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NASA NTRS1988

Formic and acetic acid over the central Amazon region, Brazil. I - Dry season

The concentrations of formic and acetic acids in the gas phase, atmospheric aerosol, and rainwater samples collected in Amazonia at ground level and in the atmosphere during the Amazon Boundary Layer Experiment in July/August 1985 were analyzed by ion exchange chromatography. The diurnal behavior of both acids at ground level and their vertical distribution in the forest canopy point to the existence of vegetative sources as well as to production by chemical reactions in the atmosphere. The concentrations of formic and acetic acids in the gas phase were about 2 orders of magnitude higher than the corresponding concentrations in the atmospheric aerosol. In rainwater, the total formate and acetate represented about one half of the anion equivalents, in contrast to less than 10 percent of the soluble anionic equivalents contributed by these acids in the atmospheric aerosol. The observed levels of these ions in rainwater are considered to be the result of a combination of chemical reactions in hydrometeors and the scavenging of the gaseous acids by cloud droplets.

Andreae, M. O.↗

NASA NTRS2003

Aerosol-Cloud Interactions during Tropical Deep Convection: Evidence for the Importance of Free Tropospheric Aerosols

NASA's 2002 CRYSTAL-FACE field experiment focused on the formation and evolution of tropical cirrus cloud systems in southern Florida. Multiple aircraft extensively sampled cumulonimbus dynamical and microphysical properties, as well as characterizing ambient aerosol populations both inside and outside the full depth of the convective column. On July 18, unique measurements were taken when a powerful updraft was traversed directly by aircraft, providing a window into the primary source region of cumulonimbus anvil crystals. Observations of the updraft, entered at approximately l0 km altitude and -34 C, indicated more than 200 cloud particles per mL at vertical velocities exceeding 20 m/s and the presence of significant condensation nuclei and liquid water within the core. In this work, aerosol and cloud phase observations are integrated by simulating the updraft conditions using a large-eddy resolving model with 3 explicit multiphase microphysics, including treatment of size-resolved aerosol fields, aerosol activation and freezing, and evaporation of cloud particles back to the aerosol phase. Simulations were initialized with observed thermodynamic and aerosol size distributions profiles and convection was driven by surface fluxes assimilated from the ARPS forecast model. Model results are consistent with the conclusions that most crystals are homogeneously frozen droplets and that entrained free tropospheric aerosols may contribute a significant fraction of the crystals. Thus most anvil crystals appear to be formed aloft in updraft cores, well above cloud base. These conclusions are supported by observations of hydrometeor size distribution made while traversing the dore, as well as aerosol and cloud particle size distributions generally observed by aircraft below 4km and crystal properties generally observed by aircraft above 12km.

Ackerman, A.↗

NASA NTRS2022

Impact of Meteorological Factors on the Mesoscale Morphology of Cloud Streets during a Cold-Air Outbreak over the Western North Atlantic

Postfrontal clouds (PFC) are ubiquitous in the marine boundary layer, and their morphology is essential to estimating the radiation budget in weather and climate models. Here we examine the roles of sea surface temperature (SST) and meteorological factors in controlling the mesoscale morphology and evolution of shallow clouds associated with a cold-air outbreak that occurred on 1 March 2020 during phase I of the Aerosol Cloud Meteorology Interactions over the Western Atlantic Experiment (ACTIVATE). Our results show that the simulated PFC structure and ambient conditions by the Weather Research and Forecasting (WRF) Model are generally consistent with observations from GOES-16 and dropsonde measurements. We also examine the thermodynamical and dynamical influences in the cloud mesoscale morphology using WRF sensitivity experiments driven by two meteorological forcing datasets with different domain-mean SST and spatial gradients, which lead to dissimilar values of hydrometeor water path and cloud core fraction. The SST from ERA5 leads to weaker stability and higher inversion height than the SST from FNL does. In addition, the use of large-scale meteorological forcings from ERA5 yields a distinctive time evolution of wind direction shear in the inner domain, which favors the formation and persistence of longer cloud rolls. Both factors contribute to a change in the time evolution of domain-mean water path and cloud core fraction of cloud streets. Our study takes advantage of the simulation driven by the differences between two large-scale forcing datasets to illustrate the importance of SST and wind direction shear in the cloud street morphology in a realistic scenario

