Hygroscopic growth of atmospheric aerosol particles based on active remote sensing and radiosounding measurements: selected cases in southeastern Spain

A new methodology based on combining active and passive remote sensing and simultaneous and collocated radiosounding data to study the aerosol hygroscopic growth effects on the particle optical and microphysical properties is presented. The identification of hygroscopic growth situations combines the analysis of multispectral aerosol particle backscatter coefficient and particle linear depolarization ratio with thermodynamic profiling of the atmospheric column. We analyzed the hygroscopic growth effects on aerosol properties, namely the aerosol particle backscatter coefficient and the volume concentration profiles, using data gathered at Granada EARLINET station. Two study cases, corresponding to different aerosol loads and different aerosol types, are used for illustrating the potential of this methodology. Values of the aerosol particle backscatter coefficient enhancement factors range from 2.1 ± 0.8 to 3.9 ± 1.5, in the ranges of relative humidity 60–90 and 40–83%, being similar to those previously reported in the literature. Differences in the enhancement factor are directly linked to the composition of the atmospheric aerosol. The largest value of the aerosol particle backscatter coefficient enhancement factor corresponds to the presence of sulphate and marine particles that are more affected by hygroscopic growth. On the contrary, the lowest value of the enhancement factor corresponds to an aerosol mixture containing sulphates and slight traces of mineral dust. The Hänel parameterization is applied to these case studies, obtaining results within the range of values reported in previous studies, with values of the γ exponent of 0.56 ± 0.01 (for anthropogenic particles slightly influenced by mineral dust) and 1.07 ± 0.01 (for the situation dominated by anthropogenic particles), showing the convenience of this remote sensing approach for the study of hygroscopic effects of the atmospheric aerosol under ambient unperturbed conditions. For the first time, the retrieval of the volume concentration profiles for these cases using the Lidar Radiometer Inversion Code (LIRIC) allows us to analyze the aerosol hygroscopic growth effects on aerosol volume concentration, observing a stronger increase of the fine mode volume concentration with increasing relative humidity.

Comparison of co-located independent ground-based middle atmospheric wind and temperature measurements with numerical weather prediction models

High-resolution, ground-based and independent observations including co-located wind radiometer, lidar stations, and infrasound instruments are used to evaluate the accuracy of general circulation models and data-constrained assimilation systems in the middle atmosphere at northern hemisphere midlatitudes. Systematic comparisons between observations, the European Centre for Medium-Range Weather Forecasts (ECMWF) operational analyses including the recent Integrated Forecast System cycles 38r1 and 38r2, the NASA’s Modern-Era Retrospective Analysis for Research and Applications (MERRA) reanalyses, and the free-running climate Max Planck Institute–Earth System Model–Low Resolution (MPI-ESM-LR) are carried out in both temporal and spectral dom ains. We find that ECMWF and MERRA are broadly consistent with lidar and wind radiometer measurements up to ~40 km. For both temperature and horizontal wind components, deviations increase with altitude as the assimilated observations become sparser. Between 40 and 60 km altitude, the standard deviation of the mean difference exceeds 5 K for the temperature and 20 m/s for the zonal wind. The largest deviations are observed in winter when the variability from large-scale planetary waves dominates. Between lidar data and MPI-ESM-LR, there is an overall agreement in spectral amplitude down to 15–20 days. At shorter time scales, the variability is lacking in the model by ~10 dB. Infrasound observations indicate a general good agreement with ECWMF wind and temperature products. As such, this study demonstrates the potential of the infrastructure of the Atmospheric Dynamics Research Infrastructure in Europe project that integrates various measurements and provides a quantitative understanding of stratosphere-troposphere dynamical coupling for numerical weather prediction applications.

High-resolution AMS (super 14) C dating of post-bomb peat archives of atmospheric pollutants.

Peat deposits in Greenland and Denmark were investigated to show that high-resolution dating of these archives of atmospheric deposition can be provided for the last 50 years by radiocarbon dating using the atmospheric bomb pulse. (super 14) C was determined in macrofossils from sequential one cm slices using accelerator mass spectrometry (AMS). Values were calibrated with a general-purpose curve derived from annually averaged atmospheric (super 14) CO (sub 2) values in the northernmost northern hemisphere (NNH, 30 degrees -90 degrees N). We present a through review of (super 14) C bomb-pulse data from the NNH including our own measurements made in tree rings and seeds from Arizona as well as other previously published data. We show that our general-purpose calibration curve is valid for the whole NNH producing accurate dates within 1-2 years. In consequence, (super 14) C AMS can precisely date individual points in recent peat deposits within the range of the bomb-pulse (from the mid-1950s on). Comparing the (super 14) C AMS results with the customary dating method for recent peat profiles by (super 210) Pb, we show that the use of (super 137) Cs to validate and correct (super 210) Pb dates proves to be more problematic than previously supposed. As a unique example of our technique, we show how this chronometer can be applied to identify temporal changes in Hg concentrations from Danish and Greenland peat cores.

