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First retrieval of tropospheric aerosol profiles using MAX-DOAS and comparison with lidar and sky radiometer measurements

Ground-based Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements were performed at Tsukuba, Japan (36.1° N, 140.1° E), in November–December 2006. By analyzing the measured spectra of scattered sunlight with DOAS and optimal estimation methods, we first retrieve the aerosol optical depth (τ) and the vertical profile of the aerosol extinction coefficient (k) at 476 nm in the lower troposphere. These retrieved quantities are characterized through comparisons with coincident lidar and sky radiometer measurements. The retrieved k values for layers of 0–1 and 1–2 km agree with lidar data to within 30% and 60%, respectively, for most cases, including partly cloudy conditions. Results similar to k at 0–1 km are obtained for the retrieved τ values, demonstrating that MAX-DOAS provides a new, unique aerosol dataset in the lower troposphere.
N2O release from agro-biofuel production negates global warming reduction by replacing fossil fuels

The relationship, on a global basis, between the amount of N fixed by chemical, biological or atmospheric processes entering the terrestrial biosphere, and the total emission of nitrous oxide (N2O), has been re-examined, using known global atmospheric removal rates and concentration growth of N2O as a proxy for overall emissions. For both the pre-industrial period and in recent times, after taking into account the large-scale changes in synthetic N fertiliser production, we find an overall conversion factor of 3–5% from newly fixed N to N2O-N. We assume the same factor to be valid for biofuel production systems. It is covered only in part by the default conversion factor for "direct" emissions from agricultural crop lands (1%) estimated by IPCC (2006), and the default factors for the "indirect" emissions (following volatilization/deposition and leaching/runoff of N: 0.35–0.45%) cited therein. However, as we show in the paper, when additional emissions included in the IPCC methodology, e.g. those from livestock production, are included, the total may not be inconsistent with that given by our "top-down" method. When the extra N2O emission from biofuel production is calculated in "CO2-equivalent" global warming terms, and compared with the quasi-cooling effect of "saving" emissions of fossil fuel derived CO2, the outcome is that the production of commonly used biofuels, such as biodiesel from rapeseed and bioethanol from corn (maize), depending on N fertilizer uptake efficiency by the plants, can contribute as much or more to global warming by N2O emissions than cooling by fossil fuel savings. Crops with less N demand, such as grasses and woody coppice species, have more favourable climate impacts. This analysis only considers the conversion of biomass to biofuel. It does not take into account the use of fossil fuel on the farms and for fertilizer and pesticide production, but it also neglects the production of useful co-products. Both factors partially compensate each other. This needs to be analyzed in a full life cycle assessment.
Past and future scenarios of the effect of carbon dioxide on plant growth and transpiration for three vegetation types of southwestern France

The sensitivity of an operational CO2-responsive land surface model (the ISBA-A-gs model of Météo-France) to the atmospheric CO2 concentration, (CO2), is investigated for 3 vegetation types (winter wheat, irrigated maize, coniferous forest). Past (1960) and future (2050) scenarios of (CO2) corresponding to 320 ppm and 550 ppm, respectively, are explored. The sensitivity study is performed for 4 annual cycles presenting contrasting conditions of precipitation regime and air temperature, based on continuous measurements performed on the SMOSREX site near Toulouse, in southwestern France. A significant CO2-driven reduction of canopy conductance is simulated for the irrigated maize and the coniferous forest. The reduction is particularly large for maize, from 2000 to 2050 (−18%), and triggers a drop in optimum irrigation (−30 mm y−1). In the case of wheat, the response is more complex, with an equal occurrence of enhanced or reduced canopy conductance.
VOC reactivity in central California: comparing an air quality model to ground-based measurements