Jingyi Chen↗

NASA NTRS2010

DSD Characteristics of a Mid-Winter Tornadic Storm Using C-Band Polarimetric Radar and Two 2D-Video Disdrometers

Drop size distributions in an evolving tornadic storm are examined using C-band polarimetric radar observations and two 2D-video disdrometers. The E-F2 storm occurred in mid-winter (21 January 2010) in northern Alabama, USA, and caused widespread damage. The evolution of the storm occurred within the C-band radar coverage and moreover, several minutes prior to touch down, the storm passed over a site where several disdrometers including two 2D video disdrometers (2DVD) had been installed. One of the 2DVDs is a low profile unit and the other is a new next generation compact unit currently undergoing performance evaluation. Analyses of the radar data indicate that the main region of precipitation should be treated as a "big-drop" regime case. Even the measured differential reflectivity values (i.e. without attenuation correction) were as high as 6-7 dB within regions of high reflectivity. Standard attenuation-correction methods using differential propagation phase have been "fine tuned" to be applicable to the "big drop" regime. The corrected reflectivity and differential reflectivity data are combined with the co-polar correlation coefficient and specific differential phase to determine the mass-weighted mean diameter, Dm, and the width of the mass spectrum, (sigma)M, as well as the intercept parameter , Nw. Significant areas of high Dm (3-4 mm) were retrieved within the main precipitation areas of the tornadic storm. The "big drop" regime assumption is substantiated by the two sets of 2DVD measurements. The Dm values calculated from 1-minute drop size distributions reached nearly 4 mm, whilst the maximum drop diameters were over 6 mm. The fall velocity measurements from the 2DVD indicate almost all hydrometeors to be fully melted at ground level. Drop shapes for this event are also being investigated from the 2DVD camera data.

Thurai, M.↗

NASA NTRS2021

The Prevalence of Precipitation From Polar Supercooled Clouds

Supercooled clouds substantially impact polar surface energy budgets, but large-scale models often underestimate their occurrence, which motivates accurately establishing metrics of basic processes. An analysis of long-term measurements at Utqiaġvik, Alaska, and McMurdo Station, Antarctica, combines lidar-validated use of soundings to identify supercooled cloud layers and colocated ground-based profiling radar measurements to quantify cloud base precipitation. We find that more than 85 % (75 %) of sampled supercooled layers are precipitating over the Arctic (Antarctic) site, with more than 75 % (50 %) precipitating continuously to the surface. Such high frequencies can be reconciled with substantially lesser spaceborne estimates by considering differences in radar hydrometeor detection sensitivity. While ice precipitation into supercooled clouds from aloft is common, we also find that the great majority of supercooled cloud layers without ice falling into them are themselves continuously generating precipitation. Such sustained primary ice formation is consistent with continuous activation of immersion-mode ice-nucleating particles (INPs), suggesting that supercooled cloud formation is a principal gateway to ice formation at temperatures greater than ∼−38 ∘C over polar regions. The prevalence of weak precipitation fluxes is also consistent with supercooled cloud longevity and with well-observed and widely simulated case studies. An analysis of colocated microwave radiometer retrievals suggests that weak precipitation fluxes can be nonetheless consequential to moisture budgets for supercooled clouds owing to small liquid water paths. The results here also demonstrate that the observed abundance of mixed-phase clouds can vary substantially with instrument sensitivity and methodology. Finally, we suggest that these ground-based precipitation rate statistics offer valuable guidance for improving the representation of polar cloud processes in large-scale models.

