Global retrieval of solar induced fluorescence emitted by terrestrial vegetation can provide an unprecedented measure for photosynthetic efficiency. The GOSAT (JAXA, launched Feb. 2009) and OCO‐2 ...(NASA, to be launched 2013) satellites record high‐resolution spectra in the O2 A‐band region, overlapping part of the chlorophyll fluorescence spectrum. We show that fluorescence cannot be unambiguously discriminated from atmospheric scattering effects using O2 absorption lines. This can cause systematic biases in retrieved scattering parameters (aerosol optical thickness, aerosol height, surface pressure, surface albedo) if fluorescence is neglected. Hence, we demonstrate an efficient alternative fluorescence least‐squares retrieval method based solely on strong Fraunhofer lines in the vicinity of the O2 A‐band, disentangling fluorescence from scattering effects. Not only does the Fraunhofer line fit produce a more accurate estimate of fluorescence emission, but it also allows improved retrievals of atmospheric aerosols from the O2 A‐band.
Atmospheric column abundances of carbon dioxide (CO2), carbon monoxide (CO), methane (CH4) and nitrous oxide (N2O) have been measured above the South Coast air basin (SCB), a densely populated urban ...region of Southern California, USA, which includes Los Angeles and the surrounding suburbs. Large diurnal variations in CO and CH4 are observed which correlate well with those in CO2. Weaker correlations are seen between N2O and CO2, with large uncertainties. We compute yearly SCB emissions of CO and CH4 to be 1.4 ± 0.3 Tg CO and 0.6 ± 0.1 Tg CH4. We compare our calculated emissions to the California Air Resources Board (CARB) and the Emission Database for Global Atmospheric Research (EDGAR) estimates. Our measurements confirm that urban emissions are a significant source of CH4 and in fact may be substantially higher than currently estimated. If our emissions are typical of other urban centers, these findings suggest that urban emissions could contribute 7–15% to the global anthropogenic budget of methane.
•HITRAN2016 molecular spectroscopic database is described.•Dynamic web interface at www.hitran.org is introduced.•HITRAN Application Programming Interface is introduced.•Substantial extent of the ...amount and quality of the data highlighted.•Many new spectroscopic parameters are now available in HITRAN.
This paper describes the contents of the 2016 edition of the HITRAN molecular spectroscopic compilation. The new edition replaces the previous HITRAN edition of 2012 and its updates during the intervening years. The HITRAN molecular absorption compilation is composed of five major components: the traditional line-by-line spectroscopic parameters required for high-resolution radiative-transfer codes, infrared absorption cross-sections for molecules not yet amenable to representation in a line-by-line form, collision-induced absorption data, aerosol indices of refraction, and general tables such as partition sums that apply globally to the data. The new HITRAN is greatly extended in terms of accuracy, spectral coverage, additional absorption phenomena, added line-shape formalisms, and validity. Moreover, molecules, isotopologues, and perturbing gases have been added that address the issues of atmospheres beyond the Earth. Of considerable note, experimental IR cross-sections for almost 300 additional molecules important in different areas of atmospheric science have been added to the database. The compilation can be accessed through www.hitran.org. Most of the HITRAN data have now been cast into an underlying relational database structure that offers many advantages over the long-standing sequential text-based structure. The new structure empowers the user in many ways. It enables the incorporation of an extended set of fundamental parameters per transition, sophisticated line-shape formalisms, easy user-defined output formats, and very convenient searching, filtering, and plotting of data. A powerful application programming interface making use of structured query language (SQL) features for higher-level applications of HITRAN is also provided.
