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At least 19 records

Opinion: A critical evaluation of the evidence for aerosol invigoration of deep convection

Deep convective updraft invigoration via indirect effects of increased aerosol number concentration on cloud microphysics is frequently cited as a driver of correlations between aerosol and deep convection properties. Here, we critically evaluate the theoretical, modeling, and observational evidence for warm- and cold-phase invigoration pathways. Though warm-phase invigoration is plausible and theoretically supported via lowering of the supersaturation with increased cloud droplet concentration in polluted conditions, the significance of this effect depends on substantial supersaturation changes in real-world convective clouds that have not been observed. Much of the theoretical support for cold-phase invigoration depends on unrealistic assumptions of instantaneous freezing and unloading of condensate in growing, isolated updrafts. When applying more realistic assumptions, impacts on buoyancy from enhanced latent heating via fusion in polluted conditions are largely canceled by greater condensate loading. Many foundational observational studies supporting invigoration have several fundamental methodological flaws that render their findings incorrect or highly questionable. Thus, much of the evidence for invigoration has come from numerical modeling, but different models and setups have produced a vast range of results. Furthermore, modeled aerosol impacts on deep convection are rarely tested for robustness, and microphysical biases relative to observations persist, rendering many results unreliable for application to the real world. Without clear theoretical, modeling, or observational support, and given that enervation rather than invigoration may occur for some deep convective regimes and environments, it is entirely possible that the overall impact of cold-phase invigoration is negligible. Substantial mesoscale variability of dominant thermodynamic controls on convective updraft strength coupled with substantial updraft and aerosol variability in any given event are poorly quantified by observations and present further challenges to isolating aerosol effects. Observational isolation and quantification of convective invigoration by aerosols is also complicated by limitations of available cloud condensation nuclei and updraft speed proxies, aerosol correlations with meteorological conditions, and cloud impacts on aerosols. Furthermore, many cloud processes, such as entrainment and condensate fallout, modulate updraft strength and aerosol–cloud interactions, varying with cloud life cycle and organization, but these processes remain poorly characterized. Considering these challenges, recommendations for future observational and modeling research related to aerosol invigoration of deep convection are provided.

54 ENVIRONMENTAL SCIENCES↗

Parameterizing deep convection using the assumed probability density function method

Due to their coarse horizontal resolution, present-day climate models must parameterize deep convection. This paper presents single-column simulations of deep convection using a probability density function (PDF) parameterization. The PDF parameterization predicts the PDF of subgrid variability of turbulence, clouds, and hydrometeors. That variability is interfaced to a prognostic microphysics scheme using a Monte Carlo sampling method.The PDF parameterization is used to simulate tropical deep convection, the transition from shallow to deep convection over land, and mid-latitude deep convection.These parameterized single-column simulations are compared with 3-D reference simulations. The agreement is satisfactory except when the convective forcing is weak. The same PDF parameterization is also used to simulate shallow cumulus and stratocumulus layers. The PDF method is sufficiently general to adequately simulate these five deep, shallow, and stratiform cloud cases with a single equation set. This raises hopes that it may be possible in the future, with further refinements at coarse time step and grid spacing, to parameterize all cloud types in a large-scale model in a unified way.

Storer, R. L.↗

Probing the transition from shallow to deep convection using ASR data and large-eddy simulations

Over the duration of this project, we have made the following advances. 1) We have developed a novel approach to obtain a Lagrangian view of convection from high-resolution numerical model through Lagrangian tracking. This approach nicely complements the more traditionally used Eulerian statistics. We have applied this approach to a range of problem. 2) We have looked into improving and extending our parameterizations based on stochastically entraining parcels, developed previously for shallow convection. 3) This grant also supported our effort on a paper where we compared cumulus parameterizations and cloud resolving models in terms of their linear response functions. This work will help the community to better evaluate and develop cumulus parameterization. 4) We have applied Lagrangian tracking to shallow convection, deep convection with and without convective organization to better characterize their dynamics and the transition between them. 5) We have devised a novel way of using Lagrangian to identify cold pools, an area identified as of great interest by the ASR community. Our algorithm has a number of advantages and in particular can handle merging cold pools more gracefully than existing techniques. 6) We demonstrated that we can, for the first time, correctly reproduce both the diurnal and seasonal cycle of the hydrologic cycle in the Amazon using a strategy that explicitly represents convection but parameterizes large-scale circulation. In addition we showed that the main cause of the wet season is the presence of an early morning fog, which insulate the surface from top of the atmosphere shortwave radiation. In essence this fog makes the day shorter because radiation cannot penetrate to the surface in the early morning. This is why all fluxes are reduced in the wet season compared to the dry season. 7) We have investigated the life cycle of cold pools and the role of surface diabatic heating. We show that surface heating can kill cold pols and reduce the number of large cold pools and the organization of convection. The effect is quite dramatic over land where the entire distribution of cold pools is modified, and the cold pools are much warmer and more humid with surface diabatic heating below the cold pools. The PI and the co-PI continue to work together on parameterization of cold pools.