Supercooled clouds↗

NASA NTRS2011

Drop Size Distribution Measurements Supporting the NASA Global Precipitation Measurement Mission: Infrastructure and Preliminary Results

Global Precipitation Measurement Mission (GPM) retrieval algorithm validation requires datasets that characterize the 4-D structure, variability, and correlation properties of hydrometeor particle size distributions (PSD) and accumulations over satellite fields of view (5 -- 50 km). Key to this process is the combined use of disdrometer and polarimetric radar platforms. Here the disdrometer measurements serve as a reference for up-scaling dual-polarimetric radar observations of the PSD to the much larger volumetric sampling domain of the radar. The PSD observations thus derived provide a much larger data set for assessing DSD variability, and satellite-based precipitation retrieval algorithm assumptions, in all three spatial dimensions for a range of storm types and seasons. As one component of this effort, the GPM Ground Validation program recently acquired five 3rd generation 2D Video disdrometers as part of its Disdrometer and Radar Observations of Precipitation Facility (DROP), currently hosted in northern Alabama by the NASA Marshall Space Flight Center and the University of Alabama in Huntsville. These next-generation 2DVDs were operated and evaluated in different phases of data collection under the scanning domain of the UAH ARMOR C-band dual-polarimetric radar. During this period approximately 7500 minutes of PSD data were collected and processed to create gamma size distribution parameters using a truncated method of moments approach. After creating the gamma parameter datasets the DSDs were then used as input to T-matrix code for computation of polarimetric radar moments at C-band. The combined dataset was then analyzed with two basic objectives in mind: 1) the investigation of seasonal variability in the rain PSD parameters as observed by the 2DVDs; 2) the use of combined polarimetric moments and observed gamma distribution parameters in a functional form to retrieve PSD parameters in 4-D using the ARMOR radar for precipitation occurring in different seasons and for different rain system types. Preliminary results suggest that seasonal variations in the DSD parameters do occur, but are most pronounced when comparing tropical PSDs to either winter or summer convective precipitation. For example the previously documented shift to relatively smaller drop diameters in higher number concentrations for equivalent rain rate bins was observed in tropical storm rainbands occurring over Huntsville. On a more inter seasonal basis empirical fits between parameters such as D0 and ZDR do not appear to exhibit robust seasonal biases- i.e., one fit seems to work for all seasons within acceptable standard error (O[10%]) for estimates of D0. In polarimetric retrievals of the vertical variability in PSD (rain layer) for a tropical rainband we find that the Do varies with height when partitioned by specified precipitation categories (e.g., convective or stratiform, heavy and light stratiform etc.) but this variation is of order 10-20% and is smaller than the difference in D0 observed between the basic delineation of convective and stratiform precipitation types. Currently we are expanding our analysis of the vertical structure of the PSD to include several seasonally and/or dynamically-different storm system types (e.g., winter convection and stratiform events; summer mid-latitude convective etc.) sampled by ARMOR. The study will present the results of our combined analyses.

Petersen, Walter A.↗

NASA NTRSDate not supplied

Observing Ice Phase Clouds and Precipitation with Millimeter- and Submillimeter-wave Radiometry during the IMPACTS field campaign: Algorithm Development for the Emerging Class of Microwave Radiometers

