ALBERT

Beschreibung: The biomisation method is used to reconstruct Latin American vegetation at 6000±500 and 18 000±1000 radiocarbon years before present (14C yr BP) from pollen data. Tests using modern pollen data from 381 samples derived from 287 locations broadly reproduce potential natural vegetation. The strong temperature gradient associated with the Andes is recorded by a transition from high altitude cool grass/shrubland and cool mixed forest to mid-altitude cool temperate rain forest, to tropical dry, seasonal and rain forest at low altitudes. Reconstructed biomes from a number of sites do not match the potential vegetation due to local factors such as human impact, methodological artefacts and mechanisms of pollen representivity of the parent vegetation. At 6000±500 14C yr BP 255 samples are analysed from 127 sites. Differences between the modern and the 6000±500 14C yr BP reconstruction are comparatively small. Patterns of change relative to the modern reconstruction are mainly to biomes characteristic of drier climate in the north of the region with a slight more mesic shift in the south. Cool temperate rain forest remains dominant in western South America. In northwestern South America a number of sites record transitions from tropical seasonal forest to tropical dry forest and tropical rain forest to tropical seasonal forest. Sites in Central America also show a change in biome assignment to more mesic vegetation, indicative of greater plant available moisture, e.g. on the Yucatán peninsula sites record warm evergreen forest, replacing tropical dry forest and warm mixed forest presently recorded. At 18 000±1000 14C yr BP 61 samples from 34 sites record vegetation that reflects a generally cool and dry environment. Cool grass/shrubland prevalent in southeast Brazil, Amazonian sites record tropical dry forest, warm temperate rain forest and tropical seasonal forest. Southernmost South America is dominated by cool grass/shrubland, a single site retains cool temperate rain forest indicating that forest was present at some locations at the LGM. Some sites in Central México and lowland Colombia remain unchanged in their biome assignments, although the affinities that these sites have to different biomes do change between 18 000±1000 14C yr BP and present. The "unresponsive" nature of these sites results from their location and the impact of local edaphic influence.

Beschreibung: This paper presents extensive validation analyses of ozone observations from the Atmospheric Chemistry Experiment (ACE) satellite instruments: the ACE Fourier Transform Spectrometer (ACE-FTS) and the Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation (ACE-MAESTRO) instrument. The ACE satellite instruments operate in the mid-infrared and ultraviolet-visible-near-infrared spectral regions using the solar occultation technique. In order to continue the long-standing record of solar occultation measurements from space, a detailed quality assessment is required to evaluate the ACE data and validate their use for scientific purposes. Here we compare the latest ozone data products from ACE-FTS and ACE-MAESTRO with coincident observations from satellite-borne, airborne, balloon-borne and ground-based instruments, by analysing volume mixing ratio profiles and partial column densities. The ACE-FTS version 2.2 Ozone Update product reports more ozone than most correlative measurements from the upper troposphere to the lower mesosphere. At altitude levels from 16 to 44 km, the mean differences range generally between 0 and +10% with a slight but systematic positive bias (typically +5%). At higher altitudes (45–60 km), the ACE-FTS ozone amounts are significantly larger than those of the comparison instruments by up to ~40% (typically +20%). For the ACE-MAESTRO version 1.2 ozone data product, agreement within ±10% (generally better than ±5%) is found between 18 and 40 km for the sunrise and sunset measurements. At higher altitudes (45–55 km), systematic biases of opposite sign are found between the ACE-MAESTRO sunrise and sunset observations. While ozone amounts derived from the ACE-MAESTRO sunrise occultation data are often smaller than the coincident observations (by as much as −10%), the sunset occultation profiles for ACE-MAESTRO show results that are qualitatively similar to ACE-FTS and indicate a large positive bias (+10 to +30%) in this altitude range. In contrast, there is no significant difference in bias found for the ACE-FTS sunrise and sunset measurements. These systematic effects in the ozone profiles retrieved from the measurements of ACE-FTS and ACE-MAESTRO are being investigated. This work shows that the ACE instruments provide reliable, high quality measurements from the tropopause to the upper stratosphere and can be used with confidence in this vertical domain.