54 ENVIRONMENTAL SCIENCES↗

Transport and chemistry of isoprene and its oxidation products in deep convective clouds

Deep convective clouds can transport trace gases from the planetary boundary layer into the upper troposphere where subsequent chemistry may impact aerosol particle formation and growth. In this modelling study, we investigate processes that affect isoprene and its oxidation products injected into the upper troposphere by an isolated deep convective cloud in the Amazon. We run a photochemical box model with coupled cloud microphysics along hundreds of individual air parcel trajectories sampled from a cloud-resolving model simulation of a convective event. The box model simulates gas-phase chemical reactions, gas scavenging by liquid and ice hydrometeors, and turbulent dilution inside a deep convective cloud. The results illustrate the potential importance of gas uptake to anvil ice in regulating the intensity of the isoprene oxidation and associated low volatility organic vapour concentrations in the outflow. Isoprene transport and fate also depends on the abundance of lightning-generated nitrogen oxide radicals (NO x = NO + NO 2 ). If gas uptake on ice is efficient and lightning activity is low, around 30% of the boundary layer isoprene will survive to the cloud outflow after approximately one hour of transport, while all the low volatile oxidation products will be scavenged by the cloud hydrometeors. If lightning NO x is abundant and gas uptake by ice is inefficient, then all isoprene will be oxidised during transport or in the immediate outflow region, while several low volatility isoprene oxidation products will have elevated concentrations in the cloud outflow. Reducing uncertainties associated with the uptake of vapours on ice hydrometeors, especially HO 2 and oxygenated organics, is essential to improve predictions of isoprene and its oxidation products in deep convective outflows and their potential contribution to new particle formation and growth.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Evaluation of a Stochastic Mixing Scheme in the Deep Convective Gray Zone Using a Tropical Oceanic Deep Convection Case Study

Abstract A stochastic horizontal subgrid‐scale mixing scheme is evaluated in ensemble simulations of a tropical oceanic deep convection case using a horizontal grid spacing (Δ h ) of 3 km. The stochastic scheme, which perturbs the horizontal mixing coefficient according to a prescribed spatiotemporal autocorrelation scale, is found to generally increase mesoscale organization and convective intensity relative to a non‐stochastic control simulation. Perturbations applied at relatively short autocorrelation scales induce differences relative to the control that are more systematic than those from perturbations applied at relatively long scales that yield more variable outcomes. A simulation with mixing enhanced by a constant factor of 4 significantly increases mesoscale organization and convective intensity, while turning off horizontal subgrid‐scale mixing decreases both. Total rainfall is modulated by a combination of mesoscale organization, areal coverage of convection, and convective intensity. The stochastic simulations tend to behave more similarly to the constant enhanced mixing simulation owing to greater impacts from enhanced mixing as compared to reduced mixing. The impacts of stochastic mixing are robust, ascertained by comparing the stochastic mixing ensembles with a non‐stochastic mixing ensemble that has grid‐scale noise added to the initial thermodynamic field. Compared to radar observations and a higher resolution Δ h = 1 km simulation, stochastic mixing seemingly degrades the simulation performance. These results imply that stochastic mixing produces non‐negligible impacts on convective system properties and evolution but does not lead to an improved representation of convective cloud characteristics in the case studied here.

54 ENVIRONMENTAL SCIENCES↗

Seasonal variation of shallow-to-deep convection transition and its link to the environmental conditions over the Central Amazon: Shallow-to-Deep Convection Transition

This study aims to characterize the seasonal variation of the shallow-to-deep convection transition and understand how environmental conditions impact the behavior of this transition using data collected from the Observations and Modeling of the Green Ocean Amazon (GOAmazon) field campaign in the Central Amazon (Manaus). The diurnal cycle of the rain/cloud fraction shows that the wet season has more extensive shallow convection before the transition to deep convection with larger fractional coverage and rainfall; deep convection in the transition season is more intense and has higher vertical extension and a stronger updraft. Surface meteorology, atmospheric moisture, instability, and wind shear are contrasted for the shallow/congestus convection (SC) cases and the locally formed shallow-to-deep convection transition (LD) cases. The comparisons suggest that occurrence of the LD is generally promoted under the conditions of high atmospheric moisture and instability but has a weaker dependence on wind shear. The relative importance of these environmental controls also varies in different seasons: The dry and transition seasons require a deeper moist layer from the boundary layer to midtroposphere than the wet season; convective available potential energy (CAPE) is higher during the transition season, but it is a less important factor for shallow-to-deep convection transition than in other seasons; LD only has significantly larger wind shears than SC during the dry season.

