ALBERT

Description: A significant source of ozone in the troposphere is transport from the stratosphere. The stratospheric contribution has been estimated mainly using global models that attribute the transport process largely to the global scale Brewer-Dobson circulation and synoptic scale dynamics associated with upper tropospheric jet streams. We report observations from research aircraft that reveal additional transport of ozone-rich stratospheric air downward into the upper troposphere by a leading-line-trailing-stratiform (LLTS) mesoscale convective system (MCS) with convection overshooting the tropopause altitude. The fine-scale transport demonstrated by these observations poses a significant challenge to global models that currently do not resolve storm scale dynamics. Thus the upper tropospheric ozone budget simulated by global chemistry-climate models where large-scale dynamics and photochemical production from lightning-produced NO are the controlling factors may require modification.

Description: We examine wet scavenging of soluble trace gases in storms observed during the Deep Convective Clouds and Chemistry (DC3) field campaign. We conduct high-resolution simulations with the Weather Research and Forecasting model with Chemistry (WRF-Chem) of a severe storm in Oklahoma. The model represents well the storm location, size, and structure as compared with NEXRAD reflectivity, and simulated CO transport is consistent with aircraft observations. Scavenging efficiencies (SEs) between inflow and outflow of soluble species are calculated from aircraft measurements and model simulations. Using a simple wet scavenging scheme, we simulate the SE of each soluble species within the error bars of the observations. The simulated SEs of all species except nitric acid (HNO 3 ) are highly sensitive to the values specified for the fractions retained in ice when cloud water freezes. To reproduce the observations, we must assume zero ice retention for formaldehyde (CH 2 O) and hydrogen peroxide (H 2 O 2 ) and complete retention for methyl hydrogen peroxide (CH 3 OOH) and sulfur dioxide (SO 2 ), likely to compensate for the lack of aqueous chemistry in the model. We then compare scavenging efficiencies among storms that formed in Alabama and northeast Colorado and the Oklahoma storm. Significant differences in SEs are seen among storms and species. More scavenging of HNO 3 and less removal of CH 3 OOH are seen in storms with higher maximum flash rates, an indication of more graupel mass. Graupel is associated with mixed phase scavenging and lightning production of nitrogen oxides (NO x ), processes that may explain the observed differences in HNO 3 and CH 3 OOH scavenging.

Description: Biogenic volatile organic compounds (BVOC) are oxidized quickly in the atmosphere to form oxygenated VOC (OVOC) and play crucial roles in the formation of ozone and secondary organic aerosols. We use the National Center for Atmospheric Research's Large-Eddy Simulation (LES) model and DISCOVER-AQ 2011 flight data to understand the role of boundary layer turbulence on the atmospheric chemistry of key BVOC species and their oxidation products. We simulate three distinct convective environments during the campaign, representing fair weather conditions (Case 1: 1 July), a convective event dominated by southwesterly flow (Case 2: 11 July) and a polluted event with high temperature and convection (Case 3: 29 July). Isoprene segregation is greatest in the lower boundary layer under warm and convective conditions, reaching up to a 10% reduction in the isoprene-OH reaction rate. Under warm and convective conditions, the BVOC lifetimes lengthen due to increased isoprene emission, elevated initial chemical concentrations and OH competition. Although turbulence-driven segregation has less influence on the OVOC species, convection mixes more OVOC into the upper atmospheric boundary layer (ABL) and increases the total OH reactivity. Production and loss rates of ozone above 2 km in all the three cases indicate in situ ozone formation in addition to vertical convective transport of ozone from the surface and aloft, consistent with the increased contribution of OH reactivity from OVOC. Together, these results show that total OH reactivity in the ABL increases under warmer and stronger convective conditions due to enhanced isoprene emission and the OVOC contribution to ozone formation.

Description: To study aerosol-cloud interactions over the Gangetic Basin of India, the Weather Research and Forecasting model coupled with chemistry (WRF-Chem) has been applied to a typical monsoon depression event prevalent between the 23rd and 29th August 2009. This event was sampled during the Cloud Aerosol Interaction and Precipitation Enhancement EXperiment (CAIPEEX) aircraft campaign, providing measurements of aerosol and cloud microphysical properties from two sorties. Comparison of the simulated meteorological, thermodynamical and aerosol fields against satellite and in-situ aircraft measurements illustrated that the westward propagation of the monsoon depression and the cloud, aerosol and rainfall spatial distribution were simulated reasonably well using MACCity+INTEX-B anthropogenic emission rates. However,the magnitude of aerosol optical depth was underestimated, by up to 50%. A simulation with aerosol emissions increased by a factor of 6 over the CAIPEEX campaign domain increased the simulated aerosol concentrations to values close to the observations, mainly within boundary layer. Comparison of the low aerosol simulation and high aerosol simulation for the two sorties illustrated that more anthropogenic aerosols increased the cloud condensing nuclei (CCN) and cloud droplet mass concentrations. The number of simulated cloud droplets increased while the cloud droplet effective radii decreased, highlighting the importance of CCN-cloud feedbacks over this region. The increase in simulated anthropogenic aerosols (including absorbing aerosols) also increased the temperature of air parcels below clouds and thus the convective available potential energy (CAPE). The increase in CAPE intensified the updraft and invigorated the cloud, inducing formation of deeper clouds with more ice phase hydrometeors for both the cases. These case studies provide evidence of aerosol-induced cloud invigoration over the Gangetic Basin.

