Background Aerosol Conditions Research Articles

Optimization of the Polarized Imaging Nephelometer (PI-Neph) for continuous monitoring of multiwavelength aerosol phase functions in support of space polarimetry missions

This work deals with the set up and optimization of a commercial multiwavelength polarized imaging nephelometer (PI-Neph, Airphoton PIN100) designed to measure F11 (phase function) and –F12/F11 (polarized phase function) from ambient aerosol samples. Such measurements are critical for the success of upcoming satellite missions based on polarimetry measurements because they will support and validate retrieval techniques. The main novelty of the instrument with respect to previous versions consists of using only one beam instead of a mirror system to fold it, avoiding internal reflections of light and loss of energy within the laser beam. The instrument also includes the automatization of the imaging technique that makes possible continuous measurements in near real time of the aerosol phase functions at different states of linear polarization directly from ambient air. Laser emits at three different wavelengths (405, 515 and 660 nm) and the beam goes through a wire grid polarizer for linearly polarizing the light, followed by two liquid crystal retarders that control the state of linear polarization. The detector is a CMOS camera perpendicular to the beam which allows to obtain final phase functions in the range 5°–175° (losses of some angles by physical limitations and stray light). The calibration of the instrument is discussed and includes geometric calibration (to account for different light paths to the camera) plus absolute calibration (to obtain physical units). Temporal stability of calibrations is observed, and different data quality tests are presented in order to obtain reliable values of F11 and –F12/F11. For an automatic operation of the instrument that permits real time phase matrix measurements, a data quality check algorithm that avoids non-physical measurements and filters outliers has been developed. Validation of the scattering matrix elements based on monodisperse aerosol measurements is also done with polystyrene latex spheres (PSL), showing good agreement with Mie theory. Finally, first results of the instrument operating at the University of Granada (UGR) station from the Andalusian Global ObseRvatory of the Atmosphere (AGORA) since April 2022 are presented. Very good agreements of the integrated scattering coefficients with an integrating nephelometer (TSI, model 3563) were obtained with high correlation coefficients for the three wavelengths (R2 > 0.81). The calculated root-mean-square error (RMSE) reveals that the performance of the PI-Neph in the measurement of the scattering coefficient is better in the 660 nm and 515 nm wavelengths than in the 405 nm one, although differences between datasets are still low. The observed differences in phase functions and especially polarized phase functions (both in shape and spectral differences) under changing atmospheric scenarios (Saharan dust, pollution and background aerosol conditions) indicated that these variables are sensitive and reliable to classify the type of ambient aerosol. Particularly, the combined measurements of F11 and –F12/F11 shows a unique potential of the PI-Neph for aerosol typology.

Impact of Lockdown on Column and Surface Aerosol Content over Ahmedabad and a Comparison with the Indo-Gangetic Plain

Changes in vertical column concentration, size distribution, and surface concentration of aerosol associated with the lockdown imposed by the COVID-19 pandemic in 2020 over the Ahmedabad region in Gujarat State, India, were analyzed. The results are compared with changes over selected Indo-Gangetic Plain (IGP) regions. On 25 March 2020, the prime minister of India declared a complete lockdown throughout the country and later lifted restrictions in a phased manner. Aerosol optical depth (AOD) over the Ahmedabad region on 29 March dropped to as low as 0.11, and in the first two weeks of lockdown, the weekly average AOD was only 0.18. On almost all days of the lockdown period, AOD over the Ahmedabad region was lower than the decadal mean. It was found that the Ahmedabad region responded differently to lockdown conditions compared to the IGP regions. During the first lockdown phase, AOD decreased by about 29% compared to the pre-lockdown period over the Ahmedabad region. However, the average reduction over the IGP was much more, about 50%. The average Angstrom exponent (AE) of 0.96 during the pre-lockdown period over the Ahmedabad region increased phase-wise to 1.36 during the L3 lockdown phase, indicating dominance of fine-mode particles during the lockdown period. It suggests a reduction in anthropogenically produced coarse-mode particles, typically dust produced by vehicular movement, construction, and industrial activities. However, on the other hand, over the IGP region, the high dominance of fine-mode particles during the pre-lockdown period had changed to a high dominance of coarse-mode particles, especially over the Delhi region. This indicates a reduction in anthropogenically produced fine-mode particles, which are mainly generated by fossil and biofuels/biomass combustion, over the IGP region by lockdown conditions. Within a few days of lockdown, PM2.5 was reduced by 64% and 76% over the Ahmedabad and Delhi regions, respectively. The lockdown imposed by the pandemic provided an excellent opportunity to ascertain background aerosol conditions in the atmosphere.

