McKain et al., 2012), which are difficult to
model. Though column measurements can depend on mixed
layer height in highly polluted areas, generally, column mea-
surements depend primarily on regional-scale meteorology,
and regional fluxes (Wunch et al., 2011b; McKain et al.,
2012). For example, Lindenmaier et al. (2014) used obser-
vations from a single TCCON site to verify 1 day of emis-
sions from coal power plants of about 2000 MW each at
4
and 12 km away. Because of their large spatial sensitivity,
column measurements are well suited for estimation of net
emissions, model comparison, and satellite validation. A sin-
gle site has been used to estimate Los Angeles, California
(L.A.), emissions based on a sufficiently accurate emissions
inventory and the observation that X
gas
anomalies within
L.A. are highly correlated (Wunch et al., 2009, 2016). Gener-
ally though, a single column measurement site is insufficient
to estimate emissions from an entire urban region (Kort et
al., 2013). However, multiple column measurements can be
combined to characterize part or all of an urban area (Hase et
al., 2015; Chen et al., 2016; Viatte et al., 2016).
The main goal of this work is to quantitatively evaluate
the robustness of EM27/SUN retrievals over a long period
of time. This is accomplished by comparing retrievals from
the EM27/SUN with a co-located standard (TCCON site)
at Caltech, in Pasadena, California, United States. TCCON
spectrometers make the same type of measurements (direct
solar near-infrared) at high spectral resolution. Here we re-
port X
CO
2
, X
CH
4
, X
CO
, and X
N
2
O
comparison measurements
from an EM27/SUN. The X
CO
and X
N
2
O
measurements were
made possible by a detector with an extended spectral range
provided by Bruker
. The EM27/SUN X
CO
2
and X
CH
4
to
TCCON comparison is the longest to date, 186 measure-
ment days spanning 11 months. In part of January 2015,
an additional three EM27/SUN instruments were at Caltech
for 9 to 12 days of X
CO
2
and X
CH
4
comparisons to assess
their relative biases. In Sect. 2 we briefly describe differences
in instruments and the data acquisition process. In Sect. 3
we describe the retrieval software. In Sect. 4 we describe
the inherent properties of EM27/SUNs such as instrument
line shapes (ILSs), frequency shifts, ghosts, detector linear-
ity, and external mirror degradation. Section 5 focuses on bi-
ases and sounding precision of different gases compared with
the TCCON. Section 6 describes sources of instrumental er-
ror. We conclude with general recommendations of tests to
perform on any new type of direct solar near-infrared (IR)
instrument used to retrieve abundances of atmospheric con-
stituents.
2 Instrumentation
2.1 TCCON IFS 125HR
All TCCON sites employ the high-resolution Bruker
Optics
IR FT spectrometer (IFS) 125HR that has been
described in detail elsewhere (Washenfelder et al., 2006;
Wunch et al., 2011b). For the Caltech TCCON site
(34.1362
N, 118.1269
W, 237 m a.s.l.), the IFS 125HR uses
an extended InGaAs (indium gallium arsenide) detector,
covering 3800–11 000 cm
1
for detection and retrieval of
all gases relevant to this study (O
2
, CO
2
, CH
4
, CO, and
N
2
O). Figure 1 has example spectra from IFS 125HR and
Atmos. Meas. Tech., 9, 3527–3546, 2016
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J. K. Hedelius et al.: Assessment of errors in Xgas from a 0.5 cm
1
spectrometer
3529
4000
6000
8000
10 000
Frequency (cm
-1
)
Signal intensity (A.U.)
HF
CO
N
2
O
H
2
O
CH
4
CO
2
O
2
6216
6220
Frequency cm
-1
0
0.5
1
Transmission (%)
TCCON InGaAs
ext. InGaAs
stnd. InGaAs
Figure 1.
Example of scaled spectra from three different detector
types, with retrieval windows highlighted. The spectrum from the
EM27/SUN extended InGaAs detector was scaled 10 times more
than the spectrum from the standard InGaAs detector.
EM27/SUN instruments, with the spectral regions where in-
dividual gases are retrieved highlighted. Oxygen (O
2
)
abun-
dance is useful in calculating the DMF because it represents
the column of dry air and is combined with the column of the
gas of interest to yield the DMF (Wunch et al., 2010).