Volatile organic compound (VOC) reactivity in central California is examined using a photochemical air quality model (the Community Multiscale Air Quality model; CMAQ) and ground-based measurements to evaluate the contribution of VOC to photochemical activity. We classify VOC into four categories: anthropogenic, biogenic, aldehyde, and other oxygenated VOC. Anthropogenic and biogenic VOC consist of primary emissions, while aldehydes and other oxygenated VOC include both primary anthropogenic emissions and secondary products from primary VOC oxidation. To evaluate the model treatment of VOC chemistry, we compare calculated and modeled OH and VOC reactivities using the following metrics: 1) cumulative distribution functions of NOx concentration and VOC reactivity (ROH,VOC), 2) the relationship between ROH,VOC and NOx, 3) total OH reactivity (ROH,total) and speciated contributions, and 4) the relationship between speciated ROH,VOC and NOx. We find that the model predicts ROH,total to within 25–40% at three sites representing urban (Sacramento), suburban (Granite Bay) and rural (Blodgett Forest) chemistry. However in the urban area of Fresno, the model under predicts NOx and VOC emissions by a factor of 2–3. At all locations the model is consistent with observations of the relative contributions of total VOC. In urban areas, anthropogenic and biogenic ROH,VOC are predicted fairly well over a range of NOx conditions. In suburban and rural locations, anthropogenic and other oxygenated ROH,VOC relationships are reproduced, but calculated biogenic and aldehyde ROH,VOC are often poorly characterized by measurements, making evaluation of the model with available data unreliable. In central California, 30–50% of the modeled urban VOC reactivity is due to aldehydes and other oxygenated species, and the total oxygenated ROH,VOC is nearly equivalent to anthropogenic VOC reactivity. In rural vegetated regions, biogenic and aldehyde reactivity dominates. This indicates that more attention needs to be paid to the accuracy of models and measurements of both primary emissions of oxygenated VOC and secondary production of oxygenates, especially formaldehyde and other aldehydes, and that a more comprehensive set of oxygenated VOC measurements is required to include all of the important contributions to atmospheric reactivity.
Impacts of the solar eclipse of 29 March 2006 on the surface ozone concentration, the solar ultraviolet radiation and the meteorological parameters at Athens, Greece

In this study the variations in the surface ozone concentration, the solar ultraviolet radiation and the meteorological parameters at the ground before, during and after the total solar eclipse of 29 March 2006 have been examined. This analysis is based on the measurements performed at four stations located in the greater Athens basin in Greece. The experimental data demonstrated that the solar eclipse phenomenon affects the surface ozone concentration as well as the temperature, the relative humidity and the wind speed near the ground. The decrease in the surface ozone concentration that observed after the beginning of the eclipse event lasted almost two hours, probably due to the decreased efficiency of the photochemical ozone formation. The reduction of the solar ultraviolet radiation at 312 and 365 nm reached 97% and 93% respectively, while the air temperature dropped, the relative humidity increased and the wind speed decreased.
Chemical composition of free tropospheric aerosol for PM1 and coarse mode at the high alpine site Jungfraujoch

The chemical composition of submicron (fine mode) and supermicron (coarse mode) aerosol particles has been investigated at the Jungfraujoch high alpine research station (3580 m a.s.l., Switzerland) as part of the GAW aerosol monitoring program since 1999. A clear seasonality was observed for all major components throughout the period with low concentrations in winter (predominantly free tropospheric aerosol) and higher concentrations in summer (enhanced vertical transport of boundary layer pollutants). In addition, mass closure was attempted during intensive campaigns in March 2004, February–March 2005 and August 2005. Ionic, carbonaceous and non-refractory components of the aerosol were quantified as well as the PM1 and coarse mode total aerosol mass concentrations. A relatively low conversion factor of 1.8 for organic carbon (OC) to particulate organic matter (OM) was found in winter (February–March 2005). Organics, sulfate, ammonium, and nitrate were the major components of the fine aerosol fraction that were identified, while calcium and nitrate were the only two measured components contributing to the coarse mode. The aerosol mass concentrations for fine and coarse mode aerosol measured during the intensive campaigns were not typical of the long-term seasonality due largely to dynamical differences. Average fine and coarse mode concentrations during the intensive field campaigns were 1.7 μg m−3 and 2.4 μg m−3 in winter and 2.5 μg m−3 and 2.0 μg m−3 in summer, respectively. The mass balance of aerosols showed higher contributions of calcium and nitrate in the coarse mode during Saharan dust events (SDE) than without SDE.
A compact and stable eddy covariance set-up for methane measurements using off-axis integrated cavity output spectroscopy