Evaluation of the OMPS/LP stratospheric aerosol extinction product using SAGE III/ISS observations

Abstract. The Ozone Mapping and Profiler Suite Limb Profiler (OMPS/LP) has been taking limb-scattered measurements since April 2012. It is designed to produce ozone and aerosol vertical profiles at a 1.6 km vertical resolution over the entire sunlit globe. The Version 1.5 (V1.5) aerosol extinction retrieval algorithm provides aerosol extinction profiles using observed radiances at 675 nm. The algorithm assumes Mie theory and a gamma function aerosol size distribution for the stratospheric aerosol that is derived from results calculated by the Community Aerosol and Radiation Model for Atmospheres (CARMA). In this paper, we compare V1.5 LP aerosol profiles with SAGE III/ISS solar occultation observations for the period from June 2017 to May 2019, when both measurements were available to evaluate our ability to characterize background aerosol conditions. Overall, LP extinction profiles agree with SAGE III/ISS data to within ±25 % for altitudes between 19 and 27 km, even during periods perturbed by volcanic eruptions or intense forest fires. In this altitude range, the slope parameter of linear fitting of LP extinction values with respect to SAGE III/ISS measurements is close to 1.0, with Pearson correlation coefficients of r≥0.95, indicating that the LP aerosol data are reliable in that altitude range. Comparisons of extinction time series show that both instruments capture the variability of the stratospheric aerosol layer quite well, and the differences between the two instruments vary from 0 % to ±25 % depending on altitude, latitude, and time. In contrast, we find erroneous seasonal variations in the OMPS/LP Version 1.5 dataset, which usually exist below 20 km in the Southern Hemisphere due to the lack of sensitivity to particles when the scattering angle (SA) is greater than 145∘. We also find that LP-retrieved extinction is systematically higher than SAGE III/ISS observations at altitudes above 28 km and systematically lower below 19 km in the tropics with significant biases up to ±13 %. This is likely due in part to the fact that the actual aerosol size distribution is altitude dependent. There are also other reasons related to cloud contamination, wavelength limitations, aerosol loading, and the influence of the viewing configuration.

Transport of the 2017 Canadian wildfire plume to the tropics via the Asian monsoon circulation

Abstract. We show that a fire plume injected into the lower stratosphere at high northern latitudes during the Canadian wildfire event in August 2017 partly reached the tropics. The transport to the tropics was mediated by the anticyclonic flow of the Asian monsoon circulation. The fire plume reached the Asian monsoon area in late August/early September, when the Asian monsoon anticyclone (AMA) was still in place. While there is no evidence of mixing into the center of the AMA, we show that a substantial part of the fire plume is entrained into the anticyclonic flow at the AMA edge and is transported from the extratropics to the tropics, and possibly the Southern Hemisphere particularly following the north–south flow on the eastern side of the AMA. In the tropics the fire plume is lifted by ∼5 km in 7 months. Inside the AMA we find evidence of the Asian tropopause aerosol layer (ATAL) in August, doubling background aerosol conditions with a calculated top of the atmosphere shortwave radiative forcing of −0.05 W m−2. The regional climate impact of the fire signal in the wider Asian monsoon area in September exceeds the impact of the ATAL by a factor of 2–4 and compares to that of a plume coming from an advected moderate volcanic eruption. The stratospheric, trans-continental transport of this plume to the tropics and the related regional climate impact point to the importance of long-range dynamical interconnections of pollution sources.

