Instrument Line Shape Function Research Articles

Assessment of the Influence of Instrument Parameters on the Detection Accuracy of Greenhouse-Gases Absorption Spectrometer-2 (GAS-2)

Satellite-based monitoring of atmospheric greenhouse gas (GHG) concentrations has emerged as a prominent and globally recognized field of research. With the imminent launch of the Greenhouse-Gases Absorption Spectrometer-2 (GAS-2) on the FengYun3-H (FY3-H) satellite in 2024, there is a promising prospect for substantial advancements in GHG detection capabilities. Crucially, the accurate acquisition of spectral information by GAS-2 is heavily reliant on its instrument parameters. However, the existing body of research predominantly emphasizes the examination of atmospheric parameters and their impact on GHG detection accuracy, thereby leaving a discernible gap in the comprehensive evaluation of instrument parameters specifically concerning the acquisition of atmospheric greenhouse gas concentration data by GAS-2. To address this knowledge gap, our study employs a radiation transfer model grounded in radiation transfer theory. This comprehensive investigation aims to quantitatively analyze the effects of various instrument parameters, encompassing crucial aspects such as spectral resolution, spectral sampling rate, signal-to-noise ratio, radiometric resolution, and spectral calibration accuracy (including instrument line shape function, central wavelength shift, and spectral resolution broadening). Based on our preliminary findings, it is evident that GAS-2 has the necessary spectral resolution, spectral sampling rate, and signal-to-noise ratio, slightly surpassing existing international instruments and enabling a significant detection accuracy level of 1 part per million (ppm). Moreover, it is essential to recognize the critical impact of instrument spectral calibration accuracy on overall detection precision. Among the five commonly used instrument line shape functions, the sinc function has the least impact on detection accuracy. Additionally, GAS-2’s radiance quantization depth is 14 bits, which is comparable to similar international payloads and maintains a root mean squared error below 0.1 ppm, thus ensuring a high level of precision. This study provides a comprehensive evaluation of the influence of GAS-2’s instrument parameters on detection accuracy, offering valuable insights for the future development of spectral calibration, the optimization of similar payload instrument parameters, and the overall improvement of instrument quantification capabilities.

Version 8 IMK–IAA MIPAS ozone profiles: nominal observation mode

Abstract. A new global O3 data product retrieved from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) spectra with the IMK–IAA MIPAS data processor has been released. These data are based on ESA version 8 recalibrated radiance spectra with improved temporal stability. Changes in the level-2 processing with respect to previous data versions include the following: (1) the retrievals use improved temperature data and thus suffer less from the propagation of related errors. (2) The background continuum is now considered up to 58 km. (3) A priori information is now used to constrain the retrieval of the radiance offset. (4) Water vapour is fitted jointly with ozone to minimize the impact of interfering water lines. (5) A more adequate regularization has been chosen. (6) Ozone absorption lines in the MIPAS A band (685–980 cm−1) are used almost exclusively because of inconsistencies in spectroscopic data in the MIPAS AB band (1010–1180 cm−1). Only at altitudes above 50 km, where A-band ozone lines do not provide sufficient information, are ozone lines in the MIPAS AB band used. (7) Temperature-adjusted climatologies of vibrational temperatures of O3 and CO2 are considered to account for non-local thermodynamic equilibrium radiation. Ozone errors are estimated to be less than 10 % in the altitude range 20–50 km. The error budget is dominated by the spectroscopic errors, followed by the uncertainty of the instrumental line shape function, the gain calibration error, and the spectral noise. The error contribution of interfering gases is almost negligible. The vertical resolution depends on altitude and atmospheric conditions. In 2002–2004 it varies between 2.5 km at the lowest altitudes and 6 km at 70 km, while in 2005–2012 it covers 2 to 5.5 km in the same altitude range. The horizontal smearing in terms of the full width at half maximum of the horizontal component of the two-dimensional averaging kernel matrix is smaller than, or approximately equal to, the distance between two subsequent limb scans at all altitudes. This implies that the horizontal resolution is sampling-limited or optimal, respectively. An additional data version is made available that is free of the formal a priori information and thus more user-friendly for certain applications. Version 8 ozone results show a better consistency between the two MIPAS measurement periods. They seem to be more realistic than preceding data versions in terms of long-term stability, as at least a part of the drift is corrected. Further, the representation of elevated stratopause situations is improved.