Beschreibung: Ultraviolet radiation is the key factor driving tropospheric photochemistry. It is strongly modulated by clouds and aerosols. A quantitative understanding of the radiation field and its effect on photochemistry is thus only possible with a detailed knowledge of the interaction between clouds and radiation. The overall objective of the project INSPECTRO was the characterization of the three-dimensional actinic radiation field under cloudy conditions. This was achieved during two measurement campaigns in Norfolk (East Anglia, UK) and Lower Bavaria (Germany) combining space-based, aircraft and ground-based measurements as well as simulations with the one-dimensional radiation transfer model UVSPEC and the three-dimensional radiation transfer model MYSTIC. During both campaigns the spectral actinic flux density was measured at several locations at ground level and in the air by up to four different aircraft. This allows the comparison of measured and simulated actinic radiation profiles. In addition satellite data were used to complete the information of the three dimensional input data set for the simulation. A three-dimensional simulation of actinic flux density data under cloudy sky conditions requires a realistic simulation of the cloud field to be used as an input for the 3-D radiation transfer model calculations. Two different approaches were applied, to derive high- and low-resolution data sets, with a grid resolution of about 100 m and 1 km, respectively. The results of the measured and simulated radiation profiles as well as the results of the ground based measurements are presented in terms of photolysis rate profiles for ozone and nitrogen dioxide. During both campaigns all spectroradiometer systems agreed within ±10% if mandatory corrections e.g. stray light correction were applied. Stability changes of the systems were below 5% over the 4 week campaign periods and negligible over a few days. The J(O1D) data of the single monochromator systems can be evaluated for zenith angles less than 70°, which was satisfied by nearly all airborne measurements during both campaigns. The comparison of the airborne measurements with corresponding simulations is presented for the total, downward and upward flux during selected clear sky periods of both campaigns. The compliance between the measured (from three aircraft) and simulated downward and total flux profiles lies in the range of ±15%.

Beschreibung: This paper presents extensive {bias determination} analyses of ozone observations from the Atmospheric Chemistry Experiment (ACE) satellite instruments: the ACE Fourier Transform Spectrometer (ACE-FTS) and the Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation (ACE-MAESTRO) instrument. Here we compare the latest ozone data products from ACE-FTS and ACE-MAESTRO with coincident observations from nearly 20 satellite-borne, airborne, balloon-borne and ground-based instruments, by analysing volume mixing ratio profiles and partial column densities. The ACE-FTS version 2.2 Ozone Update product reports more ozone than most correlative measurements from the upper troposphere to the lower mesosphere. At altitude levels from 16 to 44 km, the average values of the mean relative differences are nearly all within +1 to +8%. At higher altitudes (45–60 km), the ACE-FTS ozone amounts are significantly larger than those of the comparison instruments, with mean relative differences of up to +40% (about +20% on average). For the ACE-MAESTRO version 1.2 ozone data product, mean relative differences are within ±10% (average values within ±6%) between 18 and 40 km for both the sunrise and sunset measurements. At higher altitudes (~35–55 km), systematic biases of opposite sign are found between the ACE-MAESTRO sunrise and sunset observations. While ozone amounts derived from the ACE-MAESTRO sunrise occultation data are often smaller than the coincident observations (with mean relative differences down to −10%), the sunset occultation profiles for ACE-MAESTRO show results that are qualitatively similar to ACE-FTS, indicating a large positive bias (mean relative differences within +10 to +30%) in the 45–55 km altitude range. In contrast, there is no significant systematic difference in bias found for the ACE-FTS sunrise and sunset measurements.

Beschreibung: Ultraviolet radiation is the key factor driving tropospheric photochemistry. It is strongly modulated by clouds and aerosols. A quantitative understanding of the radiation field and its effect on photochemistry is thus only possible with a detailed knowledge of the interaction between clouds and radiation. The overall objective of the project INSPECTRO was the characterization of the three-dimensional actinic radiation field under cloudy conditions. This was achieved during two measurement campaigns in Norfolk (East Anglia, UK) and Lower Bavaria (Germany) combining space-based, aircraft and ground-based measurements as well as simulations with the one-dimensional radiation transfer model UVSPEC and the three-dimensional radiation transfer model MYSTIC. During both campaigns the spectral actinic flux density was measured at several locations at ground level and in the air by up to four different aircraft. This allows the comparison of measured and simulated actinic radiation profiles. In addition satellite data were used to complete the information of the three dimensional input data set for the simulation. A three-dimensional simulation of actinic flux density data under cloudy sky conditions requires a realistic simulation of the cloud field to be used as an input for the 3-D radiation transfer model calculations. Two different approaches were applied, to derive high- and low-resolution data sets, with a grid resolution of about 100 m and 1 km, respectively. The results of the measured and simulated radiation profiles as well as the results of the ground based measurements are presented in terms of photolysis rate profiles for ozone and nitrogen dioxide. During both campaigns all spectroradiometer systems agreed within ±10% if mandatory corrections e.g. stray light correction were applied. Stability changes of the systems were below 5% over the 4 week campaign periods and negligible over a few days. The J(O1D) data of the single monochromator systems can be evaluated for zenith angles less than 70°, which was satisfied by nearly all airborne measurements during both campaigns. The comparison of the airborne measurements with corresponding simulations is presented for the total, downward and upward flux during selected clear sky periods of both campaigns. The compliance between the measured (from three aircraft) and simulated downward and total flux profiles lies in the range of ±15%.