Inventory of African desert dust events in the north-central Iberian Peninsula in 2003–2014 based on sun-photometer–AERONET and particulate-mass–EMEP data

Abstract. A reliable identification of desert dust (DD) episodes over north-central Spain is carried out based on the AErosol RObotic NETwork (AERONET) columnar aerosol sun photometer (aerosol optical depth, AOD, and Ångström exponent, α) and European Monitoring and Evaluation Programme (EMEP) surface particulate-mass concentration (PMx, x = 10, 2.5, and 2.5–10 µm) as the main core data. The impact of DD on background aerosol conditions is detectable by means of aerosol load thresholds and complementary information provided by HYSPLIT (Hybrid Single Particle Lagrangian Integrated Trajectory Model) air mass back trajectories, MODIS (Moderate Resolution Imaging Spectroradiometer) images, forecast aerosol models, and synoptic maps, which have been carefully reviewed by a human observer for each day included in the DD inventory. This identification method allows the detection of low and moderate DD intrusions and also of mixtures of mineral dust with other aerosol types by means of the analysis of α. During the period studied (2003–2014), a total of 152 DD episodes composed of 418 days are identified. Overall, this means ∼ 13 episodes and ∼ 35 days per year with DD intrusion, representing 9.5 % days year−1. During the identified DD intrusions, 19 daily exceedances over 50 µg m−3 are reported at the surface. The occurrence of DD event days during the year peaks in March and June, with a marked minimum in April and lowest occurrence in winter. A large interannual variability is observed showing a statistically significant temporal decreasing trend of ∼ 3 days year−1. The DD impact on the aerosol climatology is addressed by evaluating the DD contribution in magnitude and percent (in brackets) for AOD, PM10, PM2.5, and PM2.5 − 10, obtaining mean values of 0.015 (11.5 %), 1.3 µg m−3 (11.8 %), 0.55 µg m−3 (8.5 %) and 0.79 µg m−3 (16.1 %), respectively. Annual cycles of the DD contribution for AOD and PM10 present two maxima – one in summer (0.03 and 2.4 µg m−3 for AOD in June and PM10 in August) and another in March (0.02 for AOD and 2.2 µg m−3 for PM10) – both displaying a similar evolution with exceptions in July and September. The seasonal cycle of the DD contribution to AOD does not follow the pattern of the total AOD (close to a bell shape), whereas both PM10 cycles (total and DD contribution) are more similar to each other in shape, with an exception in September. The interannual evolution of the DD contribution to AOD and PM10 has evidenced a progressive decrease. This decline in the levels of mineral dust aerosols can explain up to 30 % of the total aerosol load decrease observed in the study area during the period 2003–2014. The relationship between columnar and surface DD contribution shows a correlation coefficient of 0.81 for the interannual averages. Finally, synoptic conditions during DD events are also analysed, observing that the north African thermal low causes most of the events ( ∼ 53 %). The results presented in this study highlight the relevance of the area studied since it can be considered representative of the clean background in the western Mediterranean Basin where DD events have a high impact on aerosol load levels.

Comparison of atmospheric particle concentration measurements using different optical detectors: Potentiality and limits for air quality applications

Optical detectors for atmospheric aerosol concentration measurements are often used in air quality applications given their potentialities for online measurements of air quality parameters at high temporal resolution. In this work the performances of different optical aerosol detectors used in air quality applications have been tested and compared for urban background aerosol conditions. Simultaneous measurements of aerosol number concentrations, size distributions and mass concentrations were taken in two different periods: November 2013 – February 2014 and May–June 2014 at an urban background site in Lecce (Southeastern Italy). Measurements were carried out using an OPC Grimm (mod. 1.109), an OPC FAI (Multichannel Monitor) and an optical photometer Mie pDR-1200. Good correlation, with determination coefficients R2 larger than 0.93 were found between particle number concentrations measured by the two OPCs both in accumulation (0.28–0.90μm for FAI and 0.29–0.90μm for Grimm) and coarse modes (1.10–10μm for FAI and 1.15–11.25μm for Grimm). Absolute counting for the accumulation fraction shows that Grimm OPC detects more particles (about 10%) than FAI OPC at concentration higher than 200,000particles/L in condition of high RH. This could be due to the changes of the optical properties of particles in high RH conditions visible even if the inlets of the two instruments are conditioned for lowering RH in sampled air. The differences in the absolute counting of the coarse fraction does not seems to be related to RH effects. The performances in evaluating mass concentrations PM10, and PM2.5 were evaluated comparing OPCs and pDR-1200 outputs with reference gravimetric and β-ray methods (that appeared to be essentially equivalent). Good agreement between Grimm OPC and SWAM is found both in PM10 and PM2.5 fractions while FAI OPC revealed greater discrepancy and scatter with respect to reference measurements. The performances of the pDR-1200 photometer were lower with respect to the OPCs with a larger influence of RH and optical properties of particles. The analysis of diurnal average trends in number and mass concentrations as well as the high temporal resolution responses of the instruments showed that optical detectors could be very useful to investigate atmospheric aerosol for air quality applications and to individuate and investigate specific pollution events. However, especially if they are used for evaluating mass concentrations (PM1, PM2.5 or PM10), it is necessary to take into account RH effects (even if the inlet are conditioned) and, possibly, use optical detectors together with reference gravimetric or β-ray methods to check their response in the effective operative conditions.