Attribution of the causes of atmospheric trace gas and aerosol variability often requires the use of high resolution time series of anthropogenic and natural emissions inventories. Here we developed ...an approach for representing synoptic‐ and diurnal‐scale temporal variability in fire emissions for the Global Fire Emissions Database version 3 (GFED3). We disaggregated monthly GFED3 emissions during 2003–2009 to a daily time step using Moderate Resolution Imaging Spectroradiometer (MODIS)‐derived measurements of active fires from Terra and Aqua satellites. In parallel, mean diurnal cycles were constructed from Geostationary Operational Environmental Satellite (GOES) Wildfire Automated Biomass Burning Algorithm (WF_ABBA) active fire observations. Daily variability in fires varied considerably across different biomes, with short but intense periods of daily emissions in boreal ecosystems and lower intensity (but more continuous) periods of burning in savannas. These patterns were consistent with earlier field and modeling work characterizing fire behavior dynamics in different ecosystems. On diurnal timescales, our analysis of the GOES WF_ABBA active fires indicated that fires in savannas, grasslands, and croplands occurred earlier in the day as compared to fires in nearby forests. Comparison with Total Carbon Column Observing Network (TCCON) and Measurements of Pollution in the Troposphere (MOPITT) column CO observations provided evidence that including daily variability in emissions moderately improved atmospheric model simulations, particularly during the fire season and near regions with high levels of biomass burning. The high temporal resolution estimates of fire emissions developed here may ultimately reduce uncertainties related to fire contributions to atmospheric trace gases and aerosols. Important future directions include reconciling top‐down and bottom up estimates of fire radiative power and integrating burned area and active fire time series from multiple satellite sensors to improve daily emissions estimates.
Key Points
We developed an approach to distribute daily and hourly fire emissions
Daily and hourly patterns of fire activity varied among different land types
Daily and hourly fire emissions improved CO simulations
The HITRAN2012 molecular spectroscopic database Rothman, L.S.; Gordon, I.E.; Babikov, Y. ...
Journal of quantitative spectroscopy & radiative transfer,
November 2013, 2013-11-00, 20131101, 2013-11, Letnik:
130
Journal Article
Recenzirano
Odprti dostop
This paper describes the status of the 2012 edition of the HITRAN molecular spectroscopic compilation. The new edition replaces the previous HITRAN edition of 2008 and its updates during the ...intervening years. The HITRAN molecular absorption compilation is comprised of six major components structured into folders that are freely accessible on the internet. These folders consist of the traditional line-by-line spectroscopic parameters required for high-resolution radiative-transfer codes, infrared absorption cross-sections for molecules not yet amenable to representation in a line-by-line form, ultraviolet spectroscopic parameters, aerosol indices of refraction, collision-induced absorption data, and general tables such as partition sums that apply globally to the data. The new HITRAN is greatly extended in terms of accuracy, spectral coverage, additional absorption phenomena, and validity. Molecules and isotopologues have been added that address the issues of atmospheres beyond the Earth. Also discussed is a new initiative that casts HITRAN into a relational database format that offers many advantages over the long-standing sequential text-based structure that has existed since the initial release of HITRAN in the early 1970s.
•A new edition of the HITRAN molecular spectroscopic database is described.•HITRAN now includes a large number of molecules and their isotopologues.•HITRAN is now applicable to planetary atmospheres in addition to terrestrial.•A new structure for the database is described.•Many new spectroscopic phenomena are now available for the user.
We describe a method of evaluating systematic errors in measurements of total column dry-air mole fractions of CO2 (XCO2 ) from space, and we illustrate the method by applying it to the v2.8 ...Atmospheric CO2 Observations from Space retrievals of the Greenhouse Gases Observing Satellite (ACOS-GOSAT) measurements over land. The approach exploits the lack of large gradients in XCO2 south of 25° S to identify large-scale offsets and other biases in the ACOS-GOSAT data with several retrieval parameters and errors in instrument calibration. We demonstrate the effectiveness of the method by comparing the ACOS-GOSAT data in the Northern Hemisphere with ground truth provided by the Total Carbon Column Observing Network (TCCON). We use the observed correlation between free-tropospheric potential temperature and XCO2 in the Northern Hemisphere to define a dynamically informed coincidence criterion between the ground-based TCCON measurements and the ACOS-GOSAT measurements. We illustrate that this approach provides larger sample sizes, hence giving a more robust comparison than one that simply uses time, latitude and longitude criteria. Our results show that the agreement with the TCCON data improves after accounting for the systematic errors, but that extrapolation to conditions found outside the region south of 25° S may be problematic (e.g., high airmasses, large surface pressure biases, M-gain, measurements made over ocean). A preliminary evaluation of the improved v2.9 ACOS-GOSAT data is also discussed.