Covariation of deep Southern Ocean oxygenation and atmospheric CO2 through the last ice age

No single mechanism can account for the full amplitude of past atmospheric carbon dioxide (CO2) concentration variability over glacial–interglacial cycles. A build-up of carbon in the deep ocean has been shown to have occurred during the Last Glacial Maximum. However, the mechanisms responsible for the release of the deeply sequestered carbon to the atmosphere at deglaciation, and the relative importance of deep ocean sequestration in regulating millennial-timescale variations in atmospheric CO2 concentration before the Last Glacial Maximum, have remained unclear. Here we present sedimentary redox-sensitive trace metal records from the Antarctic Zone of the Southern Ocean that provide a reconstruction of transient changes in deep ocean oxygenation and, by inference, respired carbon storage throughout the last glacial cycle. Our data suggest that respired carbon was removed from the abyssal Southern Ocean during the Northern Hemisphere cold phases of the deglaciation, when atmospheric CO2 concentration increased rapidly, reflecting—at least in part— a combination of dwindling iron fertilization by dust and enhanced deep ocean ventilation. Furthermore, our records show that the observed covariation between atmospheric CO2 concentration and abyssal Southern Ocean oxygenation was maintained throughout most of the past 80,000 years. This suggests that on millennial timescales deep ocean circulation and iron fertilization in the Southern Ocean played a consistent role in modifying atmospheric CO2 concentration.

Biological and physical controls in the Southern Ocean on past millennial-scale atmospheric CO2 changes

Millennial-scale climate changes during the last glacial period and deglaciation were accompanied by rapid changes in atmospheric CO2 that remain unexplained. While the role of the Southern Ocean as a ’control valve’ on ocean–atmosphere CO2 exchange has been emphasized, the exact nature of this role, in particular the relative contributions of physical (for example, ocean dynamics and air–sea gas exchange) versus biological processes (for example, export productivity), remains poorly constrained. Here we combine reconstructions of bottom-water [O2], export production and 14C ventilation ages in the sub-Antarctic Atlantic, and show that atmospheric CO2 pulses during the last glacial- and deglacial periods were consistently accompanied by decreases in the biological export of carbon and increases in deep-ocean ventilation via southern-sourced water masses. These findings demonstrate how the Southern Ocean’s ’organic carbon pump’ has exerted a tight control on atmospheric CO2, and thus global climate, specifically via a synergy of both physical and biological processes.

History of Atmospheric Lead Deposition Since 12,370 14C yr BP from a Peat Bog, Jura Mountains, Switzerland

A continuous record of atmospheric lead since 12,370 carbon-14 years before the present (14C yr BP) is preserved in a Swiss peat bog. Enhanced fluxes caused by climate changes reached their maxima 10,590 14C yr BP (Younger Dryas) and 823014C yr BP. Soil erosion caused by forest clearing and agricultural tillage increased lead deposition after 532014C yr BP. Increasing lead/scandium and decreasing lead-206/lead-207 beginning 3000 14C yr BP indicate the beginning of lead pollution from mining and smelting, and anthropogenic sources have dominated lead emissions ever since. The greatest lead flux (15.7 milligrams per square meter per year in A.D. 1979) was 1570 times the natural, background value (0.01 milligram per square meter per year from 8030 to 5320 14C yr BP).

Integrated Data Sets of the EU FP5 Research Project ORFOIS: Origin and fate of biogenic particle fluxes in the ocean and their interactions with atmospheric CO2 concentrations as well as the marine sediment

For a reliable simulation of the time and space dependent CO2 redistribution between ocean and atmosphere an appropriate time dependent simulation of particle dynamics processes is essential but has not been carried out so far. The major difficulties were the lack of suitable modules for particle dynamics and early diagenesis (in order to close the carbon and nutrient budget) in ocean general circulation models, and the lack of an understanding of biogeochemical processes, such as the partial dissolution of calcareous particles in oversaturated water. The main target of ORFOIS was to fill in this gap in our knowledge and prediction capability infrastructure. This goal has been achieved step by step. At first comprehensive data bases (already existing data) of observations of relevance for the three major types of biogenic particles, organic carbon (POC), calcium carbonate (CaCO3), and biogenic silica (BSi or opal), as well as for refractory particles of terrestrial origin were collated and made publicly available.