Millimeter- and submillimeter-wave (mmWave, submm) radiometers provide significant information content on atmospheric water in liquid, ice, and vapor phases. Recent sensors, such as the Global Precipitation Measurement (GPM) or the Temporal Experiment for Storms and Tropical Systems Technology – Demonstration (TEMPEST-D), use mmWave bands to improve estimation of ice-phase precipitation, and future missions, such as the Atmosphere Observing System (AOS), will extend to submm to provide additional information on thinner ice clouds, linking clouds and precipitation and therefore elucidating the links between weather, climate, and the water cycle. To support the expanded use of mmWave/submm radiometry and exploit the available information content on condensed water mass, we demonstrate ice and liquid water path retrievals for NASA Goddard Space Flight Center's airborne radiometers the Conical Scanning Millimeter-wave Imaging Radiometer (CoSMIR) and the Configurable Scanning Submillimeter-wave Instrument/Radiometer (CoSSIR, formerly the Compact Scanning Submillimeter Imaging Radiometer). The analysis is based on data collected during the Investigation of Microphysics and Precipitation for Atlantic Coast-Threatening Storms (IMPACTS) field campaign. A simulation study compares and contrasts retrievals for CoSMIR and CoSSIR, with CoSSIR demonstrating higher skill in ice retrievals, particularly for thin clouds, and the CoSMIR frequencies performing better for liquid. Additionally, we look at dual-polarized radiances observed by CoSMIR during the first two IMPACTS deployments to understand the polarization signatures induced by oriented hydrometeors. Results will be presented in the context of upcoming missions and sensors including AOS and the Ice Cloud Imager (ICI). We will describe the objectives for the expected first flight of the newly upgraded CoSSIR during the final IMPACTS deployment, and we will share novel science investigations we plan to undertake with CoSSIR's new capabilities. Popular Summary: Ice in clouds and falling snow is an important component of weather, climate, and water resources. To better use a new class of sensors that provide information on atmospheric ice, we developed an approach to measure ice clouds and falling snow using airborne data taken during the Investigation of Microphysics and Precipitation for Atlantic Coast-Threatening Storms (IMPACTS), a field campaign to study winter storms. We look at the results for two similar instruments to understand how those differences affect these measurements of clouds and snow, and we further investigate the information the sensors can provide on properties of the clouds and snow.

Ian S Adams↗

NASA NTRSDate not supplied

Observing Ice Phase Clouds and Precipitation with Millimeter- and Submillimeter-wave Radiometry during the IMPACTS field campaign: Algorithm Development for the Emerging Class of Microwave Radiometers

Ian S Adams↗

NASA NTRS1998

Characterization of Mesoscale Convective Systems by Means of Composite Radar Reflectivity Data

A mesoscale convective system (MCS) is broadly defined as a cloud and precipitation system of mesoscale dimensions (often too large for most aircraft to circumnavigate) with deep-convective activity concentrated in at least part of the MCS, or present during part of its evolution. A large areal fraction of MCSs is stratiform in nature, yet estimates from MCSs over the Great Plains, the Southeast, and tropical waters indicate that at least half of the precipitation is of convective origin. The presence of localized convection is important, because within convective towers cloud particles and hydrometeors are carried upward towards the cloud top. Ice crystals then move over more stratiform regions, either laterally, or through in situ settling over decaying and spreading convection. These ice crystals then grow to precipitation-size particles in mid- to upper tropospheric mesoscale updrafts. The convective portion of a MCS is often a more or less continuous line of thunderstorms, and may be either short-lived or long-lived. Geerts (1997) presents a preliminary climatology of MCSs in the southeastern USA, using just one year of composite digital radar reflectivity data. In this study MCSs are identified and characterized by means of visual inspection of animated images. A total of 398 MCSs were identified. In the warm season MCSs were found to be about twice as frequent as in the cold season. The average lifetime and maximum length of MCSs are 9 hours, and 350 km, respectively, but some MCSs are much larger and more persistent. In the summer months small and short-lived MCSs are relatively more common, whereas in winter larger and longer-lived systems occur more frequently. MCSs occur more commonly in the afternoon, in phase with thunderstorm activity, but the amplitude of the diurnal cycle is small compared to that of observed thunderstorms. It is estimated that in the Southeast more than half of all precipitation and severe weather results from MCSs.