Beschreibung: We provide here an overview of, and a summary of results arising from, an extensive experimental campaign (the Spread F Experiment, or SpreadFEx) performed from September to November 2005, with primary measurements in Brazil. The motivation was to define the potential role of neutral atmosphere dynamics, specifically gravity wave motions propagating upward from the lower atmosphere, in seeding Rayleigh-Taylor instability (RTI) and plasma bubbles extending to higher altitudes. Campaign measurements focused on the Brazilian sector and included ground-based optical, radar, digisonde, and GPS measurements at a number of fixed and temporary sites. Related data on convection and plasma bubble structures were also collected by GOES 12, and the GUVI instrument aboard the TIMED satellite. Initial results of our SpreadFEx analyses are described separately by Fritts et al. (2009). Further analyses of these data provide additional evidence of 1) gravity wave (GW) activity near the mesopause apparently linked to deep convection predominantly to the west of our measurement sites, 2) small-scale GWs largely confined to lower altitudes, 3) larger-scale GWs apparently penetrating to much higher altitudes, 4) substantial GW amplitudes implied by digisonde electron densities, and 5) apparent influences of these perturbations in the lower F-region on the formation of equatorial spread F, RTI, and plasma bubbles extending to much higher altitudes. Other efforts with SpreadFEx data have also yielded 6) the occurrence, locations, and scales of deep convection, 7) the spatial and temporal evolutions of plasma bubbles, 8) 2-D (height-resolved) structures in electron density fluctuations and equatorial spread F at lower altitudes and plasma bubbles above, and 9) the occurrence of substantial tidal perturbations to the large-scale wind and temperature fields extending to bottomside F-layer and higher altitudes. Collectively, our various SpreadFEx analyses suggest direct links between deep tropical convection and large GW perturbations at large spatial scales at the bottomside F-layer and their likely contributions to the excitation of RTI and plasma bubbles extending to much higher altitudes.

Beschreibung: The MARSCHALS (Millimetre-wave Airborne Receiver for Spectroscopic CHaracterisation of Atmospheric Limb-Sounding) project has the general objectives of demonstrating the measurement capabilities of a limb viewing instrument working in the millimetre and sub-millimetre spectral regions for the study of the Upper Troposphere – Lower Stratosphere (UTLS). MARSCHALS has flown on board the M-55 stratospheric aircraft (Geophysica) in two measurements campaigns. Here we report the results of the analysis of MARSCHALS measurements during the SCOUT-O3 campaign held in Darwin (Australia) in December 2005 obtained with MARC (Millimetre-wave Atmospheric-Retrieval Code). MARSCHALS measured vertical distributions of Temperature, water vapour, ozone and nitric acid. The retrieval has been performed in the altitude range from 10 to 20 km in presence of clouds that obscure measurements in the middle infrared spectroscopic region. The minimum altitude range is determined by the high water concentration typical of the tropical region rather than the extensive cloud coverage experienced during the flight. The results have been validated using a few measurement made in less cloudy conditions by MIPAS-STR, an infrared limb-viewing instrument on board the M-55 during the same flight.