54 ENVIRONMENTAL SCIENCES↗

Advection, moistening, and shallow‐to‐deep convection transitions during the initiation and propagation of M adden‐ J ulian O scillation

Abstract Using observations from the 2011 AMIE/DYNAMO field campaign over the Indian Ocean and a high‐resolution regional model simulation, the processes that lead to the rapid shallow‐to‐deep convection transitions associated with the initiation and eastward propagation of the Madden‐Julian Oscillation (MJO) are examined. By tracking the evolution of the depth of several thousand individual model simulated precipitation features, the role of and the processes that control the observed midtropospheric moisture buildup ahead of the detection of deep convection are quantified at large and convection scales. The frequency of shallow‐to‐deep convection transitions is found to be sensitive to this midlevel moisture and large‐scale uplift. This uplift along with the decline of large‐scale drying by equator‐ward advection causes the moisture buildup leading to the initiation of the MJO. Convection scale moisture variability and uplift, and large‐scale zonal advection play secondary roles.

Hagos, Samson↗

A PDF-Based Parameterization of Subgrid-Scale Hydrometeor Transport in Deep Convection

Abstract A parameterization scheme is proposed for the subgrid-scale transport of hydrometeors in an assumed probability density function (PDF) scheme. Joint distributions of vertical velocity and hydrometeor mixing ratios are typically unknown, but marginal (1D) PDFs of these variables are available. The parameterization is developed using high-resolution simulations of continental and tropical deep convection. A 3D cloud-resolving model (CRM) providing benchmark solutions has a horizontal grid spacing of 250 m and employs the Morrison microphysics scheme, which treats prognostically mass and number mixing ratios for four types of precipitating hydrometeors (rain, graupel, snow, and ice) as well as cloud droplet number mixing ratio. The subgrid-scale hydrometeor transport scheme assumes input given in the form of marginal PDFs of vertical velocity and hydrometeor mixing ratios; in this study, these marginal distributions are provided by the cloud-resolving model. Conditional sampling and scaling are then applied to the marginal distributions to account for subplume correlations. The parameterized fluxes tested for four episodes of deep convection show good agreement with benchmark fluxes computed directly from the CRM output. The results demonstrate the potential use of the subgrid-scale hydrometeor transport scheme in an assumed PDF scheme to parameterize the covariances of vertical velocity and hydrometeor mixing ratios.

Wong, May↗

A high-resolution unified observational data product of mesoscale convective systems and isolated deep convection in the United States for 2004–2017

Deep convection possesses markedly distinct properties at different spatiotemporal scales. We present an original high-resolution (4 km, hourly) unified data product of mesoscale convective systems (MCSs) and isolated deep convection (IDC) in the United States east of the Rocky Mountains and examine their climatological characteristics from 2004 to 2017. The data product is produced by applying an updated Flexible Object Tracker algorithm to hourly satellite brightness temperature, radar reflectivity, and precipitation datasets. Analysis of the data product shows that MCSs are much larger and longer-lasting than IDC, but IDC occurs about 100 times more frequently than MCSs, with a mean convective intensity comparable to that of MCSs. Hence both MCS and IDC are essential contributors to precipitation east of the Rocky Mountains, although their precipitation shows significantly different spatiotemporal characteristics. IDC precipitation concentrates in summer in the Southeast with a peak in the late afternoon, while MCS precipitation is significant in all seasons, especially for spring and summer in the Great Plains. The spatial distribution of MCS precipitation amounts varies by season, while diurnally, MCS precipitation generally peaks during nighttime except in the Southeast. Potential uncertainties and limitations of the data product are also discussed. The data product is useful for investigating the atmospheric environments and physical processes associated with different types of convective systems; quantifying the impacts of convection on hydrology, atmospheric chemistry, and severe weather events; and evaluating and improving the representation of convective processes in weather and climate models.

