Retrieval of XCO2 from simulated Orbiting Carbon Observatory measurements using the fast linearized R-2OS radiative transfer model

In a recent paper, we introduced a novel technique to compute the polarization in a vertically inhomogeneous, scattering-absorbing medium using a two orders of scattering (2OS) radiative transfer (RT) model. The 2OS computation is an order of magnitude faster than a full multiple scattering scalar calculation and can be implemented as an auxiliary code to compute polarization in operational retrieval algorithms. In this paper, we employ the 2OS model for polarization in conjunction with a scalar RT model (Radiant) to simulate backscatter measurements in near infrared (NIR) spectral regions by space-based instruments such as the Orbiting Carbon Observatory (OCO). Computations are performed for six different sites and two seasons, representing a variety of viewing geometries, surface and aerosol types. The aerosol extinction (at 13000 cm^−1) was varied from 0 to 0.3. The radiance errors using the Radiant/2OS (R-2OS) RT model are an order of magnitude (or more) smaller than errors arising from the use of the scalar model alone. In addition, we perform a linear error analysis study to show that the errors in the retrieved column-averaged dry air mole fraction of CO2 (XCO2) using the R-2OS model are much lower than the “measurement” noise and smoothing errors appearing in the inverse model. On the other hand, we show that use of the scalar model alone induces X CO2 errors that could dominate the retrieval error budget

Synthesis of satellite (MODIS), aircraft (ICARTT), and surface (IMPROVE, EPA-AQS, AERONET) aerosol observations over eastern North America to improve MODIS aerosol retrievals and constrain surface aerosol concentrations and sources

We use an ensemble of satellite (MODIS), aircraft, and ground-based aerosol observations during the ICARTT field campaign over eastern North America in summer 2004 to (1) examine the consistency between different aerosol measurements, (2) evaluate a new retrieval of aerosol optical depths (AODs) and inferred surface aerosol concentrations (PM2.5) from the MODIS satellite instrument, and (3) apply this collective information to improve our understanding of aerosol sources. The GEOS-Chem global chemical transport model (CTM) provides a transfer platform between the different data sets, allowing us to evaluate the consistency between different aerosol parameters observed at different times and locations. We use an improved MODIS AOD retrieval based on locally derived visible surface reflectances and aerosol properties calculated from GEOS-Chem. Use of GEOS-Chem aerosol optical properties in the MODIS retrieval not only results in an improved AOD product but also allows quantitative evaluation of model aerosol mass from the comparison of simulated and observed AODs. The aircraft measurements show narrower aerosol size distributions than those usually assumed in models, and this has important implications for AOD retrievals. Our MODIS AOD retrieval compares well to the ground-based AERONET data (R = 0.84, slope = 1.02), significantly improving on the MODIS c005 operational product. Inference of surface PM2.5 from our MODIS AOD retrieval shows good correlation to the EPA-AQS data (R = 0.78) but a high regression slope (slope = 1.48). The high slope is seen in all AOD-inferred PM2.5 concentrations (AERONET: slope = 2.04; MODIS c005: slope = 1.51) and could reflect a clear-sky bias in the AOD observations. The ensemble of MODIS, aircraft, and surface data are consistent in pointing to a model overestimate of sulfate in the mid-Atlantic and an underestimate of organic and dust aerosol in the southeastern United States. The sulfate overestimate could reflect an excessive contribution from aqueous-phase production in clouds, while the organic carbon underestimate could possibly be resolved by a new secondary pathway involving dicarbonyls

Air mass factor formulation for spectroscopic measurements from satellites: Application to formaldehyde retrievals from the Global Ozone Monitoring Experiment

Abstract. We present a new formulation for the air mass factor (AMF) to convert slant column measurements of optically thin atmospheric species from space into total vertical columns. Because of atmospheric scattering, the AMF depends on the vertical distribution of the species. We formulate the AMF as the integral of the relative vertical distribution (shape factor) of the species over the depth of the atmosphere, weighted by altitudedependent coefficients (scattering weights) computed independently from a radiative transfer model. The scattering weights are readily tabulated, and one can then obtain the AMF for any observation scene by using shape factors from a three dimensional (3-D) atmospheric chemistry model for the period of observation. This approach subsequently allows objective evaluation of the 3-D model with the observed vertical columns, since the shape factor and the vertical column in the model represent two independent pieces of information. We demonstrate the AMF method by using slant column measurements of formaldehyde at 346 nm from the Global Ozone Monitoring Experiment satellite instrument over North America during July 1996. Shape factors are computed with the Global Earth Observing System CHEMistry (GEOS-CHEM) global 3-D model and are checked for consistency with the few available aircraft measurements. Scattering weights increase by an order of magnitude from the surface to the upper troposphere. The AMFs are typically 20-40 % less over continents than over the oceans and are approximately half the values calculated in the absence of scattering. Model-induced errors in the AMF are estimated to be • 10%. The GEOS-CHEM model captures 50 % and 60 % of the variances in the observed slant and vertical columns, respectively. Comparison of the simulated and observed vertical columns allows assessment of model bias. 1