Impact of instrumental line shape characterization on ozone monitoring by FTIR spectrometry

Abstract. Retrieving high-precision concentrations of atmospheric trace gases from FTIR (Fourier transform infrared) spectrometry requires a precise knowledge of the instrumental performance. In this context, this paper examines the impact on the ozone (O3) retrievals of several approaches used to characterize the instrumental line shape (ILS) function of ground-based FTIR spectrometers within NDACC (Network for the Detection of Atmospheric Composition Change). The analysis has been carried out at the subtropical Izaña Observatory (IZO, Spain) by using the 20-year time series of the high-resolution FTIR solar absorption spectra acquired between 1999 and 2018. The theoretical quality assessment and the comparison to independent O3 observations available at IZO (Brewer O3 total columns and electrochemical concentration cell, ECC, sondes) reveal consistent findings. The inclusion of a simultaneous retrieval of the ILS parameters in the O3 retrieval strategy allows, on the one hand, a rough instrumental characterization to be obtained and, on the other hand, the precision of the FTIR O3 products to be slightly improved. The improvement is of special relevance above the lower stratosphere, where the cross-interference between the O3 vertical distribution and the instrumental performance is more significant. However, it has been found that the simultaneous ILS retrieval leads to a misinterpretation of the O3 variations on daily and seasonal scales. Therefore, in order to ensure the independence of the O3 retrievals and the instrumental response, the optimal approach to deal with the FTIR instrumental characterization is found to be the continuous monitoring of the ILS function by means of independent observations, such as gas cell measurements.

Improved ozone monitoring by ground-based FTIR spectrometry

Abstract. Accurate observations of atmospheric ozone (O3) are essential to monitor in detail its key role in atmospheric chemistry. The present paper examines the performance of different O3 retrieval strategies from FTIR (Fourier transform infrared) spectrometry by using the 20-year time series of the high-resolution solar spectra acquired from 1999 to 2018 at the subtropical Izaña Observatory (IZO, Spain) within NDACC (Network for the Detection of Atmospheric Composition Change). In particular, the effects of two of the most influential factors have been investigated: the inclusion of a simultaneous atmospheric temperature profile fit and the spectral O3 absorption lines used for the retrievals (the broad spectral region of 1000–1005 cm−1 and single micro-windows between 991 and 1014 cm−1). Additionally, the water vapour (H2O) interference in O3 retrievals has been evaluated, with the aim of providing an improved O3 strategy that minimises its impact and, therefore, could be applied at any NDACC FTIR station under different humidity conditions. The theoretical and experimental quality assessments of the different FTIR O3 products (total column (TC) amounts and volume mixing ratio (VMR) profiles) provide consistent results. Combining a simultaneous temperature retrieval with the optimal selection of single O3 micro-windows results in superior FTIR O3 products, with a precision of better than 0.6 %–0.7 % for O3 TCs as compared to coincident NDACC Brewer observations taken as a reference. However, this improvement can only be achieved provided the FTIR spectrometer is properly characterised and stable over time. For unstable instruments, the temperature fit is found to exhibit a strong negative influence on O3 retrievals due to the increase in the cross-interference between the temperature retrieval and instrumental performance (given by the instrumental line shape function and measurement noise), which leads to a worsening of the precision of FTIR O3 TCs of up to 2 %. This cross-interference becomes especially noticeable beyond the upper troposphere/lower stratosphere, as documented theoretically as well as experimentally by comparing FTIR O3 profiles to those measured using electrochemical concentration cell (ECC) sondes within NDACC. Consequently, it should be taken into account for the reliable monitoring of the O3 vertical distribution, especially over long-term timescales.

Fast Quantification of Air Pollutants by Mid-Infrared Hyperspectral Imaging and Principal Component Analysis.