The effect of coal-fired power-plant SO<sub>2</sub> and NO<sub>x</sub> control technologies on aerosol nucleation in the source plumes

Abstract. Nucleation in coal-fired power-plant plumes can greatly contribute to particle number concentrations near source regions. The changing emissions rates of SO2 and NOx due to pollution-control technologies over recent decades may have had a significant effect on aerosol formation and growth in the plumes with ultimate implications for climate and human health. We use the System for Atmospheric Modeling (SAM) large-eddy simulation model with the TwO-Moment Aerosol Sectional (TOMAS) microphysics algorithm to model the nucleation in plumes of coal-fired plants. We test a range of cases with varying emissions to simulate the implementation of emissions-control technologies between 1997 and 2010. We start by simulating the W. A. Parish power plant (near Houston, TX) during this time period, when NOx emissions were reduced by ~90% and SO2 emissions decreased by ~30%. Increases in plume OH (due to the reduced NOx) produced enhanced SO2 oxidation and an order-of-magnitude increase in particle nucleation in the plume despite the reduction in SO2 emissions. These results suggest that NOx emissions could strongly regulate particle nucleation and growth in power-plant plumes. Next, we test a range of cases with varying emissions to simulate the implementation of SO2 and NOx emissions-control technologies. Particle formation generally increases with SO2 emission, while NOx shows two different regimes: increasing particle formation with increasing NOx under low-NOx emissions and decreasing particle formation with increasing NOx under high-NOx emissions. Next, we compare model results with airborne measurements made in the W. A. Parish power-plant plume in 2000 and 2006, confirming the importance of NOx emissions on new particle formation and highlighting the substantial effect of background aerosol loadings on this process (the more polluted background of the 2006 case caused more than an order-of-magnitude reduction in particle formation in the plume compared to the cleaner test day in 2000). Finally, we calculate particle-formation statistics of 330 coal-fired power plants in the US in 1997 and 2010, and the model results show a median decrease of 19% in particle formation rates from 1997 to 2010 (whereas the W. A. Parish case study showed an increase). Thus, the US power plants, on average, show a different result than was found for the W. A. Parish plant specifically, and it shows that the strong NOx controls (90% reduction) implemented at the W. A. Parish plant (with relatively weak SO2 emissions reductions, 30%) are not representative of most power plants in the US during the past 15 yr. These results suggest that there may be important climate implications of power-plant controls due to changes in plume chemistry and microphysics, but the magnitude and sign of the aerosol changes depend greatly on the relative reductions in NOx and SO2 emissions in each plant. More extensive plume measurements for a range of emissions of SO2 and NOx and in varying background aerosol conditions are needed, however, to better quantify these effects.

Quantifying the impact of dust on heterogeneous ice generation in midlevel supercooled stratiform clouds

Dust aerosols have been regarded as effective ice nuclei (IN), but large uncertainties regarding their efficiencies remain. Here, four years of collocated CALIPSO and CloudSat measurements are used to quantify the impact of dust on heterogeneous ice generation in midlevel supercooled stratiform clouds (MSSCs) over the ‘dust belt’. The results show that the dusty MSSCs have an up to 20% higher mixed‐phase cloud occurrence, up to 8 dBZ higher mean maximum Ze (Ze_max), and up to 11.5 g/m2 higher ice water path (IWP) than similar MSSCs under background aerosol conditions. Assuming similar ice growth and fallout history in similar MSSCs, the significant differences in Ze_max between dusty and non‐dusty MSSCs reflect ice particle number concentration differences. Therefore, observed Ze_max differences indicate that dust could enhance ice particle concentration in MSSCs by a factor of 2 to 6 at temperatures colder than −12°C. The enhancements are strongly dependent on the cloud top temperature, large dust particle concentration and chemical compositions. These results imply an important role of dust particles in modifying mixed‐phase cloud properties globally.