The Caltech IFS 125HR uses a resolution of approxi-
mately 0.02 cm
1
(with a maximum optical path difference
(MOPD) of 45 cm). It takes about 170 s to complete one for-
ward/backward scan pair. TCCON sites have single sound-
ing 2
σ
uncertainties of 0.8 ppm (X
CO
2
)
, 7 ppb (X
CH
4
)
, 4 ppb
(X
CO
)
, and 3 ppb (X
N
2
O
)
(Wunch et al., 2010). TCCON data
are tied to the World Meteorological Organization (WMO)
in situ trace gas measurement scale through extensive com-
parisons with in situ profiles obtained from aircraft and bal-
loon flights. We use the TCCON as a standard against which
to compare the EM27/SUN instruments. TCCON data from
this study are publicly available from the Carbon Dioxide In-
formation Analysis Center (Wennberg et al., 2014).
2.2 Caltech EM27/SUN
EM27/SUN spectrometers have been described elsewhere
(Gisi et al., 2012; Frey et al., 2015; Klappenbach et al., 2015)
so we focus on differences in setup and acquisition here. The
standard EM27/SUN configuration uses an InGaAs detector
sensitive to the spectral range spanning 5500–12 000 cm
1
,
which permits detection of O
2
, CO
2
, CH
4
, and H
2
O (Frey
et al., 2015). For this study, the Caltech EM27/SUN was
delivered with an extended-band InGaAs detector sensitive
to 4000–12 000 cm
1
, which allowed for additional mea-
surements of CO and N
2
O (Fig. 1). All EM27/SUN spec-
trometers used in this study (Sects. 2.2, 2.3) used the typ-
ical MOPD of 1.8 cm, corresponding to a spectral reso-
lution of 0.5 cm
1
. Interferograms (ifgs) were acquired in
direct-current-coupled mode to allow post-acquisition low-
pass filtering of brightness fluctuations to reduce the impact
of variable aerosol and cloud cover effects (Keppel-Aleks
et al., 2007). Ghosts were reduced as data were acquired
by employing the interpolated sampling option provided by
Bruker
(see also Sect. 4.3). A 10 KHz laser fringe rate is
used to reduce scanner velocity deviations, and each for-
ward/backward scan took 11.6 s, or 5.8 s per individual mea-
surement.
To be more consistent with the TCCON measurements,
no spectrum averaging or interferogram apodization was ap-
plied before retrieving DMFs. We recommend averaging
only after retrievals if disc storage and processor speeds are
sufficient, so spurious data can be filtered. To test the pre- vs.
post-averaging effect we used 9 retrieval days with 26 000
forward/backward measurements and used Bruker
OPUS
software to create spectra from ifgs. We compared retrievals
from using five combined backward/forward measurements
averaged pre-retrieval with those averaged post-retrieval. We
also compared combined forward/backward measurements
using a medium Norton–Beer apodization with those using
no special apodization. Results are in Table 1 and suggest
that different averaging methods cause only small inconsis-
tencies, under
0.02 % for X
CO
2
and X
CH
4
.
The EM27/SUN was placed within 5 m of the Cal-
tech TCCON solar tracker mirrors on the roof of the
Linde
+
Robinson building (Hale, 1935). Measurements
started on 2 June 2014 and, for this study, we include
186 measurement days that end on 4 May 2015. About
800 000 individual EM27/SUN measurements and 40 000 in-
dividual TCCON measurements were acquired over this
period. Of these, about 580 000 and 15 000 were consid-
ered coincident and were not screened out by our qual-
ity control filters (QCFs). Our QCFs were conservative,
and they required signal > 30 (Sect. 4.4), solar zenith angle
(SZA) < 82
, 370 ppm < X
CO
2
< 430 ppm, X
CO
2
,
error
< 5 ppm,
X
CO
,
error
< 20 ppb, and X
CH
4
,
error
< 0.1 ppm. Other users may
consider stricter QCFs. After averaging data into 10 min bins,
there were about 6500 binned comparison points.