An imaging Fourier-transform spectrometer in the mid-infrared (1850–6667 cm) has been used to acquire transmittance spectra at a resolution of 1 cm of three atmospheric pollutants with known column densities (Q): methane (258 ppm·m), nitrous oxide (107.5 ppm·m) and propane (215 ppm·m). Values of Q and T have been retrieved by fitting them with theoretical spectra generated with parameters from the HITRAN database, based on a radiometric model that takes into account gas absorption and emission, and the instrument lineshape function. A principal component analysis (PCA) of experimental data has found that two principal components are enough to reconstruct gas spectra with high fidelity. PCA-processed spectra have better signal-to-noise ratio without loss of spatial resolution, improving the uniformity of retrieval. PCA has been used also to speed up retrieval, by pre-calculating simulated spectra for a range of expected Q and T values, applying PCA to them and then comparing the principal components of experimental spectra with those of the simulated ones to find the gas Q and T values. A reduction in calculation time by a factor larger than one thousand is achieved with improved accuracy. Retrieval can be further simplified by obtaining T and Q as quadratic functions of the two first principal components.

Precision Spectroscopy of Nitrous Oxide Isotopocules with a Cross-Dispersed Spectrometer and a Mid-Infrared Frequency Comb.

As a potent greenhouse gas and an ozone-depleting agent, nitrous oxide (N2O) plays a critical role in the global climate. Effective mitigation relies on understanding global sources and sinks, which can be supported through isotopic analysis. We present a cross-dispersed spectrometer, coupled with a mid-infrared frequency comb, capable of simultaneously monitoring all singly substituted, stable isotopic variants of N2O. Rigorous evaluation of the instrument lineshape function and data treatment using a Doppler-broadened, low-pressure gas sample are discussed. Laboratory characterization of the spectrometer demonstrates sub-GHz spectral resolution and an average precision of 6.7 × 10-6 for fractional isotopic abundance retrievals in 1 s.

Optical frequency comb-based cavity-enhanced Fourier-transform spectroscopy: Application to collisional line-shape study

Direct-comb spectroscopy techniques uses optical frequency combs (OFCs) as spectroscopic light source. They deliver high sensitivity, high frequency resolution and precision in a broad spectral range. Due to these features, the field has burgeoned in recent years. In this work we constructed an OFC-based cavity-enhanced Fourier-transform spectrometer in the near-infrared region and used it for a line-shape study of rovibrational transitions of CO perturbed by Ar. The highly sensitive measurements spanned the wavenumber range from 6270 cm−1 to 6410 cm−1, which covered both P and R branch of the second overtone band of CO. The spectrometer delivers high-resolution surpassing the Fourier-transform resolution limit determined by interferogram length, successfully removing ringing and broadening effects caused by instrumental line shape function. The instrumental-line-shape-free method and high signal-to-noise ratio in the measurement allowed us to observe collisional effects beyond those described by the Voigt profile. We retrieved collisional line-shape parameters by fitting the speed-dependent Voigt profile and found good agreement with the values given by precise cavity ring-down spectroscopy measurements that used a continuous-wave laser referenced to a stabilized OFC. The results demonstrate that OFC-based cavity-enhanced Fourier-transform spectroscopy is a strong tool for accurate line-shape studies that will be crucial for future spectral databases.

Two-dimensional spatial heterodyne spectrometer for atmospheric nitrogen dioxide observations.

A broadband monolithic spatial heterodyne spectrometer (SHS) system is built for measuring nitrogen dioxide in the atmosphere based on our newly developed fabrication technique. This system is calibrated and tested with Hg, Kr and Xe lamps, as well as monochromator output illuminated by a high-voltage Xe lamp (as a white light source). The obtained overall efficiency profile presents an effective spectral range of 425-495 nm (when the efficiency values are greater than 40%). The maximum fringe visibility is ~0.85. The measured instrumental line shape function gives an actual spectral resolution of ~0.073 nm. The effect of phase distortion of this 2-D SHS system can be neglected. Direct solar-irradiance spectra in the NO2 absorption band were measured with the SHS system. The measured spectra are consistent with the results simulated by Modtran6 within the SHS spectral range. The vertical column contents of NO2, VC(NO2), derived from the SHS data by the direct sun - differential optical absorption spectroscopy (DS-DOAS) method coincide closely with the simultaneously acquired (OMI) satellite data.