Nucleation and growth of sulfate aerosol in coal-fired power plant plumes: sensitivity to background aerosol and meteorology

Abstract. New-particle formation in the plumes of coal-fired power plants and other anthropogenic sulfur sources may be an important source of particles in the atmosphere. It remains unclear, however, how best to reproduce this formation in global and regional aerosol models with grid-box lengths that are 10s of kilometers and larger. The predictive power of these models is thus limited by the resultant uncertainties in aerosol size distributions. In this paper, we focus on sub-grid sulfate aerosol processes within coal-fired power plant plumes: the sub-grid oxidation of SO2 with condensation of H2SO4 onto newly-formed and pre-existing particles. We have developed a modeling framework with aerosol microphysics in the System for Atmospheric Modelling (SAM), a Large-Eddy Simulation/Cloud-Resolving Model (LES/CRM). The model is evaluated against aircraft observations of new-particle formation in two different power-plant plumes and reproduces the major features of the observations. We show how the downwind plume aerosols can be greatly modified by both meteorological and background aerosol conditions. In general, new-particle formation and growth is greatly reduced during polluted conditions due to the large pre-existing aerosol surface area for H2SO4 condensation and particle coagulation. The new-particle formation and growth rates are also a strong function of the amount of sunlight and NOx since both control OH concentrations. The results of this study highlight the importance for improved sub-grid particle formation schemes in regional and global aerosol models.

Manipulating marine stratocumulus cloud amount and albedo: a process-modelling study of aerosol-cloud-precipitation interactions in response to injection of cloud condensation nuclei

Abstract. We use a cloud-system-resolving model to study marine-cloud brightening. We examine how injected aerosol particles that act as cloud condensation nuclei (CCN) are transported within the marine boundary layer and how the additional particles in clouds impact cloud microphysical processes, and feedback on dynamics. Results show that the effectiveness of cloud brightening depends strongly on meteorological and background aerosol conditions. Cloud albedo enhancement is very effective in a weakly precipitating boundary layer and in CCN-limited conditions preceded by heavy and/or persistent precipitation. The additional CCN help sustain cloud water by weakening the precipitation substantially in the former case and preventing the boundary layer from collapse in the latter. For a given amount of injected CCN, the injection method (i.e., number and distribution of sprayers) is critical to the spatial distribution of these CCN. Both the areal coverage and the number concentration of injected particles are key players but neither one always emerges as more important than the other. The same amount of injected material is much less effective in either strongly precipitating clouds or polluted clouds, and it is ineffective in a relatively dry boundary layer that supports clouds of low liquid water path. In the polluted case and "dry" case, the CCN injection increases drop number concentration but lowers supersaturation and liquid water path. As a result, the cloud experiences very weak albedo enhancement, regardless of the injection method.

Estimation of the contributions of long range transported aerosol in East Asia to carbonaceous aerosol and PM concentrations in Seoul, Korea using highly time resolved measurements: a PSCF model approach