Geerts, Bart↗

NASA NTRSDate not supplied

An Ensemble Investigation of the Causes for Regional Air-Quality Model Critical Load Exceedances Prediction Variability in European and North American Domains Using Diagnostics From Phase 4 of the Air Quality Model Evaluation International Initiative

We summarize tentative findings from multi air quality model ensembles for the years 2009 and 2010 in Europe (EU), and 2010 and 2016 in North America (NA), under AQMEII-4. The model predictions of sulphur and nitrogen deposition were used to estimate exceedances of critical loads for acidification and eutrophication, to show the extent to which the ensemble members agree in the magnitude and the trend of ecologically meaningful impacts. Model exceedance variability was analyzed using AQMEII-4 diagnostics. Evaluation against concentration and wet deposition observations, coupled with these diagnostics, identified specific process representations as the causes for variability between model predictions and for reduced model performance. All models predicted reductions in ecosystem acidification impacts in North America between the years 2010 and 2016, in accord with SO2 emissions reduction legislation which started in 2010 (SO2 SIP) However, all models in EU and NA domains had net negative biases for wet deposition of sulphur and nitrogen relative to observations. The wet S deposition average mean bias for the NA ensemble was -0.17 eq ha-1 d-1, and for the EU ensemble -1.15 eq ha-1 d-1. The NA daily wet deposition average mean bias for NH4+ was -0.37 eq ha-1d-1; EU -1.19 eq ha-1 d-1. The daily NA wet NO3- deposition average mean bias was -0.24 eq ha-1d-1; EU -0.69 eq ha-1 d-1. The members of the ensemble diverged (factor of 10) in their North American predictions for Ndep and consequently their eutrophication exceedances. The models with the highest eutrophication predictions also predicted the highest levels of gas-phase ammonia dry deposition (standard deviation of ammonia dry deposition flux across ensemble members was larger than the ensemble average). These models also had negative biases of predicted ammonia concentrations; average mean biases of -0.63 (satellite NH3) and -0.85 ppbv (surface NH3) compared to ensemble averages of -0.30 and -0.34 ppbv. Diagnostics showed that these differences resulted from the manner in which bidirectional ammonia fluxes were parameterized within these models. The second largest source of NA eutrophication prediction variability were models with positive biases in particulate ammonium and nitrate concentrations, and higher particle nitrogen deposition levels ( particle ammonium concentration bias +0.35 ug m-3; ensemble bias +0.15 ug m-3). We believe two factors may have led to these latter overestimates: higher levels of fine mode particle nitrate formation compared to other models (due to the use of an inorganic heterogeneous chemistry algorithm which did not take base cation chemistry into account), and updates to particle dry deposition velocities carried out in the absence of concurrent updates to wet scavenging algorithms. The relative importance of dry gas, dry particulate, and wet deposition towards total sulphur and nitrogen deposition totals differed between EU and North American domains, though all models had negative biases in wet deposition as noted above. Parallel and subsequent work suggests that multiphase hydrometeor scavenging may improve model wet deposition performance. An increased research focus is recommended for four model processes: multiphase hydrometeor scavenging, ammonia bidirectional fluxes, base cation chemistry and emissions, and particle dry deposition.

regional air-quality model↗

NASA NTRS2022

Mind-the-Gap - Part 3: Doppler Velocity Measurements From Space

Convective motions and hydrometeors microphysical properties are highly sought-after parameters for evaluating atmospheric numerical models. With most of the Earth’s surface covered by water, space-borne Doppler radars are ideal for acquiring such measurements at a global scale. While these systems have proven to be useful tools for retrieving cloud microphysical and dynamical properties from the ground, their adequacy, and specific requirements for spaceborne operation still need to be evaluated. Comprehensive forward simulations enable us to assess the advantages and drawbacks of six different Doppler radar architectures currently planned or under consideration by space agencies for the study of cloud dynamics. Radar performance is examined against state-of-the-art numerical model simulations of well-characterized shallow and deep, continental, and oceanic convective cases. Mean Doppler velocity (MDV) measurements collected at multiple frequencies (13, 35 and 94 GHz) provide complementary information in deep convective cloud systems. The high penetration capability of the 13-GHz radar enables to obtain a complete, albeit horizontally under-sampled, view of deep convective storms. The smaller instantaneous field of view (IFOV) of the 35-GHz radar captures more precise information about the location and size of convective updrafts above 5-8 km height of most systems which was determined is the portion of storms where the mass flux peak is typically located. Finally, the lower mean Doppler velocity uncertainty of displaced phase center antenna (DPCA) radars makes them an ideal system for studying microphysics in shallow convection and frontal systems, as well as ice and mixed-phase clouds. It is demonstrated that a 94-GHz DCPA system can achieve retrieval errors as low as 0.05-0.15 mm for raindrop volume-weighted mean diameter and 25% for rime fraction (for a -10 dBZ echo).