Cloud remote sensing with EPIC/DSCOVR observations: A sensitivity study with radiative transfer simulations

The Earth Polychromatic Imaging Camera (EPIC) onboard the Deep Space Climate Observatory (DSCOVR) views nearly the whole sunlit face of the Earth with 10 spectral bands ranging from the UV to the near-infrared, including two oxygen absorbing bands centered at 764 nm (A-band) and 687.75 nm (B-band). Clouds are among the primary remote sensing targets using EPIC images because of their important impacts on the Earth’s radiation budget. In order to facilitate the EPIC cloud data product development, we have built a radiative transfer simulator featuring flexible cloud microphysical parameters, gas absorptions, and the instrument line shape functions for each EPIC band. The radiative transfer simulator is used to explore the sensitivity of EPIC observations on liquid-phase cloud microphysical parameters, including optical depth, geometric thickness, and cloud top height. We found that the ratios of the reflectances in the oxygen A and B bands to their respective continuum measurements can be used to increase the confidence level of cloud masking over scenes with sun-glint. In addition, the 388 nm band can be used to differentiate low and high clouds with the uncertainty of roughly 2–3 km. Combining this information with the oxygen absorption bands, the cloud geometric thickness can be obtained with the rough uncertainty of 3–4 km.

Instrument line shape function of laser heterodyne spectrometer

Laser heterodyne is a kind of technique based on coherent detection with high sensitivity and spectral resolution for spectrum measurements. For these reasons, it has been widely used in many research fields, such as trace gases’ detection of earth’s or terrestrial planets’ atmosphere. However, when the laser heterodyne spectrometer is used for measuring the spectrum, the instrument line shape (ILS) function usually smooth the spectrum, which affects the inversion results of the gas column density. In previous researches, the radio frequency (RF) filter response function was usually used as the ILS, but recent studies indicated that the ILS without consideration of the influence of lock-in amplifier was not precise enough. In order to obtain the ILS function of the laser heterodyne spectrometer, the main factors which influence the ILS are analyzed, including the RF filter bandwidth, integral time and low-pass filter of lock-in amplifier, and the process is based on the principle of laser heterodyne technology and the flow of heterodyne signal processing. The presented ILS is the convolution of RF filter, wavelength variation in the integral time and the low-pass filter. In addition, for testing the effectiveness of the ILS in this paper, the laser heterodyne spectrometer which was built in our laboratory is used for the multiple measurement of the absorption of water vapor and methane in the band of 3.53 <inline-formula><tex-math id="M2">\begin{document}${\text{μm}}$\end{document}</tex-math><alternatives><graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="6-20181620_M2.jpg"/><graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="6-20181620_M2.png"/></alternatives></inline-formula> and the column densities are retrieved with different ILS. The experimental results show that the actual resolutions of the laser heterodyne spectrometer are about 0.005 cm<sup>–1</sup> and 0.025 cm<sup>–1</sup> when the integral times are set to be 10 ms and 100 ms respectively. Furthermore, the RF filter response function and the ILS function presented in the paper are respectively used in the procedure of water vapor and methane inversion. The results show that when the ILS function used for the retrieval, the sum of squared residual reduces about 16% and the residuals at the peak of methane absorption reduces almost 100% compared with the scenario when using the RF filter function. Above all, the comprehensive analysis of the laser heterodyne spectrometer in this paper indicates that the ILS function is more precise than pioneering studies and this work will be helpful for retrieving the precise profiles of trace gases.

Laboratory spectral calibration of the TanSat atmospheric carbon dioxide grating spectrometer