2.3 LANL and Harvard EM27/SUN instruments
Three additional EM27/SUN instruments were compared
with the Caltech TCCON site in January 2015 – one owned
by Los Alamos National Laboratory (LANL) and two owned
by Harvard University (HU). To be consistent, all the acqui-
sition and retrieval settings were the same as for the Caltech
EM27/SUN. As opposed to the Caltech EM27/SUN (also
abbr. cn), the LANL (abbr. pl) and HU instruments (abbr.
ha and hb) used the original InGaAs detector type sensitive
over 5500–12 000 cm
1
(Frey et al., 2015). The LANL in-
strument, however, has a different high-pass filter, allowing
it to measure up to 14 500 cm
1
. This different filter is nei-
ther beneficial nor disadvantageous to this instrument as no
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Atmos. Meas. Tech., 9, 3527–3546, 2016
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J. K. Hedelius et al.: Assessment of errors in Xgas from a 0.5 cm
1
spectrometer
Table 1.
Pre-averaging and apodization effects on EM27/SUN retrievals.
X
CO
2
X
CH
4
X
H
2
O
X
CO
X
N
2
O
% error
Md.
σ
Md.
σ
Md.
σ
Md.
σ
Md.
σ
5 fwd/bwd pre-avgd.
a
,
b
< 0.01
0.01
0.02
0.01
0.36
0.13
< 0.01
0.15
0.30
0.12
NB med. apodz.
a
,
c
0.29
0.09
0.07
0.10
0.35
0.23
1.01
0.58
1.36
0.55
Measurement compared over 1–10 July 2014. Md denotes the median. NB denotes the medium Norton–Beer apodization.
a
As compared to retrievals from 1
fwd/bwd averaged non-apodized measurement averaged over same time post-retrieval.
b
Same apodization as standard.
c
Same pre-averaging as standard.
gas column amounts are retrieved in that region. The LANL
instrument was first used in January 2014 and has been com-
pared with multiple TCCON sites in the United States, in-
cluding sites at Four Corners, LANL, NASA Armstrong, La-
mont, Park Falls, and multiple Caltech comparisons (Parker
et al., 2015). The HU instruments have been operational
since May 2014 and were compared against each other at
Harvard before traveling over 4100 km to Caltech. As noted
by Gisi et al. (2012) and Chen et al. (2016), the ILS of these
instruments is remarkably stable considering the long dis-
tances they traveled.
3 Retrieval software
SFIT (Pougatchev et al., 1995), PROFFIT (“PROFile fit”,
Hase et al., 2004), and GGG (Wunch et al., 2015) are
the three widely used retrieval algorithms to fit direct so-
lar spectra and obtain column abundances of atmospheric
gases. PROFFIT is maintained by the Karlsruhe Institute
of Technology (KIT) and has been used to obtain DMFs
from EM27/SUN instruments as well as NDACC-IRWG
sites (Gisi et al., 2012; Frey et al., 2015; Hase et al., 2015).
GGG is maintained by the Jet Propulsion Laboratory (JPL)
and has been used to obtain DMFs from other low-resolution
instrument measurements (e.g., an IFS 66, see Petri et al.,
2012), in addition to being used to retrieve DMFs from the
MkIV spectrometer in balloon-borne measurements (Toon,
1991) and for the Atmospheric Trace Molecule Spectroscopy
Experiment (ATMOS) flown on the space shuttle (Irion et al.,
2002). GGG is the retrieval algorithm used by the TCCON
(Wunch et al., 2011b). We chose to use GGG for our anal-
ysis because (1) we want to be consistent with the TCCON
for comparison and (2) the GGG software suite containing
GFIT is open-source allowing us to adapt routines if needed.
We used the GGG2014 version for retrievals (Wunch et al.,
2015).
All retrievals used the same pTz and H
2
O modeled pro-
files as well as the same a priori profiles (Wunch et al.,
2015). We also used the same meteorological surface data
for retrievals from all five instruments. All retrievals also
used the same 0.2 hPa surface pressure offset. This offset
was determined by comparing measurements from the stan-
dard barometer with a calibrated Paroscientific Inc. 765–16B
Barometric Pressure Standard that has a stated accuracy of
better than 0.1 hPa.