The contributions of long range transported aerosol in East Asia to carbonaceous aerosol and particulate matter (PM) concentrations in Seoul, Korea were estimated with potential source contribution function (PSCF) calculations. Carbonaceous aerosol (organic carbon (OC) and elemental carbon (EC)), PM(2.5), and PM(10) concentrations were measured from April 2007 to March 2008 in Seoul, Korea. The PSCF and concentration weighted trajectory (CWT) receptor models were used to identify the spatial source distributions of OC, EC, PM(2.5), and coarse particles. Heavily industrialized areas in Northeast China such as Harbin and Changchun and East China including the Pearl River Delta region, the Yangtze River Delta region, and the Beijing-Tianjin region were identified as high OC, EC and PM(2.5) source areas. The conditional PSCF analysis was introduced so as to distinguish the influence of aerosol transported from heavily polluted source areas on a receptor site from that transported from relatively clean areas. The source contributions estimated using the conditional PSCF analysis account for not only the aerosol concentrations of long range transported aerosols but also the number of transport days effective on the measurement site. Based on the proposed algorithm, the condition of airmass pathways was classified into two types: one condition where airmass passed over the source region (PS) and another condition where airmass did not pass over the source region (NPS). For most of the seasons during the measurement period, 249.5-366.2% higher OC, EC, PM(2.5), and coarse particle concentrations were observed at the measurement site under PS conditions than under NPS conditions. Seasonal variations in the concentrations of OC, EC, PM(2.5), and coarse particles under PS, NPS, and background aerosol conditions were quantified. The contributions of long range transported aerosols on the OC, EC, PM(2.5), and coarse particle concentrations during several Asian dust events were also estimated. We also investigated the performance of the PSCF results obtained from combining highly time resolved measurement data and backward trajectory calculations via comparison with those from data in low resolutions. Reduced tailing effects and the larger coverage over the area of interest were observed in the PSCF results obtained from using the highly time resolved data and trajectories.

Particle backscatter, extinction, and lidar ratio profiling with Raman lidar in south and north China

Aerosol Raman lidar observations of profiles of the particle extinction and backscatter coefficients and the respective extinction-to-backscatter ratio (lidar ratio) were performed under highly polluted conditions in the Pearl River Delta (PRD) in southern China in October 2004 and at Beijing during a clear period with moderately polluted to background aerosol conditions in January 2005. The anthropogenic haze in the PRD is characterized by volume light-extinction coefficients of particles ranging from approximately 200 to 800 Mm(-1) and lidar ratios mostly between 40 and 55 sr (average of 47+/-6 sr). Almost clean air masses were observed throughout the measurements of the Beijing campaign. These air masses originated from arid desert-steppe-like regions (greater Gobi area). Extinction values usually varied between 100 and 300 Mm(-1), and the lidar ratios were considerably lower (compared with PRD values) with values mostly from 30 to 45 sr (average of 38+/-7 sr). Gobi dust partly influenced the observations. Unexpectedly low lidar ratios of approximately 25 sr were found for a case of background aerosol with a low optical depth of 0.05. The low lidar ratios are consistent with Mie-scattering calculations applied to ground-based observations of particle size distributions.

Atmospheric effects of volcanic eruptions as seen by famous artists and depicted in their paintings

Abstract. Paintings created by famous artists, representing sunsets throughout the period 1500–1900, provide proxy information on the aerosol optical depth following major volcanic eruptions. This is supported by a statistically significant correlation coefficient (0.8) between the measured red-to-green ratios of a few hundred paintings and the dust veil index. A radiative transfer model was used to compile an independent time series of aerosol optical depth at 550 nm corresponding to Northern Hemisphere middle latitudes during the period 1500–1900. The estimated aerosol optical depths range from 0.05 for background aerosol conditions, to about 0.6 following the Tambora and Krakatau eruptions and cover a period practically outside of the instrumentation era.

Description and sensitivity analysis of a limb scattering ozone retrieval algorithm

We present the theoretical basis for an algorithm that retrieves vertical profiles of ozone concentration using measurements of light scattered from the limb of the atmosphere. Simulated radiances at wavelengths between 300 and 675 nm are inverted using the optimal estimation technique, producing a retrieved ozone number density profile between 10 and 55 km. A detailed sensitivity analysis of this ozone retrieval algorithm follows. The largest source of ozone retrieval error is tangent height misregistration (i.e., instrument pointing error), which is relevant throughout the altitude range of interest and produces retrieval errors on the order of 10–20% due to a tangent height registration error of 0.5 km. The retrieved profile is shifted in altitude relative to the true profile, with very little distortion of the profile shape. Sensitivity to stratospheric aerosol is also a significant source of error, with errors of 5–8% for altitudes less than 40 km under background aerosol conditions when an aerosol‐free atmosphere is assumed by the algorithm. Using an incorrect a priori ozone estimate can produce errors up to 15% at altitudes near 10 km, but the a priori profile has little influence above that level. Addressing these error sources (e.g., with better instrument pointing knowledge, introduction of reliable aerosol information, and better instrument signal‐to‐noise to reduce the importance of the a priori ozone estimate, respectively) is the key to significantly improving the retrieval accuracy. Further improvement would then be limited by several secondary error sources that produce retrieval errors at the 5% level.