Abstract. TanSat is a key satellite mission in the Chinese Earth Observation program and is designed to measure the global atmospheric column-averaged dry-air CO2 mole fraction by measuring the visible and near-infrared solar-reflected spectra. The first Chinese super-high-resolution grating spectrometer for measuring atmospheric CO2 is aboard TanSat. This spectrometer is a suite incorporating three grating spectrometers that make coincident measurements of reflected sunlight in the near-infrared CO2 band near 1.61 and 2.06 µm and in the molecular oxygen (O2) A-band at 0.76 µm. The spectral resolving power (λ∕Δλ) values are ∼19 000, ∼12 800, and ∼12 250 in the O2 A-band, and the weak and strong absorption bands of CO2, respectively. This paper describes the prelaunch spectral calibration of the atmospheric carbon dioxide grating spectrometer aboard TanSat. Several critical aspects of the spectrometer, including the spectral resolution, spectral dispersion, and the instrument line shape function of each channel, which are directly related to producing the Level 1 products are evaluated in this paper. The instrument line shape function of the spectrometer is notably symmetrical and perfectly consistent across all channels in the three bands. The symmetry is better then 99.99 %, and the consistency in the worst case is better then 99.97 %, 99.98 %, and 99.98 % in the O2 A, WCO2, and SCO2 bands, respectively. The resulting variations in the spectral calibrations and the radiometric response errors are negligible. The spectral resolution characterizations meet the mission requirements. The spectral dispersions have excellent consistency in the spatial dimension of each band, and there is good linearity in the spectral dimension of each band. The RMS errors of the fitting residuals are 0.9, 1, and 0.7 pm in the O2 A-band, the WCO2 band, and the SCO2 band, respectively. Taken together, these results suggest that the spectral characterizations of the spectrometer aboard TanSat meet the mission requirements.

A Fast Atmospheric Trace Gas Retrieval for Hyperspectral Instruments Approximating Multiple Scattering—Part 1: Radiative Transfer and a Potential OCO-2 XCO2 Retrieval Setup

Satellite retrievals of the atmospheric dry-air column-average mole fraction of CO 2 (XCO 2 ) based on hyperspectral measurements in appropriate near (NIR) and short wave infrared (SWIR) O 2 and CO 2 absorption bands can help to answer important questions about the carbon cycle but the precision and accuracy requirements for XCO 2 data products are demanding. Multiple scattering of light at aerosols and clouds can be a significant error source for XCO 2 retrievals. Therefore, so called full physics retrieval algorithms were developed aiming to minimize scattering related errors by explicitly fitting scattering related properties such as cloud water/ice content, aerosol optical thickness, cloud height, etc. However, the computational costs for multiple scattering radiative transfer (RT) calculations can be immense. Processing all data of the Orbiting Carbon Observatory-2 (OCO-2) can require up to thousands of CPU cores and the next generation of CO 2 monitoring satellites will produce at least an order of magnitude more data. Here we introduce the Fast atmOspheric traCe gAs retrievaL FOCAL including a scalar RT model which approximates multiple scattering effects with an analytic solution of the RT problem of an isotropic scattering layer and a Lambertian surface. The computational performance is similar to an absorption only model and currently determined by the convolution of the simulated spectra with the instrumental line shape function (ILS). We assess FOCAL’s quality by confronting it with accurate multiple scattering vector RT simulations using SCIATRAN. The simulated scenarios do not cover all possible geophysical conditions but represent, among others, some typical cloud and aerosol scattering scenarios with optical thicknesses of up to 0.7 which have the potential to survive the pre-processing of a XCO 2 algorithm for real OCO-2 measurements. Systematic errors of XCO 2 range from −2.5 ppm (−6.3‰) to 3.0 ppm (7.6‰) and are usually smaller than ±0.3 ppm (0.8‰). The stochastic uncertainty of XCO 2 is typically about 1.0 ppm (2.5‰). FOCAL simultaneously retrieves the dry-air column-average mole fraction of H 2 O (XH 2 O) and the solar induced chlorophyll fluorescence at 760 nm (SIF). Systematic and stochastic errors of XH 2 O are most times smaller than ±6 ppm and 9 ppm, respectively. The systematic SIF errors are always below 0.02 mW/m 2 /sr/nm, i.e., it can be expected that instrumental or forward model effects causing an in-filling of the used Fraunhofer lines will dominate the systematic errors when analyzing actually measured data. The stochastic uncertainty of SIF is usually below 0.3 mW/m 2 /sr/nm. Without understating the importance of analyzing synthetic measurements as presented here, the actual retrieval performance can only be assessed by analyzing measured data which is subject to part 2 of this publication.