3.1 Interferogram-to-spectrum – double-sided
TCCON uses an interferogram-to-spectrum subroutine part
of GGG to perform fast Fourier transforms (FFTs) to create
spectra from ifgs (Wunch et al., 2015). Though the Bruker
OPUS software used to operate the spectrometer can also
perform FFTs, we again chose to use GGG to maintain con-
sistency. A developmental version of GGG was used, which
was adapted to also allow FFT processing on EM27/SUN
interferograms. GGG splits a raw forward/backward ifg into
two different double-sided ifgs which are then FFTed to yield
two spectra. GGG also corrects source brightness fluctua-
tions (Keppel-Aleks et al., 2007).
3.2 EM27/SUN GGG and interferogram processing
suite (EGI)
To make GGG retrievals simpler for new EM27/SUN users,
an add-in software suite (EGI) was developed at Caltech
to create correctly formatted input files. This suite is open-
source and can be obtained through correspondence to the
email address listed. EGI can be run using MATLAB or
Python. EGI runs in UNIX, Mac OS, and Linux environ-
ments and runs GGG on multiple processors. EGI central-
izes settings for paths to read and write files, it coordinates
separately acquired ground weather station and GPS data
with EM27/SUN ifgs, and it optimizes processing order. It
also provides some ancillary calculations such as a spectral
signal-to-noise ratio (SNR) calculation. EGI provides a sim-
ple way to turn on and off saving of ancillary retrieval files
(i.e., spectral fits and averaging kernels). EGI can run for in-
struments employing one or two detectors, such as the type
described by Hase et al. (2016). Like the GGG software suite,
EGI also includes benchmark spectra acquired under differ-
ent conditions to run simple tests on. EGI is automated, re-
ducing the learning time as well as the amount of user time
needed to retrieve DMFs. After an initial setup, EGI will run
from ifgs to retrieved X
gas
with two commands. On a com-
puter with 1400 MHz processors the code takes
30 s per
CPU to process each interferogram from the EM27/SUN ex-
tended InGaAs detector.
Atmos. Meas. Tech., 9, 3527–3546, 2016
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J. K. Hedelius et al.: Assessment of errors in Xgas from a 0.5 cm
1
spectrometer
3531
Table 2.
ILS of EM27/SUN instruments.
Instrument
num – ID
9 January 2015
ME, PE (mrad)
a
28 January 2015
ME, PE (mrad)
Caltech (42 – cn)
0.986,
4.88
0.979
b
,
3.58
LANL (34 – pl)
0.999,
1.34
Harvard 1 (45 – ha)
0.973
c
,
1.99
Harvard 2 (46 – hb)
0.991
c
,
4.18
0.991,
4.00
Missing values indicate ILS not characterized on that day.
a
Phase error values are
italicized.
b
After realigning this instrument the ME was as high as 0.994.
c
As reported by Chen et al. (2016).
4 Instrument characterizations and performance
4.1 Instrument line shape
Knowledge of the instrument line shape (ILS), or the ob-
served shape of a spectral line from a monochromatic input,
is crucial in assessing instrument performance and avoiding
unknown biases in retrievals. Two parameters in the the LIN-
EFIT algorithm (Hase et al., 1999) are used to characterize
the ILS in relation to an ideal instrument, namely the modu-
lation efficiency (ME) and phase error (PE). ME and PE both
describe the interferogram and vary with OPD (Hase et al.,
1999; Frey et al., 2015). PE is the angle between the real and
imaginary parts of the FT of the ILS (Wunch et al., 2007).
PE has an ideal value of 0 radians, and indicates the degree
of asymmetry in spectral lines. ME is a measure of the nor-
malized observed interferogram signal compared with that
of a nominal instrument with an ideal value of 1 (unitless)
(Hase, 2012). At maximum OPD (MOPD), an ME < 1 causes
a broadening of the measured spectral lines, while an ME > 1
at MOPD causes a narrowing. The ILS can be calculated by
analyzing absorption lines measured through a low-pressure
gas cell, and varies with OPD (Hase et al., 1999). Here, we
use only single ME and PE values at the MOPD (Frey et
al., 2015) to describe the ILS. We characterized the ILS for
the EM27/SUN instruments using the method described else-
where (Frey et al., 2015; Klappenbach et al., 2015). This
method is able to characterize ME to within 0.15 % using
the LINEFIT algorithm (Hase et al., 1999), with supplemen-
tal MATLAB scripts for automation purposes (Chen et al.,
2016). ILS can affect retrieved column values. We note that
the ME at MOPD of the cn and ha instruments in Table 2 are
significantly lower than those reported by KIT on campus of
0.997 (Frey et al., 2015), and post-campaign of
0.996
(Klappenbach et al., 2015).