Stratospheric temperature monitoring using a vibrational Raman lidar : Part 1: aerosols and ozone interferences

Lidar measurements of temperature for the upper troposphere and lower stratosphere are commonly derived by the Raman technique. Lidar signals derived from vibrational Raman processes have been subjected to numerous simulation tests to examine their sensitivity to the presence of aerosols and ozone in the atmosphere. The influence of aerosols characteristics (wavelength dependence of aerosol extinction and particle phase function) and of ozone concentration on Raman temperature profiles is estimated. Simulations indicate large temperature deviations for post-volcanic conditions. For a Raman backscatter at 607 nm, bias is below 1 K for a total optical depth less than 9 x 10(-3) in the case of a stratospheric contamination and less than 6 x 10(-3) for a tropospheric contamination. The effect of aerosols depends on phase function and a few parameters such as altitude, optical depth and the shape of the high-altitude cloud. The wavelength dependence of aerosol extinction has some influence only for severe post-volcanic conditions (Scattering Ratio, SR >2). For a Raman backscatter at 387 nm, bias is larger and can be significant even in background aerosol conditions. Changes in the ozone density profile lead to significant Raman temperature deviations only for some specific conditions. Results suggest that both aerosol and ozone corrections are necessary to obtain an accuracy better than the 1 K requested for most atmospheric applications.

Stratospheric aerosol measurements by dual polarisation lidar

Abstract. We present measurements of stratospheric aerosol made at Aberystwyth, UK (52.4° N, 4.06° W) during periods of background aerosol conditions. The measurements were made with a lidar system based on a 532nm laser and two polarisation channels in the receiver. When stratospheric aerosol amounts are very small, as at present, this method is, potentially, free of a number of systematic errors that bedevil more commonly-used methods. The method rests on the assumption that the aerosol consists of spherical droplets which do not depolarise the lidar signal, which is valid under most conditions. Maximum lidar ratios in background aerosol of 1.03-1.06 were measured during the period 2001-2004, with integrated backscatter in the range 2-7x10-5sr-1. In January 2003, depolarising aerosol was measured, which invalidated the dual-polarisation measurements. On 10-11 January, the depolarising aerosol was clearly a polar stratospheric cloud (the first lidar observations of such clouds in the British Isles) but the aerosol observed on 7-8 January was too low in altitude and too warm to be a PSC.

Thirty years of in situ stratospheric aerosol size distribution measurements from Laramie, Wyoming (41°N), using balloon‐borne instruments

Vertical profiles of size‐resolved aerosol concentrations above Laramie, Wyoming (41°N), have been measured for the past thirty years, 1971‐2001. During this period, two somewhat different optical particle counters have been used to measure particles with radii ≥0.15 μm, whereas the instrument to measure condensation nuclei (CN) has not changed significantly since the late 1970s. The two optical particle counters measure aerosols ≥0.15, 0.25 μm and aerosols ≥0.15–2.0 μm in twelve size classes. These measurements have concentration (N) uncertainties ∝ ±N−0.5, but with a minimum of ±10%. Sizing uncertainties are about ±10%. The impact of these uncertainties on size distribution fitting parameters and aerosol moments are approximately ±30% and ±40%. The long‐term record from these measurements indicates that volcanoes have controlled stratospheric aerosol abundance for 20 of the past 30 years. The present period, beginning in 1997, represents the longest volcanically quiescent period in the record. These and other measurements clearly show that stratospheric aerosol are now in a background state, a state rarely occurring in recent times, and that this background state is not significantly different than observations in 1979. Aerosol volumes and surface areas, inferred from size distributions fit to the measurements, are compared with SAGE II satellite estimates of surface area and volume. For volume the measurements are in agreement within measurement error throughout the record. For surface area there is good agreement for a volcanic aerosol laden stratosphere, but for background aerosol conditions the SAGE II estimates are about 40% less than the in situ measurements. Present aerosol surface areas are ∼1.0 (0.6) μm2 cm−3 in the 15–20 (20–25) km layer based on in situ measurements. The Laramie size distribution record is now available to the community over the internet.