Preflight Spectral Calibration of the Orbiting Carbon Observatory 2

This paper describes the preflight spectral calibration methods and results for the Orbiting Carbon Observatory 2 (OCO-2), following the approach developed for the first OCO. The instrument line shape (ILS) function and dispersion parameters were determined through laser-based spectroscopic measurements, and then further optimized by comparing solar spectra recorded simultaneously on the ground by the OCO-2 flight instrument and a collocated high-resolution Fourier transform spectrometer (FTS). The resulting ILS profiles and dispersion parameters, when applied to the FTS solar data, showed agreement between the spectra recorded by the spectrometers and FTS to approximately 0.2% RMS, satisfying the preflight spectral calibration accuracy requirement of <0.25% RMS. Specific changes to the OCO-2 instrument and calibration process, compared to the original OCO, include stray-light protection; improved laser setup; increased spectral sampling; enhanced data screening, and incremental improvements in the ILS, dispersion, and FTS optimization analyses.

Prelaunch spectral calibration of a carbon dioxide spectrometer

The carbon dioxide spectrometer (CDS) on board the Chinese Carbon Dioxide Observation Satellite (TanSat) is a high spectral and spatial resolution grating spectrometer with three specific spectral bands dedicated to atmospheric CO2 detection. The CDS’s design and on-ground spectral calibration are presented in this paper. The instrument line shape functions and spectral dispersion were characterized using a tunable diode laser-based testing system for all spectral pixels of the CDS placed in a thermal vacuum chamber.

Characterization of the OCO-2 instrument line shape functions using on-orbit solar measurements

Abstract. Accurately characterizing the instrument line shape (ILS) of the Orbiting Carbon Observatory-2 (OCO-2) is challenging and highly important due to its high spectral resolution and requirement for retrieval accuracy (0. 25 %) compared to previous spaceborne grating spectrometers. On-orbit ILS functions for all three bands of the OCO-2 instrument have been derived using its frequent solar measurements and high-resolution solar reference spectra. The solar reference spectrum generated from the 2016 version of the Total Carbon Column Observing Network (TCCON) solar line list shows significant improvements in the fitting residual compared to the solar reference spectrum currently used in the version 7 Level 2 algorithm in the O2 A band. The analytical functions used to represent the ILS of previous grating spectrometers are found to be inadequate for the OCO-2 ILS. Particularly, the hybrid Gaussian and super-Gaussian functions may introduce spurious variations, up to 5 % of the ILS width, depending on the spectral sampling position, when there is a spectral undersampling. Fitting a homogeneous stretch of the preflight ILS together with the relative widening of the wings of the ILS is insensitive to the sampling grid position and accurately captures the variation of ILS in the O2 A band between decontamination events. These temporal changes of ILS may explain the spurious signals observed in the solar-induced fluorescence retrieval in barren areas.

FT-IR spectra of 18O-, and 13C-enriched CO2 in the ν3 region: High accuracy frequency calibration and spectroscopic constants for 16O12C18O, 18O12C18O, and 16O13C16O

In this report, we extend our Fourier transform infrared (FT-IR) spectroscopy measurements of CO2 in the ν3 region (2200–2450cm−1, 65–75THz) to the 18O-, and 13C-substituted isotopologues, using the JPL Bruker IFS-125HR Fourier Transform Spectrometer (JPL-FTS). High quality (S/N∼2000) spectra were obtained separately for each of the 18O-, and 13C-isotopically enriched samples. The absolute wavenumber accuracies were better than 3×10−6cm−1 (∼100kHz) for strong, isolated transitions, calibrated against the highest accuracy reported CO and 16O12C16O (626) frequency measurements. The JPL-FTS performance and calibration procedure is shown to be reliable and consistent, achievable through vigorous maintenance of the optical alignment and regular monitoring of its instrumental line shape function. Effective spectroscopic constant fits of the 00011←00001 fundamental bands for 16O12C18O (628), 18O12C18O (828), and 16O13C16O (636) were obtained with RMS residuals of 2.9×10−6cm−1, 2.8×10−6cm−1, and 2.9×10−6cm−1, respectively. The observed bands encompassed 79 lines over the Jmax range of P67/R67, 47 lines over P70/R62, and 60 lines over P70/R70 for 628, 828, and 636, respectively. These results complement our recent work on the 17O-enriched isotopologues (Elliott et al., 2014), providing additional high-quality frequency measurements for atmospheric remote sensing applications.

Hyperspectral quantitative imaging of gas sources in the mid-infrared.