This work describes the NASA Atmospheric CO2 Observations from Space (ACOS) XCO2 retrieval algorithm, and its performance on highly realistic, simulated observations. These tests, restricted to ...observations over land, are used to evaluate retrieval errors in the face of realistic clouds and aerosols, polarized non-Lambertian surfaces, imperfect meteorology, and uncorrelated instrument noise. We find that post-retrieval filters are essential to eliminate the poorest retrievals, which arise primarily due to imperfect cloud screening. The remaining retrievals have RMS errors of approximately 1 ppm. Modeled instrument noise, based on the Greenhouse Gases Observing SATellite (GOSAT) in-flight performance, accounts for less than half the total error in these retrievals. A small fraction of unfiltered clouds, particularly thin cirrus, lead to a small positive bias of ~0.3 ppm. Overall, systematic errors due to imperfect characterization of clouds and aerosols dominate the error budget, while errors due to other simplifying assumptions, in particular those related to the prior meteorological fields, appear small.
Micrometeorites that ablate in the lower thermosphere and upper mesosphere are thought to recondense into nanometer‐sized smoke particles and then coagulate into larger dust particles. Previous ...studies with one‐dimensional models have determined that the meteoric dust size distribution is sensitive to the background vertical velocity and have speculated on the importance of the mesospheric meridional circulation to the dust spatial distribution. We conduct the first three‐dimensional simulations of meteoric dust using a general circulation model with sectional microphysics to study the distribution and characteristics of meteoric dust in the mesosphere and upper stratosphere. We find that the mesospheric meridional circulation causes a strong seasonal pattern in meteoric dust concentration in which the summer pole is depleted and the winter pole is enhanced. This summer pole depletion of dust particles results in fewer dust condensation nuclei (CN) than has traditionally been assumed in numerical simulations of polar mesospheric clouds (PMCs). However, the total number of dust particles present is still sufficient to account for PMCs if smaller particles can nucleate to form ice than is conventionally assumed. During winter, dust is quickly transported down to the stratosphere in the polar vortex where it may participate in the nucleation of sulfate aerosols, the formation of the polar CN layer, and the formation of polar stratospheric clouds (PSCs). These predictions of the seasonal variation and resulting large gradients in dust concentration should assist the planning of future campaigns to measure meteoric dust.
The Total Carbon Column Observing Network (TCCON) produces precise measurements of the column average dry-air mole fractions of CO2, CO, CH4, N2O and H2O at a variety of sites worldwide. These ...observations rely on spectroscopic parameters that are not known with sufficient accuracy to compute total columns that can be used in combination with in situ measurements. The TCCON must therefore be calibrated to World Meteorological Organization (WMO) in situ trace gas measurement scales. We present a calibration of TCCON data using WMO-scale instrumentation aboard aircraft that measured profiles over four TCCON stations during 2008 and 2009. These calibrations are compared with similar observations made in 2004 and 2006. The results indicate that a single, global calibration factor for each gas accurately captures the TCCON total column data within error.
The quality of the version 2.2 (v2.2) middle atmosphere water vapor and nitrous oxide measurements from the Microwave Limb Sounder (MLS) on the Earth Observing System (EOS) Aura satellite is ...assessed. The impacts of the various sources of systematic error are estimated by a comprehensive set of retrieval simulations. Comparisons with correlative data sets from ground‐based, balloon and satellite platforms operating in the UV/visible, infrared and microwave regions of the spectrum are performed. Precision estimates are also validated, and recommendations are given on the data usage. The v2.2 H2O data have been improved over v1.5 by providing higher vertical resolution in the lower stratosphere and better precision above the stratopause. The single‐profile precision is ∼0.2–0.3 ppmv (4–9%), and the vertical resolution is ∼3–4 km in the stratosphere. The precision and vertical resolution become worse with increasing height above the stratopause. Over the pressure range 0.1–0.01 hPa the precision degrades from 0.4 to 1.1 ppmv (6–34%), and the vertical resolution degrades to ∼12–16 km. The accuracy is estimated to be 0.2–0.5 ppmv (4–11%) for the pressure range 68–0.01 hPa. The scientifically useful range of the H2O data is from 316 to 0.002 hPa, although only the 82–0.002 hPa pressure range is validated here. Substantial improvement has been achieved in the v2.2 N2O data over v1.5 by reducing a significant low bias in the stratosphere and eliminating unrealistically high biased mixing ratios in the polar regions. The single‐profile precision is ∼13–25 ppbv (7–38%), the vertical resolution is ∼4–6 km and the accuracy is estimated to be 3–70 ppbv (9–25%) for the pressure range 100–4.6 hPa. The scientifically useful range of the N2O data is from 100 to 1 hPa.