54 ENVIRONMENTAL SCIENCES↗

Dependence of Deep Convective Cell Properties on Meteorological and Aerosol Conditions during TRACER

Deep convective cells significantly influence Earth’s energy balance and water cycle. However, their accurate representation in numerical models remains challenging due to their small spatiotemporal scales and limited observational constraints. This study examines over ∼400 deep convective cells near Houston, observed by a dual-polarization C-band radar during the Tracking Aerosol Convection Interactions Experiment (TRACER) intensive observation period (June–September 2022). Cells are categorized by lifetime into short-lived (<40 min), intermediate-lived (40–80 min), and long-lived (80+ min) groups. Long-lived cells were broader (∼13.2 km at 2–4-km height) and deeper (∼11.4 km) than short-lived cells (∼6.4-km width, ∼7.31-km height). Using random forest (RF) modeling and correlation analyses, precipitable water vapor (PWV), 2–6-km lapse rate, 0–8-km bulk shear, and fine aerosol mass concentration (Mass_f) are identified as key predictors of cell lifetime. Higher PWV is associated with significantly longer convective cell lifetimes compared to the low-PWV group, particularly within low 2–6-km temperature lapse rate (LR_26km), moderate-to-higher 0–8-km bulk shear (BS_08km), and low-to-moderate Mass_f environments. RF analysis also identifies low-level (0–2 km) equivalent potential temperature, PWV, Mass_f, and surface latent heat flux as key predictors for cell width and height. Short-lived cells have higher aerosol number concentrations (500–1000-nm size range), linked to onshore wind conditions and marine aerosols; however, their low concentration suggests the sensitivity may reflect associated meteorological regimes rather than a direct aerosol effect. Long-lived cells have higher concentrations of organic and sulfate aerosols, while short-lived cells exhibit higher black carbon concentrations. These results highlight the intricate dependence of convective cell lifetimes and structure on environmental moisture, thermodynamics, wind shear, and aerosol characteristics.

54 ENVIRONMENTAL SCIENCES↗

Effects of Scavenging, Entrainment, and Aqueous Chemistry on Peroxides and Formaldehyde in Deep Convective Outflow Over the Central and Southeast United States

Deep convective transport of gaseous precursors to ozone (O3) and aerosols to the upper troposphere is affected by liquid phase and mixed-phase scavenging, entrainment of free tropospheric air and aqueous chemistry. The contributions of these processes are examined using aircraft measurements obtained in storm inflow and outflow during the 2012 Deep Convective Clouds and Chemistry (DC3) experiment combined with high-resolution (dx = 3 km) WRF-Chem simulations of a severe storm, an air mass storm, and a mesoscale convective system (MCS). The simulation results for the MCS suggest that formaldehyde (CH2O) is not retained in ice when cloud water freezes, in agreement with previous studies of the severe storm. By analyzing WRF-Chem trajectories, the effects of scavenging, entrainment, and aqueous chemistry on outflow mixing ratios of CH2O, methyl hydroperoxide (CH3OOH), and hydrogen peroxide (H2O2) are quantified. Liquid phase microphysical scavenging was the dominant process reducing CH2O and H2O2 outflow mixing ratios in all three storms. Aqueous chemistry did not significantly affect outflow mixing ratios of all three species. In the severe storm and MCS, the higher than expected reductions in CH3OOH mixing ratios in the storm cores were primarily due to entrainment of low-background CH3OOH. In the air mass storm, lower CH3OOH and H2O2 scavenging efficiencies (SEs) than in the MCS were partly due to entrainment of higher background CH3OOH and H2O2. Overestimated rain and hail production in WRF-Chem reduces the confidence in ice retention fraction values determined for the peroxides and CH2O.

Bela, Megan↗

Environmental Thermodynamic Effects on Future Changes of Mesoscale Convective Systems and Isolated Deep Convection Over the US: A Case Study

Mesoscale convective systems (MCSs) and isolated deep convection (IDC) significantly influence local weather conditions and the hydrological cycle across the United States. Their future changes under warming is critical to the society. However, the exact impacts of thermodynamic environmental changes on them are difficult to resolve using climate model simulations which integrate both dynamic and thermodynamic factors. This study explores a theoretical modeling approach to isolate environmental thermodynamic effects on their future changes through a case study. For a 50-day period during the 2020 summer, a pair of convection-permitting model simulations indicate contrasting changes in MCSs and IDC between inland and coastal regions under pseudo global warming. Driven by the thermodynamic environments of these simulations, a single-column parcel model indicates a decrease in the frequency of IDC occurrences, along with increases in duration and precipitation amount under warming, attributable to rising most unstable convective available potential energy (MUCAPE), convective inhibition (MUCIN), and precipitable water (PW). A multi-column parcel model reveals contrasting changes in the frequency and mean area of MCSs between inland and coastal regions, underscoring the increase in mean MUCIN over inland regions and increases in mean MUCAPE and PW over coastal regions. The increase in mean MCS area over inland regions is linked to the interplay between accelerated gust fronts and enhanced subsidence strength, which is further traced to the unchanged mean MUCIN but increased mean MUCAPE in large-scale environments. In conclusion, these case study results suggest a major role of thermodynamic environmental changes in controlling characteristics of MCSs and IDC under warming.