An imaging Fourier transform spectrometer operating in the medium infrared (1800-5000 cm(-1)) has been used to image two gas sources: a controlled CO2 leak at room temperature and the exhaust of a combustion engine. Spectra have been acquired at a resolution of 0.5 cm(-1) using an extended blackbody as the background. By fitting them with theoretical spectra generated with parameters from the High-Resolution Transmission Molecular Absorption database, quantitative maps of temperature and gas column density (concentration·path product) for the gas plumes have been obtained. Spectra are related to gas plume parameters by means of a radiometric model that takes into account not only gas absorption, but also its emission and the atmospheric absorption, as well as the instrument lineshape function. Measurements for the gas leak show very good agreement between retrieved and nominal values of temperature and CO2 column density. This result has direct application to obtain quantitative imaging of exhaust emissions from automobiles and other mobile sources, as shown here with measurements of exhaust gases in a diesel engine.

Retrieval of Atmospheric CO2and CH4Variations Using Ground-Based High Resolution Fourier Transform Infrared Spectra

High resolution Fourier transform near IR solar spectra are used to estimate the column-averaged dry-air mole fraction (DMF) of CO2andCH4variations in the atmosphere. The preliminary retrieval results for CO2andCH4variations in the area of Hefei, China, are presented, and the underlying error sources are also analyzed. Both a forward analysis and an inversion algorithm are included in the retrieval. The forward analysis uses the modeled atmospheric transmittance to line-by-line (LBL) convolute the instrument line shape function. The influences of the temperature, pressure, humidity, and a priori gases are considered in the atmospheric transmittance model. The inversion algorithm is based on the nonlinear iterative and nonlinear least squares spectral fitting, which is used to obtainVCDCO2andVCDCH4(which represent vertical column density of CO2andCH4, resp.). Furthermore, theVCDO2is also retrieved for converting the VCDs into DMFs. DMFs are final products of data analysis. The inversion results can clearly resolve the tiny variations of CO2andCH4under strong atmospheric background. Spectral fitting residuals for bothVCDCO2andVCDCH4are less than 0.5%. Finally, CO2andCH4diurnal variations are investigated based on a typical observation. About 2 ppm amplitude forDMFCO2diurnal variations and less than 15 ppb amplitude forDMFCH4are observed.

Preflight Spectral Calibration of the Orbiting Carbon Observatory

We report on the preflight spectral calibration of the first Orbiting Carbon Observatory (OCO) instrument. In particular, the instrument line shape (ILS) function as well as spectral position was determined experimentally for all OCO channels. Initial determination of these characteristics was conducted through laser-based spectroscopic measurements. The resulting spectral calibration was validated by comparing solar spectra recorded simultaneously by the OCO flight instrument and a collocated high-resolution Fourier transform spectrometer (FTS). The spectral calibration was refined by optimizing parameters of the ILS as well as the dispersion relationship, which determines spectral position, to yield the best agreement between these two measurements. The resulting ILS profiles showed agreement between the spectra recorded by the spectrometers and FTS to approximately 0.2% rms, satisfying the preflight spectral calibration accuracy requirement of better than 0.25% rms.

Multi-decade measurements of the long-term trends of atmospheric species by high-spectral-resolution infrared solar absorption spectroscopy

Solar absorption spectra were recorded for the first time in 5 years with the McMath Fourier transform spectrometer at the US National Solar Observatory on Kitt Peak in southern Arizona, USA (31.91°N latitude, 111.61°W longitude, 2.09 km altitude). The solar absorption spectra cover 750–1300 and 1850–5000 cm −1 and were recorded on 20 days during March–June 2009. The measurements mark the continuation of a long-term record of atmospheric chemical composition measurements that have been used to quantify seasonal cycles and long-term trends of both tropospheric and stratospheric species from observations that began in 1977. Fits to the measured spectra have been performed, and they indicate the spectra obtained since return to operational status are nearly free of channeling and the instrument line shape function is well reproduced taking into account the measurement parameters. We report updated time series measurements of total columns for six atmospheric species and their analysis for seasonal cycles and long-term trends. As an example, the time series fit shows a decrease in the annual increase rate in Montreal-Protocol-regulated chlorofluorocarbon CCl 2F 2 from 1.51±0.38% yr −1 at the beginning of the time span to −1.54±1.28% yr −1 at the end of the time span, 1 sigma, and hence provides evidence for the impact of those regulations on the trend.