Systematic DIAL lidar monitoring of the stratospheric ozone vertical distribution at Observatoire de Haute-Provence (43.92 degrees N, 5.71 degrees E).

Long term stratospheric DIAL (Differential Absorption Lidar) ozone lidar (Light Detection and Ranging) measurements have been performed at the Observatoire de Haute-Provence (OHP) since 1985 and as part of the Network for the Detection of Stratospheric Changes (NDSC) since 1991. This paper provides a detailed description of the DIAL lidar instrument implemented at OHP and a discussion of the ozone retrieval analysis. The instrument includes the detection of atmospheric nitrogen Raman scattering wavelengths, which is required for ozone measurements in the presence of strong volcanic aerosol loading. A comprehensive evaluation of the error budget in the 10-50 km altitude range is performed with particular emphasis on the bias associated with background and volcanic stratospheric aerosol. This bias is evaluated using ancillary measurements of the aerosol size distribution obtained from 1991 to 1999 after the Mount Pinatubo volcanic eruption. Results show that the bias associated with background aerosols is smaller than 1% above 13 km while the bias due to volcanic aerosols reaches a maximum of 5% above 15 km in the DIAL Raman ozone retrieval. In background aerosol conditions the total accuracy of the DIAL ozone vertical distribution at OHP ranges from 5% below 20 km to 15-30% above 45 km with a vertical resolution varying from 0.5 km to 5 km.

Observed reductions of total solar irradiance by biomass‐burning aerosols in the Brazilian Amazon and Zambian Savanna

Several aerosol and solar flux monitoring sites were established in Brazil for the Large Scale Biosphere‐Atmosphere Experiment in Amazônia project. CIMEL sunphotometers and collocated pyranometers were employed at two southern Amazonian sites in order to quantify instantaneous reductions of total irradiance due to high aerosol optical thickness (AOT) smoke events (relative to values modeled for background aerosol conditions). Results from the Brazilian sites are presented for 1999 and for comparison, a similar analysis is discussed for data from three south‐central African sites during the burning season of 2000. The relative reductions in total irradiance at the surface resulting from biomass burning aerosol are observed to be substantial at all sites, ranging from 16% for an aerosol optical thickness (500 nm) of 1.0 for the Brazilian sites to an average rate of 22% for the African sites. For a solar zenith interval (25–35°), these rates equate to reductions of roughly 145 W/m2 and 210 W/m2 respectively, for an AOT = 1.0. Instantaneous reductions of 337 W/m2 were observed for the heaviest smoke conditions (AOT: ∼3.0) in Brazil.

Buffering interactions in the modeled response of stratospheric O3 to increased NOx and HOx

The response of stratospheric O3 to changes in NOx and HOx is tested in a two‐dimensional model with the goal of exploring photochemical buffering mechanisms. The model tests are performed under background aerosol conditions at both current (1996) and preindustrial levels of stratospheric halogens. The tests are prompted in part by comparisons to observations from the POLARIS (Polar Ozone Loss in the Arctic Region in Summer) high‐altitude aircraft campaign, which show that models significantly underestimate the NOx/NOy ratio in the lower stratosphere but are more successful at reproducing observed O3. Model tests with increased NOx show that increases in NOx‐catalyzed O3 loss are subject to photochemical buffering in the lower stratosphere through reduced HOx‐catalyzed O3 loss and, at current halogen levels, reduced halogen‐catalyzed O3 loss. In contrast, these tests show that O3 is not well buffered with respect to increased NOx in the middle stratosphere, especially at preindustrial halogen levels. Consequently, an NOy increase that reaches the middle stratosphere could lead to modest depletion of column O3, while an NOy increase confined to the lower stratosphere more likely would have a neutral or slightly positive effect on column O3. These results are only mildly sensitive to uncertainties in the NOx/NOy ratio. Additional model tests with increased HOx show some photochemical buffering, but generally lead to mixed effects on O3 which depend on the nature of the HOx source gas. This source gas dependence is especially strong at current halogen levels.