Effects of the physical state of tropospheric ammonium-sulfate-nitrate particles on global aerosol direct radiative forcing

International audienceThe effect of aqueous versus crystalline sulfate-nitrate-ammonium tropospheric particles on global aerosol direct radiative forcing is assessed. A global three-dimensional chemical transport model predicts sulfate, nitrate, and ammonium aerosol mass. An aerosol thermodynamics model is called twice, once for the upper side (US) and once for lower side (LS) of the hysteresis loop of particle phase. On the LS, the sulfate mass budget is 40% solid ammonium sulfate, 12% letovicite, 11% ammonium bisulfate, and 37% aqueous. The LS nitrate mass budget is 26% solid ammonium nitrate, 7% aqueous, and 67% gas-phase nitric acid release due to increased volatility upon crystallization. The LS ammonium budget is 45% solid ammonium sulfate, 10% letovicite, 6% ammonium bisulfate, 4% ammonium nitrate, 7% ammonia release due to increased volatility, and 28% aqueous. LS aerosol water mass partitions as 22% effloresced to the gas-phase and 78% remaining as aerosol mass. The predicted US/LS global fields of aerosol mass are employed in a Mie scattering model to generate global US/LS aerosol optical properties, including scattering efficiency, single scattering albedo, and asymmetry parameter. Global annual average LS optical depth and mass scattering efficiency are, respectively, 0.023 and 10.7 m2 (g SO42?)?1, which compare to US values of 0.030 and 13.9 m2 (g SO42?)?1. Radiative transport is computed, first for a base case having no aerosol and then for the two global fields corresponding to the US and LS of the hysteresis loop. Regional, global, seasonal, and annual averages of top-of-the-atmosphere aerosol radiative forcing on the LS and US (FL and FU, respectively, in W m2?) are calculated. Including both anthropogenic and natural emissions, we obtain global annual averages of FL = ?0.750, FU = ?0.930, and ?FU,L = 24% for full sky calculations without clouds and FL = ?0.485, FU = ?0.605, and ?FU,L = 25% when clouds are included. Regionally, ?FU,L = 48% over the USA, 55% over Europe, and 34% over East Asia. Seasonally, ?FU,L varies from 18% in DJF to 75% in SON over the USA. The global annual average contribution from anthropogenic aerosol is FL = ?0.314 and FU = ?0.404, which yield normalized direct radiative forcings (G) of GL = ?205 W (g SO42?)?1 and GU = ?264 W (g SO42?)?1

Geophysical validation and long-term consistency between GOME-2/MetOp-A total ozone column and measurements from the sensors GOME/ERS-2, SCIAMACHY/ENVISAT and OMI/Aura

The main aim of the paper is to assess the consistency of five years of Global Ozone Monitoring Experiment-2/Metop-A [GOME-2] total ozone columns and the long-term total ozone satellite monitoring database already in existence through an extensive inter-comparison and validation exercise using as reference Brewer and Dobson ground-based measurements. The behaviour of the GOME-2 measurements is being weighed against that of GOME (1995–2011), Ozone Monitoring Experiment [OMI] (since 2004) and the Scanning Imaging Absorption spectroMeter for Atmospheric CartograpHY [SCIAMACHY] (since 2002) total ozone column products. Over the background truth of the ground-based measurements, the total ozone columns are inter-evaluated using a suite of established validation techniques; the GOME-2 time series follow the same patterns as those observed by the other satellite sensors. In particular, on average, GOME-2 data underestimate GOME data by about 0.80%, and underestimate SCIAMACHY data by 0.37% with no seasonal dependence of the differences between GOME-2, GOME and SCIAMACHY. The latter is expected since the three datasets are based on similar DOAS algorithms. This underestimation of GOME-2 is within the uncertainty of the reference data used in the comparisons. Compared to the OMI sensor, on average GOME-2 data underestimate OMI_DOAS (collection 3) data by 1.28%, without any significant seasonal dependence of the differences between them. The lack of seasonality might be expected since both the GOME data processor [GDP] 4.4 and OMI_DOAS are DOAS-type algorithms and both consider the variability of the stratospheric temperatures in their retrievals. Compared to the OMI_TOMS (collection 3) data, no bias was found. We hence conclude that the GOME-2 total ozone columns are well suitable to continue the long-term global total ozone record with the accuracy needed for climate monitoring studies