Pavlos Kollias↗

NASA NTRSDate not supplied

Exploring Environmental and Aerosol Impacts on Maritime Tropical Convection using Airborne Radiometer, Radar, Lidar, and Dropsondes

The field deployment phase of NASA’s Cloud, Aerosol and Monsoon Processes Philippines Experiment (CAMP2Ex) took place around the Philippines during August–October 2019, with the primary goal of jointly investigating aerosols and tropical meteorology at the micro-β to meso-β scales. A suite of instruments was deployed on NASA’s P-3B Orion aircraft to accomplish this mission, including: the Advanced Microwave Precipitation Radiometer (AMPR), Airborne Precipitation and cloud Radar 3rd Generation (APR-3), High Spectral Resolution Lidar 2 (HSRL2), and Advanced Vertical Atmospheric Profiling System (AVAPS) dropsondes. To examine potential aerosol influences on maritime tropical convection, P-3 flight segments throughout CAMP2Ex were binned into similar environmental groups using “low,” “medium,” and “high” values of nine AVAPS-derived parameters with known physical connections to convective frequency and/or intensity. Aerosol concentrations in each flight segment were evaluated using three HSRL2 variables at 355 and 532 nm: aerosol backscatter, aerosol extinction, and aerosol optical thickness. A set of radiometer- and radar-derived variables directly related to convective frequency and/or intensity was used to characterize convection, which included: AMPR-derived integrated cloud liquid water; polarization-corrected temperatures at 10.7, 19.35, 37.1, and 85.5 GHz; peak equivalent radar reflectivity factor (ZH); peak height of 30-dBZ ZH; and the number of radar data columns with composite ZH > 30 dBZ. The ZH analyses were performed using both Ku- and Ka-band APR-3 data. For each flight segment, correlation coefficients were calculated between each convective parameter and aerosol concentrations within the “low,” “medium,” and “high” groups for each environmental variable. The environmental stratification thresholds were then varied in a series of sensitivity tests. Several noteworthy correlations were observed between the convective and aerosol parameters within the environmental groups, especially when stratifying the environments based on their 850–500-hPa temperature lapse rate, 700–500-hPa temperature lapse rate, and K-Index. The convective parameters were often correlated most strongly with 355-nm extinction, 532-nm extinction, and 532-nm backscatter, while the presence of precipitation-sized liquid and ice hydrometeors contributed to some unexpected negative correlations. In general, as environmental conditions became more favorable for convection, a stronger correlation was observed between the convective parameters and aerosol concentrations. However, a “Goldilocks” zone of medium aerosol concentration was correlated most strongly with the convective parameters in many cases. These results stress the importance of considering environmental and aerosol conditions together when evaluating their impacts on convection. This presentation will provide a detailed discussion of these results and their implications, a summary of the limitations associated with such an analysis, and suggestions for future work.

Corey G. Amiot↗

NASA NTRS2024

Critical Load Exceedances for North America and Europe using an Ensemble of Models and an Investigation of Causes for Environmental Impact Estimate Variability: An AQMEII4 Study