Mesoscale convective system↗

A high-resolution database of mesoscale convective systems and isolated deep convection in the United States for 2004 – 2017

The database provides high-resolution (4-km, hourly) information of mesoscale convective systems (MCSs) and isolated deep convection events (IDC) east of the Rocky Mountains over the contiguous United States from 2004 – 2017. The database contains various characteristics of MCSs and IDC, such as their lifecycle evolutions, lifetimes, spatial coverages, echo-top heights, precipitation features, convective and stratiform separation, convective core features, propagation speed, etc.

54 ENVIRONMENTAL SCIENCES↗

A high-resolution database of mesoscale convective systems and isolated deep convection in the United States for 2004 – 2017

The database provides high-resolution (4-km, hourly) information of mesoscale convective systems (MCSs) and isolated deep convection events (IDC) east of the Rocky Mountains over the contiguous United States from 2004 – 2017. The database contains various characteristics of MCSs and IDC, such as their lifecycle evolutions, lifetimes, spatial coverages, echo-top heights, precipitation features, convective and stratiform separation, convective core features, propagation speed, etc.

54 ENVIRONMENTAL SCIENCES↗

An Observational Comparison of Level of Neutral Buoyancy and Level of Maximum Detrainment in Tropical Deep Convective Clouds

Tropical deep convective clouds are important drivers of large-scale atmospheric circulation representing the main vertical transport pathway through the depth of the troposphere for heat, momentum, water, and chemical species. The strength and depth of this transport are impacted by the convective updraft size and intensity that are driven by buoyancy, dynamical forcing, and mixing of environmental air, i.e., entrainment. In this paper, we identify tropical deep convective systems with well-defined forward anvils using Atmospheric Radiation Measurement (ARM) ground-based profiling radars, at three ARM fixed-sites in the Tropical Western Pacific (TWP; i.e., Manus, Nauru, Darwin) and three ARM Mobile Facility deployments in Niamey, Niger; Gan Island, Maldives; and Manacapuru, Brazil. We use the difference between the level of neutral buoyancy (LNB) and the level of maximum detrainment (LMD) as a proxy for the effective bulk convective entrainment (εproxy). The LNB, the theoretical height that a parcel raised above the level of free convection would reach with no mixing, is calculated based on pre-convection radiosonde measurements using parcel theory. The LMD is the height of the maximum reflectivity observed in forward anvil clouds by profiling radars. Deep convective systems over the TWP show higher LNBs that extend to 16.3 km on average and larger εproxy (median LNB minus LMD up to 6.5 km) compared to their continental counterparts in the Amazon and West Africa. Oceanic conditions show larger convective available potential energy (CAPE) coupled with higher moisture at low levels which favors larger εproxy. In contrast, continental cases initiate and develop under high convective inhibition, steeper environmental lapse rate, and high wind shear conditions, which show smaller offset between LNB and LMD. Deep convective cases that promote significant cold pools at the surface experience less εproxy. Using a Random Forest regression algorithm, CAPE is associated with the highest feature importance score for predicting convective εproxy, followed by low-level relative humidity. For continental cases, the low-level wind shear also indicates higher importance.

54 ENVIRONMENTAL SCIENCES↗

Evaluation of Cloud-resolving and Limited Area Model Intercomparison Simulations using TWP-ICE Observations. Part 1: Deep Convective Updraft Properties