A Fast Methane Analyzer (FMA) is assessed for its applicability in a closed path eddy covariance field set-up in a peat meadow. The FMA uses off-axis integrated cavity output spectroscopy combined with a highly specific narrow band laser for the detection of CH4 and strongly reflective mirrors to obtain a laser path length of 2–20×103 m. Statistical testing and a calibration experiment showed high precision (7.8×10−3 ppb) and accuracy (<0.30%) of the instrument, while no drift was observed. The instrument response time was determined to be 0.10 s. In the field set-up, the FMA is attached to a scroll pump and combined with a 3-axis ultrasonic anemometer and an open path infrared gas analyzer for measurements of carbon dioxide and water vapour. The power-spectra and co-spectra of the instruments were satisfactory for 10 Hz sampling rates. Due to erroneous measurements, spikes and periods of low turbulence the data series consisted for 26% of gaps. Observed CH4 fluxes consisted mainly of emission, showed a diurnal cycle, but were rather variable over. The average CH4 emission was 29.7 nmol m−2 s−1, while the typical maximum CH4 emission was approximately 80.0 nmol m−2 s−1 and the typical minimum flux was approximately 0.0 nmol m−2 s−1. The correspondence of the measurements with flux chamber measurements in the footprint was good and the observed CH4 emission rates were comparable with eddy covariance CH4 measurements in other peat areas. Additionally, three measurement techniques with lower sampling frequencies were simulated, which might give the possibility to measure CH4 fluxes without an external pump and save energy. Disjunct eddy covariance appeared to be the most reliable substitute for 10 Hz eddy covariance, while relaxed eddy accumulation gave reliable estimates of the fluxes over periods in the order of days or weeks.
Changes in aerosol properties during spring-summer period in the Arctic troposphere

The change in aerosol properties during the transition from the more polluted spring to the clean summer in the Arctic troposphere was studied. A six-year data set of observations from Ny-Ålesund on Svalbard, covering the months April through June, serve as the basis for the characterisation of this time period. In addition four-day-back trajectories were used to describe air mass histories. The observed transition in aerosol properties from an accumulation-mode dominated distribution to an Aitken-mode dominated distribution is discussed with respect to long-range transport and influences from natural and anthropogenic sources of aerosols and pertinent trace gases. Our study shows that the air-mass transport is an important factor modulating the physical and chemical properties observed. However, the air-mass transport cannot alone explain the annually repeated systematic and rather rapid change in aerosol properties, occurring within a limited time window of approximately 10 days. With a simplified phenomenological model, which delivers the nucleation potential for new-particle formation, we suggest that the rapid shift in aerosol microphysical properties between the Arctic spring and summer is mainly driven by the incoming solar radiation in concert with transport of precursor gases and changes in condensational sink.
The relationship between tropospheric wave forcing and tropical lower stratospheric water vapor

Using water vapor data from HALOE and SAGE II, an anti-correlation between planetary wave driving (here expressed by the mid-latitude eddy heat flux at 50 hPa added from both hemispheres) and tropical lower stratospheric (TLS) water vapor has been obtained. This appears to be a manifestation of the inter-annual variability of the Brewer-Dobson (BD) circulation strength (the driving of which is generally measured in terms of the mid-latitude eddy heat flux), and hence amount of water vapor entering the stratosphere. Some years such as 1991 and 1997 show, however, a clear departure from the anti-correlation which suggests that the water vapor changes in TLS can not be attributed solely to changes in extratropical planetary wave activity (and its effect on the BD circulation). After 2000 a sudden decrease in lower stratospheric water vapor has been reported in earlier studies based upon satellite data from HALOE, SAGE II and POAM III indicating that the lower stratosphere has become drier since then. This is consistent with a sudden rise in the combined mid-latitude eddy heat flux with nearly equal contribution from both hemispheres as shown here and with the increase in tropical upwelling and decrease in cold point temperatures found by Randel et al. (2006). The low water vapor and enhanced planetary wave activity (in turn strength of the BD circulation) has persisted until the end of the satellite data records. From a multi-variate regression analysis applied to 27 years of NCEP and HadAT2 (radiosonde) temperatures (up to 2005) with contributions from solar cycle, stratospheric aerosols and QBO removed, the enhancement wave driving after 2000 is estimated to contribute up to 0.7 K cooling to the overall TLS temperature change during the period 2001–2005 when compared to the period 1996–2000. NCEP cold point temperature show an average decrease of nearly 0.4 K from changes in the wave driving, which is consistent with observed mean TLS water vapor changes of about −0.2 ppm after 2000.
Some considerations about Ångström exponent distributions

A simulation study has been performed in order to show the influence of the aerosol optical depth (AOD) distribution together with the corresponding error distribution on the resulting Ångström exponent (AE) distribution. It will be shown that the Ångström exponent frequency of occurrence distribution is only normal distributed when the relative error at the two wavelengths used for estimation of the Ångström exponent is the same. In all other cases a shift of the maximum of the AE-distribution will occur. It will be demonstrated that the Ångström exponent (or the maximum of an AE distribution) will be systematically over- or underestimated depending on whether the relative error of the shorter wavelength is larger or smaller compared with the relative error of the longer wavelength. In such cases the AE distribution are also skewed.