For this study, the ILS is used to help explain biases, to
demonstrate the stability of the instruments, and gives insight
into how well the EM27/SUN instruments are aligned and
their optical aberrations. Though GGG2014 retrievals do not
account for non-ideal ILS, future versions of GGG will. For
the current study, we assume that ILS impacts using PROF-
FIT will be similar to impacts using GGG. This assumption
5
10
15
20
25
30
35
40
Ambient temperature °C
-120
-100
-80
-60
-40
-20
0
CO
2
6220 cm
-1
FS (ppm)
CIT EM27
LANL EM27
HU EM27 (1)
HU EM27 (2)
Figure 2.
Frequency shifts (FS) of all four instruments vary with
temperature because the lasers are not frequency-stabilized. FS for
the CO
2
6220 cm
1
window are shown. FS of the Caltech (CIT)
instrument are far from zero, so an empirical correction is made to
correct the sample spacing number. Only every 300th CIT point and
every 20th LANL point is plotted for clarity. HU EM27 1 and 2 are
also referred to as ha and hb respectively by Chen et al. (2016).
will need to be tested when GGG also can account for a non-
ideal ILS. Because future GGG retrievals will be revised us-
ing historical ILS measurements, a need remains to monitor
the ILS both for future retrievals and as an indicator if re-
alignment is necessary.
4.2 Frequency shifts
EM27/SUN units contain a HeNe 633 nm (15 798 cm
1
)
metrology laser to sample the IR signal accurately as a func-
tion of the OPD. The laser is not frequency-stabilized (Gisi
et al., 2012). This causes apparent spectral frequency to
change with temperature as is shown in Fig. 2. Frequency
shifts are affected by changes in the input laser wavenum-
ber, laser alignment, and IR beam alignment. The input laser
wavenumber will affect the spacing between spectral points.
Since the frequency shift is furthest from zero for the Caltech
EM27/SUN (on order of
100 ppm, in red Fig. 2), the spec-
tral spacing is empirically corrected in the EGI suite based on
the CO
2
6220 cm
1
window frequency shifts. This made lit-
tle difference for the primary gases of interest affecting X
CO
2
by 0.015 % and X
CH
4
by
0.005 %, though it did affect X
H
2
O
by 4 %.
4.3 Ghosts
Ghosts are artificial spectral features linked to the aliasing
of true spectral lines that arise in FTS spectra (Learner et
al., 1996). The InGaAs detectors are optically sensitive at
wavenumbers greater than half the HeNe metrology laser
frequency (7899 cm
1
)
. To fulfill the Nyquist criterion and
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Atmos. Meas. Tech., 9, 3527–3546, 2016
3532
J. K. Hedelius et al.: Assessment of errors in Xgas from a 0.5 cm
1
spectrometer
prevent aliasing, the IR interferogram is sampled twice each
laser interferogram cycle, on the rising and falling edge.
However, if the laser sampling is asymmetric – for exam-
ple from a faulty electronics board – aliasing can still occur,
folded across the half laser frequency (Messerschmidt et al.,
2010). Because the asymmetry is typically small, the aliased
signal, or ghost spectrum, is small compared with the true
spectrum (Dohe et al., 2013; Wunch et al., 2015).
In EM27/SUN instruments the laser sampling error (LSE)
can be minimized as data are collected by employing the in-
terpolated sampling option provided by Bruker
. This re-
sampling mode uses only the rising edge of the laser interfer-
ogram and assumes constant velocity in between the rising
edges to interpolate the sampling (Gisi, 2014). We use a nar-
row band-pass filter (3 dB band width 5820–6150 cm
1
)
in
the Caltech EM27/SUN to test for LSE ghosts at 9800 cm
1
.
The ghost to parent ratio is 1.73
×
10
4
at a 10 kHz acqui-
sition rate without the interpolated sampling activated. This
ghost is eliminated with the interpolated sampling turned on.