Ten 3D cloud-resolving model (CRM) simulations and four 3D limited area model (LAM) simulations of an intense mesoscale convective system observed on January 23-24, 2006 during the Tropical Warm Pool – International Cloud Experiment (TWP-ICE) are compared with each other and with observed radar reflectivity fields and dual-Doppler retrievals of vertical wind speeds in an attempt to explain published results showing a high bias in simulated convective radar reflectivity aloft. This high bias results from ice water content being large, which is a product of large, strong convective updrafts, although hydrometeor size distribution assumptions modulate the size of this bias. Snow reflectivity can exceed 40 dBZ in a two-moment scheme when a constant bulk density of 100 kg m-3 is used. Making snow mass more realistically proportional to area rather than volume should somewhat alleviate this problem. Graupel, unlike snow, produces high biased reflectivity in all simulations. This is associated with large amounts of liquid water above the freezing level in updraft cores. Peak vertical velocities in deep convective updrafts are greater than dual-Doppler retrieved values, especially in the upper troposphere. Freezing of large rainwater contents lofted above the freezing level in simulated updraft cores greatly contributes to these excessive upper tropospheric vertical velocities. Strong simulated updraft cores are nearly undiluted, with some showing supercell characteristics. Decreasing horizontal grid spacing from 900 meters to 100 meters weakens strong updrafts, but not enough to match observational retrievals. Therefore, overly intense simulated updrafts may partly be a product of interactions between convective dynamics, parameterized microphysics, and large-scale environmental biases that promote different convective modes and strengths than observed.

clould-resolving↗

Improving Convection Trigger Functions in Deep Convective Parameterization Schemes Using Machine Learning

Abstract Deficiencies in convection trigger functions, used in deep convection parameterizations in General Circulation Models (GCMs), have critical impacts on climate simulations. A novel convection trigger function is developed using the machine learning (ML) classification model XGBoost. The large‐scale environmental information associated with convective events is obtained from the long‐term constrained variational analysis forcing data from the Atmospheric Radiation Measurement (ARM) program at its Southern Great Plains (SGP) and Manaus (MAO) sites representing, respectively, continental mid‐latitude and tropical convection. The ML trigger is separately trained and evaluated per site, and jointly trained and evaluated at both sites as a unified trigger. The performance of the ML trigger is compared with four convective trigger functions commonly used in GCMs: dilute convective available potential energy (CAPE), undilute CAPE, dilute dynamic CAPE (dCAPE), and undilute dCAPE. The ML trigger substantially outperforms the four CAPE‐based triggers in terms of the F 1 score metric, widely used to estimate the performance of ML methods. The site‐specific ML trigger functions can achieve, respectively, 91% and 93% F 1 scores at SGP and MAO. The unified trigger also has a 91% F 1 score, with virtually no degradation from the site‐specific training, suggesting the potential of a global ML trigger function. The ML trigger alleviates a GCM deficiency regarding the overprediction of convection occurrence, offering a promising improvement to the simulation of the diurnal cycle of precipitation. Furthermore, to overcome the black box issue of the ML methods, insights derived from the ML model are discussed, which may be leveraged to improve traditional CAPE‐based triggers.

54 ENVIRONMENTAL SCIENCES↗

Aerosol transport and wet scavenging in deep convective clouds: a case study and model evaluation using a multiple passive tracer analysis approach

The effect of wet scavenging on ambient aerosols in deep, continental convective clouds in the mid-latitudes is studied for a severe storm case in Oklahoma during the Deep Convective Clouds and Chemistry (DC3) field campaign. A new passive-tracer based transport analysis framework is developed to characterize the convective transport based on the vertical distribution of several slowly reacting and nearly insoluble trace gases. The passive gas concentration in the upper troposphere convective outflow results from a mixture of 47% from the lower level (0-3 km), 21% entrained from the upper troposphere, and 32% from mid-atmosphere based on observations. The transport analysis framework is applied to aerosols to estimate aerosol transport and wet-scavenging efficiency. Observations yield high overall scavenging efficiencies of 81% and 68% for aerosol mass (Dp < 1μm) and aerosol number (0.03< Dp < 2.5μm), respectively. Little chemical selectivity to wet scavenging is seen among observed submicron sulfate (84%), organic (82%), and ammonium (80%) aerosols, while nitrate has a much lower scavenging efficiency of 57% likely due to the uptake of nitric acid. Observed larger size particles (0.15 - 2.5μm) are scavenged more efficiently (84%) than smaller particles (64%; 0.03 - 0.15μm). The storm is simulated using the chemistry version of the WRF model. Compared to the observation based analysis, the standard model underestimates the wet scavenging efficiency for both mass and number concentrations with low biases of 31% and 40%, respectively. Adding a new treatment of secondary activation significantly improves simulation results, so that the bias in scavenging efficiency in mass and number concentrations is reduced to <10%. This supports the hypothesis that secondary activation is an important process for wet removal of aerosols in deep convective storms.

Yang, Qing↗