Beschreibung: Methyl chloride (CH3Cl) is a chlorine-containing trace gas in the atmosphere contributing significantly to stratospheric ozone depletion. Large uncertainties in estimates of its source and sink magnitudes and temporal and spatial variations currently exist. GEIA inventories and other bottom-up emission estimates are used to construct a priori maps of the surface fluxes of CH3Cl. The Model of Atmospheric Transport and Chemistry (MATCH), driven by NCEP interannually varying meteorological data, is then used to simulate CH3Cl mole fractions and quantify the time series of sensitivities of the mole fractions at each measurement site to the surface fluxes of various regional and global sources and sinks. We then implement the Kalman filter (with the unit pulse response method) to estimate the surface fluxes on regional/global scales with monthly resolution from January 2000 to December 2004. High frequency observations from the AGAGE, SOGE, NIES, and NOAA/ESRL HATS in situ networks and low frequency observations from the NOAA/ESRL HATS flask network are used to constrain the source and sink magnitudes. The inversion results indicate global total emissions around 4100±470 Gg yr−1 with very large emissions of 2200±390 Gg yr−1 from tropical plants, which turn out to be the largest single source in the CH3Cl budget. Relative to their a priori annual estimates, the inversion increases global annual fungal and tropical emissions, and reduces the global oceanic source. The inversion implies greater seasonal and interannual oscillations of the natural sources and sink of CH3Cl compared to the a priori. The inversion also reflects the strong effects of the 2002/2003 globally widespread heat waves and droughts on global emissions from tropical plants, biomass burning and salt marshes, and on the soil sink.

Beschreibung: A wide array of volatile organic compound (VOC) measurements was conducted in the Valley of Mexico during the MCMA-2002 and 2003 field campaigns. Study sites included locations in the urban core, in a heavily industrial area and at boundary sites in rural landscapes. In addition, a novel mobile-laboratory-based conditional sampling method was used to collect samples dominated by fresh on-road vehicle exhaust to identify those VOCs whose ambient concentrations were primarily due to vehicle emissions. Five distinct analytical techniques were used: whole air canister samples with Gas Chromatography/Flame Ionization Detection (GC-FID), on-line chemical ionization using a Proton Transfer Reaction Mass Spectrometer (PTR-MS), continuous real-time detection of olefins using a Fast Olefin Sensor (FOS), and long path measurements using UV Differential Optical Absorption Spectrometers (DOAS). The simultaneous use of these techniques provided a wide range of individual VOC measurements with different spatial and temporal scales. The VOC data were analyzed to understand concentration and spatial distributions, diurnal patterns, origin and reactivity in the atmosphere of Mexico City. The VOC burden (in ppbC) was dominated by alkanes (60%), followed by aromatics (15%) and olefins (5%). The remaining 20% was a mix of alkynes, halogenated hydrocarbons, oxygenated species (esters, ethers, etc.) and other unidentified VOCs. However, in terms of ozone production, olefins were the most relevant hydrocarbons. Elevated levels of toxic hydrocarbons, such as 1,3-butadiene, benzene, toluene and xylenes were also observed. Results from these various analytical techniques showed that vehicle exhaust is the main source of VOCs in Mexico City and that diurnal patterns depend on vehicular traffic. Finally, examination of the VOC data in terms of lumped modeling VOC classes and its comparison to the VOC lumped emissions reported in other photochemical air quality modeling studies suggests that some, but not all, VOC classes are underestimated in the emissions inventory by factors of 1.1 to 3.

Beschreibung: The MARSCHALS (Millimetre-wave Airborne Receiver for Spectroscopic CHaracterisation of Atmospheric Limb-Sounding) project has the general objectives of demonstrating the measurement capabilities of a limb viewing instrument working in the millimetre and sub-millimetre spectral regions (from 294 to 349 GHz) for the study of the Upper Troposphere – Lower Stratosphere (UTLS). MARSCHALS has flown on board the M-55 stratospheric aircraft (Geophysica) in two measurements campaigns. Here we report the results of the analysis of MARSCHALS measurements during the SCOUT-O3 campaign held in Darwin (Australia) in December 2005 obtained with MARC (Millimetre-wave Atmospheric-Retrieval Code). MARSCHALS measured vertical distributions of temperature, water vapour, ozone and nitric acid in the altitude range from 10 to 20 km in presence of clouds that obscure measurements in the middle infrared spectroscopic region. The minimum altitude at which the retrieval has been possible is determined by the high water concentration typical of the tropical region rather than the extensive cloud coverage experienced during the flight. Water has been measured from 10 km to flight altitude (~18 km) with a 10% accuracy, ozone from 14 km to flight altitude with accuracy ranging from 10% to 60%, while the retrieval of nitric acid has been possible with an accuracy not better than 40% only from 16 km to flight altitude due to the low signal to noise ratio of its emission in the analysed spectral region. The results have been validated using measurement made in a less cloudy region by MIPAS-STR, an infrared limb-viewing instrument on board the M-55, during the same flight.