Exceedances of critical loads for deposition of sulphur (S) and nitrogen (N) to different ecosystems were estimated using European and North American ensembles of air quality models, under Phase 4 of the Air Quality Model Evaluation International Initiative (AQMEII4), to identify where risk of ecosystem harm is expected to occur based on model deposition estimates. The ensembles were driven by common emissions and lateral boundary condition inputs. Model output was regridded to common North American and Europe 0.125° resolution domains, which were then used to calculate critical load exceedances. New, targeted deposition diagnostics implemented in AQMEII4 allowed an unprecedented level of post-simulation analysis to be carried out and facilitated the identification of specific causes of model-to-model variability in critical load exceedance estimates. New datasets for North American critical loads for acidity for forest soil water and aquatic ecosystems were combined with the ensemble deposition predictions to show a substantial decrease in the area and number of locations in exceedance between 2010 and 2016 (forest soils: 13.2 % to 6.1 %; aquatic ecosystems: 21.2 % to 11.4 %). All models agreed in the direction of the ensemble exceedance change between 2010 and 2016. The North American ensemble also predicted a decrease in both severity and total area in exceedance between the years 2010 and 2016 for eutrophication-impacted ecosystems in the USA (sensitive epiphytic lichen: 81.5 % to 75.8 %). The exceedances for herbaceous community richness also decreased between 2010 and 2016, from 13.9 % to 3.9 %. The uncertainty associated with the North American eutrophication results is high; there were sharp differences between the models in both predictions of total N deposition and the change in N deposition, and hence in the predicted eutrophication exceedances between the two years. The European ensemble was used to predict relatively static exceedances of critical loads with respect to acidification (4.48 % to 4.32 % from 2009 to 2010) while eutrophication exceedance increased slightly (60.2 % to 62.2 %). While most models showed the same changes in critical load exceedances as the ensemble between the two years, the spatial extent and magnitude of exceedances varied significantly between the models. The reasons for this variation were examined in detail by first ranking the relative contribution of different sources of sulphur and nitrogen deposition in terms of deposited mass and model-to-model variability in that deposited mass, followed by their analysis using AQMEII4 diagnostics, along with evaluation of the most recent literature. All models in both the North American and European ensembles had net annual negative biases with respect to observed wet deposition of sulphate, nitrate and ammonium. Diagnostics and recent literature suggest that this bias may stem from insufficient cloud scavenging of aerosols and gases, and may be improved through the incorporation of multiphase hydrometeor scavenging within the modelling frameworks. The inability of North American models to predict the timing of the seasonal peak in wet ammonium ion deposition (observed maximum was in April, while all models predicted a June maximum) may also relate to the need for multiphase hydrometeor scavenging (absence of snow scavenging in all models employed here). High variability in the relative importance of particulate sulphate, nitrate and ammonium deposition fluxes between models was linked to the use of updated particle dry deposition parameterizations in some models. However, recent literature and further development of some of the models within the ensemble suggests these particulate biases may also be ameliorated via the incorporation of multiphase hydrometeor scavenging. Annual sulphur and nitrogen deposition prediction variability was linked to SO 2 and HNO 3 dry deposition parameterizations, and diagnostic analysis showed that the cuticle and soil deposition pathways dominate the deposition mass flux of these species. Further work improving parameterizations for these deposition pathways should reduce variability in model acidifying gas deposition estimates. The absence of base cation chemistry in some models was shown to be a major factor in positive biases in fine mode particulate ammonium and particle nitrate concentrations. Models employing ammonia bidirectional fluxes had both the largest and the smallest magnitude biases, depending on the model and bidirectional flux algorithm employed. A careful analysis of bidirectional flux models suggests that those with poor NH 3 performance may underestimate the extent of NH 3 emissions fluxes from forested areas. Based on these results, an increased process-research focus is therefore recommended for the following model processes and on observations which may assist in model evaluation and improvement: multiphase hydrometeor scavenging combined with updated particle dry deposition, cuticle and soil deposition pathway algorithms for acidifying gases, base cation chemistry and emissions, and NH 3 bidirectional fluxes. Comparisons with satellite observations suggest that oceanic NH 3 emissions sources should be included in regional chemical transport models. The choice of land use database employed within any given model was shown to significantly influence deposition totals in several instances, and employing a common land use database across chemical transport models and critical load calculations is recommended for future work.

critical loads↗