Synthesis of Satellite (MODIS), Aircraft (ICARTT), and Surface (IMPROVE, EPA-AQS, AERONET) Aerosol Observations over Eastern North America to Improve MODIS Aerosol Retrievals and Constrain Surface Aerosol Concentrations and Sources

We use an ensemble of satellite (MODIS), aircraft, and ground-based aerosol observations during the ICARTT field campaign over eastern North America in summer 2004 to (1) examine the consistency between different aerosol measurements, (2) evaluate a new retrieval of aerosol optical depths (AODs) and inferred surface aerosol concentrations $(PM_{2.5})$ from the MODIS satellite instrument, and (3) apply this collective information to improve our understanding of aerosol sources. The GEOS-Chem global chemical transport model (CTM) provides a transfer platform between the different data sets, allowing us to evaluate the consistency between different aerosol parameters observed at different times and locations. We use an improved MODIS AOD retrieval based on locally derived visible surface reflectances and aerosol properties calculated from GEOS-Chem. Use of GEOS-Chem aerosol optical properties in the MODIS retrieval not only results in an improved AOD product but also allows quantitative evaluation of model aerosol mass from the comparison of simulated and observed AODs. The aircraft measurements show narrower aerosol size distributions than those usually assumed in models, and this has important implications for AOD retrievals. Our MODIS AOD retrieval compares well to the ground-based AERONET data (R = 0.84, slope = 1.02), significantly improving on the MODIS c005 operational product. Inference of surface $PM_{2.5}$ from our MODIS AOD retrieval shows good correlation to the EPA-AQS data (R = 0.78) but a high regression slope (slope = 1.48). The high slope is seen in all AOD-inferred $PM_{2.5}$ concentrations (AERONET: slope = 2.04; MODIS c005: slope = 1.51) and could reflect a clear-sky bias in the AOD observations. The ensemble of MODIS, aircraft, and surface data are consistent in pointing to a model overestimate of sulfate in the mid-Atlantic and an underestimate of organic and dust aerosol in the southeastern United States. The sulfate overestimate could reflect an excessive contribution from aqueous-phase production in clouds, while the organic carbon underestimate could possibly be resolved by a new secondary pathway involving dicarbonyls.Engineering and Applied Science

Effects of the physical state of tropospheric ammonium-sulfate-nitrate particles on global aerosol direct radiative forcing

The effect of aqueous versus crystalline sulfate-nitrate-ammonium tropospheric particles on global aerosol direct radiative forcing is assessed. A global three-dimensional chemical transport model predicts sulfate, nitrate, and ammonium aerosol mass. An aerosol thermodynamics model is called twice, once for the upper side (US) and once for lower side (LS) of the hysteresis loop of particle phase. On the LS, the sulfate mass budget is 40% solid ammonium sulfate, 12% letovicite, 11% ammonium bisulfate, and 37% aqueous. The LS nitrate mass budget is 26% solid ammonium nitrate, 7% aqueous, and 67% gas-phase nitric acid release due to increased volatility upon crystallization. The LS ammonium budget is 45% solid ammonium sulfate, 10% letovicite, 6% ammonium bisulfate, 4% ammonium nitrate, 7% ammonia release due to increased volatility, and 28% aqueous. LS aerosol water mass partitions as 22% effloresced to the gas-phase and 78% remaining as aerosol mass. The predicted US/LS global fields of aerosol mass are employed in a Mie scattering model to generate global US/LS aerosol optical properties, including scattering efficiency, single scattering albedo, and asymmetry parameter. Global annual average LS optical depth and mass scattering efficiency are, respectively, 0.023 and 10.7 m² (g SO₄^-2)^-1, which compare to US values of 0.030 and 13.9 m² (g SO₄^-2)^-1. Radiative transport is computed, first for a base case having no aerosol and then for the two global fields corresponding to the US and LS of the hysteresis loop. Regional, global, seasonal, and annual averages of top-of-the-atmosphere aerosol radiative forcing on the LS and US (<i>F_L </i> and <i>F_U</i>, respectively, in W m^-2) are calculated. Including both anthropogenic and natural emissions, we obtain global annual averages of <i>F_L</i>=-0.750, <i>F_U</i>=-0.930, and <font face='Symbol'>D</font><i>F_U,L</i>=24% for full sky calculations without clouds and <i>F_L</i>=-0.485, <i>F_U</i>=-0.605, and <font face='Symbol'>D</font><i>F_U,L</i>=25% when clouds are included. Regionally, <font face='Symbol'>D</font><i>F_U,L</i>=48% over the USA, 55% over Europe, and 34% over East Asia. Seasonally, <font face='Symbol'>D</font><i>F_U,L</i>varies from 18% in DJF to 75% in SON over the USA. The global annual average contribution from anthropogenic aerosol is <i>F_L</i>=-0.314 and <i>F_U</i>=-0.404, which yield normalized direct radiative forcings (<i>G</i>) of <i>G_L</i>=-205 W (g SO₄^-2)^-1 and <i>G_U</i>=-264 W (g SO₄^-2)^-1