In actual solar tests, turning the interpolated sampling on
and off had no noticeable effect on the DMF retrievals for
the Caltech EM27/SUN; however this may not hold true for
all instruments. The LSE ghost also disappeared at an ac-
quisition frequency of 20 kHz, and returned at higher acqui-
sition frequencies. We opted for the recommended 10 kHz
acquisition rate with the interpolated sampling on for all
EM27/SUNs in this analysis because other instruments may
be more significantly affected by LSE ghosts. A double-
frequency ghost remains at
11 900 cm
1
from radiation
passing through the interferometer twice that is much larger
than the LSE ghost, but is not in a region that will affect re-
trievals.
4.4 Mirror degradation and detector linearity
Solar tracking mirrors provided with the EM27/SUN instru-
ments are gold with a protective coating. Gold is used be-
cause of its excellent reflectance in the near-IR and low re-
flectance in the visible region (Bennett and Ashley, 1965),
which allows a high signal while reducing excess heating of
the field stop and other optics. Through extended tests, we
noted the first two mirrors (gold on plated aluminum, with
a coating) degrade over time, with an e-folding degradation
time of
90 days as is shown in Fig. 3. Arbitrary units (AUs)
for signal are the maximum ordinate values of the unmodi-
fied interferograms multiplied by 6450. The AUs of signal
happen to be close to the spectral SNR – a scaling factor of
1.3 applied to the arbitrary signal has an
R
2
of 0.63 relative
to the SNR. Cleaning helped restore some signal, but never to
the original values. The mirror change may not have restored
full signal because the rest of the optics were not cleaned at
the time of the mirror change. Below the blue 150 AU line in
Fig. 3 the fitted O
2
root mean square (rms) as a percentage of
the continuum level dropped 26 times faster with signal in-
tensity than above it. The instrument did come with an extra
07-14
10-14
01-15
04-15
Month-year
0
200
400
600
800
1000
ifm
#
6450 (A.U.)
A
Mirror change
0
100
200
300
400
500
600
Hours of sun observations
Figure 3.
Interferograms from EM27/SUN instruments are nega-
tive, with the most negative ordinate values at ZPD and saturation
occurring at
1. Here the interferogram maximums (ifm) refer to
the maximum (least negative) ordinate values of the raw interfer-
ograms. They were normalized so the maximum is 1000 and are
plotted with time showing the loss of signal. These values are af-
fected by clouds, which are the cause for much of the scatter. They
are also affected by SZA which explains some apparent interme-
diate increases. Only every 50th point is plotted for clarity. Mirror
cleaning (thin black lines) helped restore some signal, but never to
original values. The 150 AU line is in blue.
set of mirrors, but because mirrors are consumable parts, it
adds recurring cost and effort to maintain these instruments
long-term. After 1 year of use, the third mirror (gold coated
glass) still remains completely intact. Feist et al. (2016) had
success using steel mirrors under the very harsh conditions at
the Ascension Island TCCON site, though at a cost of 35 %
reflectivity per mirror. The JPL TCCON sites near Caltech
noted no degradation on the external gold mirrors over more
than 1 year of measurements. The lack of degradation on the
third external mirror and the JPL TCCON mirrors is likely
due to differences in how the mirrors were manufactured, in-
cluding how the gold is applied to the substrate and the coat-
ings used. Mirror degradation has likely not been a widely re-
ported problem for most of the EM27/SUN community, per-
haps because these instruments typically are stored indoors
and only used for a few days for campaigns (for example,
Frey et al., 2015). However, this problem may affect mirrors
on other EM27/SUN instruments when mirrors are exposed
outside for extended periods of time.
With signal loss, we would anticipate that gas measure-
ments would become noisier but remain unbiased. However,
with time, the Caltech EM27/SUN X
CO
2
and X
CH
4
DMFs
decreased relative to the TCCON DMFs as mirror reflectance
decreased, and X
CO
2
and X
CH
4
increased when the mirrors
were replaced. The TCCON IFS 125HR InGaAs detectors
are already known to be sufficiently linear that no correc-
tion is required (Wunch et al., 2011b). We also performed a
simple test repeatedly adding mesh screens in front of the en-
Atmos. Meas. Tech., 9, 3527–3546, 2016
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