Effects of the physical state of tropospheric ammonium-sulfate-nitrate particles on global aerosol direct radiative forcing

International audienceThe effect of aqueous versus crystalline sulfate-nitrate-ammonium tropospheric particles on global aerosol direct radiative forcing is assessed. A global three-dimensional chemical transport model predicts sulfate, nitrate, and ammonium aerosol mass. An aerosol thermodynamics model is called twice, once for the upper side (US) and once for lower side (LS) of the hysteresis loop of particle phase. On the LS, the sulfate mass budget is 40% solid ammonium sulfate, 12% letovicite, 11% ammonium bisulfate, and 37% aqueous. The LS nitrate mass budget is 26% solid ammonium nitrate, 7% aqueous, and 67% gas-phase nitric acid release due to increased volatility upon crystallization. The LS ammonium budget is 45% solid ammonium sulfate, 10% letovicite, 6% ammonium bisulfate, 4% ammonium nitrate, 7% ammonia release due to increased volatility, and 28% aqueous. LS aerosol water mass partitions as 22% effloresced to the gas-phase and 78% remaining as aerosol mass. The predicted US/LS global fields of aerosol mass are employed in a Mie scattering model to generate global US/LS aerosol optical properties, including scattering efficiency, single scattering albedo, and asymmetry parameter. Global annual average LS optical depth and mass scattering efficiency are, respectively, 0.023 and 10.7 m2 (g SO4-2)-1, which compare to US values of 0.030 and 13.9 m2 (g SO4-2)-1. Radiative transport is computed, first for a base case having no aerosol and then for the two global fields corresponding to the US and LS of the hysteresis loop. Regional, global, seasonal, and annual averages of top-of-the-atmosphere aerosol radiative forcing on the LS and US (FL and FU, respectively, in W m-2) are calculated. Including both anthropogenic and natural emissions, we obtain global annual averages of FL=-0.750, FU=-0.930, and DFU,L=24% for full sky calculations without clouds and FL=-0.485, FU=-0.605, and DFU,L=25% when clouds are included. Regionally, DFU,L=48% over the USA, 55% over Europe, and 34% over East Asia. Seasonally, DFU,L varies from 18% in DJF to 75% in SON over the USA. The global annual average contribution from anthropogenic aerosol is FL=-0.314 and FU=-0.404, which yield normalized direct radiative forcings (G) of GL=-205 W (g SO4-2)-1 and GU=-264 W (g SO4-2)-1

The validation of a computer-based food record for older adults: the Novel Assessment of Nutrition and Ageing (NANA) method

Dietary assessment in older adults can be challenging. The Novel Assessment of Nutrition and Ageing (NANA) method is a touch-screen computer-based food record that enables older adults to record their dietary intakes. The objective of the present study was to assess the relative validity of the NANA method for dietary assessment in older adults. For this purpose, three studies were conducted in which a total of ninety-four older adults (aged 65–89 years) used the NANA method of dietary assessment. On a separate occasion, participants completed a 4 d estimated food diary. Blood and 24 h urine samples were also collected from seventy-six of the volunteers for the analysis of biomarkers of nutrient intake. The results from all the three studies were combined, and nutrient intake data collected using the NANA method were compared against the 4 d estimated food diary and biomarkers of nutrient intake. Bland–Altman analysis showed a reasonable agreement between the dietary assessment methods for energy and macronutrient intake; however, there were small, but significant, differences for energy and protein intake, reflecting the tendency for the NANA method to record marginally lower energy intakes. Significant positive correlations were observed between urinary urea and dietary protein intake using both the NANA and the 4 d estimated food diary methods, and between plasma ascorbic acid and dietary vitamin C intake using the NANA method. The results demonstrate the feasibility of computer-based dietary assessment in older adults, and suggest that the NANA method is comparable to the 4 d estimated food diary, and could be used as an alternative to the food diary for the short-term assessment of an individual’s dietary intake