Description: We investigate diurnal variability of isoprene and related chemical species in the Amazonian region. The dynamics and chemistry of an atmospheric boundary layer are studied with a large-eddy simulation code and a mixed-layer model which are guided by observations available for the same area. The main features of isoprene and related species are reproduced well, but their evolution raises questions regarding the physical and chemical processes responsible for the observed diurnal behaviors. To address these questions, we systematically examine the role of (1) the exchange of chemical species between the free troposphere and the atmospheric boundary layer (entrainment), (2) surface isoprene and nitric oxide emissions, and (3) new chemical pathways to recycle the hydroxyl radical. The entrainment flux of isoprene is shown to be equally important as surface isoprene emissions in determining the isoprene temporal evolution. Varying the relationship between the initial isoprene mixing ratio in the boundary layer and that in the overlying free troposphere in the early morning results in an 50% increase/decrease in isoprene mixing ratio or more within the atmospheric boundary layer at noon. Entrainment of free tropospheric nitrogen oxides creates changes of similar magnitude to the boundary layer isoprene mixing ratio. These effects of entrainment and surface emissions on isoprene are found for two different chemical regimes. The introduction of an OH recycling pathway in the chemical mechanism increases midday OH. Our findings show that atmospheric dynamics and chemistry are equally important for interpreting the diurnal observation of reactants and for including in regional-scale modeling efforts where turbulence is parameterized.

Description: We present an aerosol–cloud-precipitation modeling study of convective clouds using the fully coupled meteorology chemical model WRF-Chem version 3.1.1. Comparison of the model output with measurements from a research site in the Rocky Mountains in Colorado revealed that the fraction of organics in the model is underpredicted. This is most likely due to missing processes in the aerosol module in the model version used, such as new particle formation and growth of secondary organic aerosols. When boundary conditions and domain wide initial conditions of aerosol loading are changed in the model (factors of 0.1, 0.2 and 10 of initial aerosol mass of SO 4 −2 , NH 4 + and NO 3 − ), the domain wide precipitation changes by about 5%. Analysis of the model results reveals that the Rocky Mountain region and Front Range environment is not conducive for convective invigoration to play a major role, or to be sustained, in increasing precipitation, as seen in some other studies. When localized organic aerosol emission are increased to mimic new particle formation, the resulting increased aerosol loading leads to increases in domain wide precipitation, opposite to what is seen in the model simulations with changed boundary and initial conditions.

Description: Deep convective transport of surface moisture and pollution from the planetary boundary layer to the upper troposphere and lower stratosphere affects the radiation budget and climate. This study analyzes the deep convective transport in three different convective regimes from the 2012 Deep Convective Clouds and Chemistry (DC3) field campaign: May 21 st Alabama airmass thunderstorms, May 29 th Oklahoma supercell severe storm, and June 11 th mesoscale convective system (MCS). Lightning data assimilation within the Weather Research and Forecasting (WRF) model coupled with chemistry (WRF-Chem) is utilized to improve the simulations of storm location, vertical structure and chemical fields. Analysis of vertical flux divergence shows that deep convective transport in the May 29 th supercell case is the strongest per unit area while transport of boundary layer insoluble trace gases is relatively weak in the MCS and airmass cases. The weak deep convective transport in the strong MCS is unexpected and is caused by the injection into low levels of mid-level clean air by a strong rear inflow jet. In each system, the magnitude of tracer vertical transport is more closely related to the vertical distribution of mass flux density than the vertical distribution of trace gas mixing ratio. Finally, the net vertical transport is strongest in high composite reflectivity regions and dominated by upward transport.

Description: We investigate the impacts of cloud aqueous processes on the chemistry and transport of biogenic volatile organic compounds (BVOC) using the National Center for Atmospheric Research's large-eddy simulation code with an updated chemical mechanism that includes both gas- and aqueous-phase reactions. We simulate transport and chemistry for a meteorological case with a diurnal pattern of non-precipitating cumulus clouds from the Baltimore-Washington area DISCOVER-AQ campaign. We evaluate two scenarios with and without aqueous-phase chemical reactions. In the cloud layer (2-3 km), the addition of aqueous phase reactions decreases HCHO by 18% over the domain due to its solubility and the fast depletion from aqueous reactions, resulting in a corresponding decrease in radical oxidants (e.g., 18% decrease in OH). The decrease of OH increases the mixing ratios of isoprene and MACR (100% and 15%, respectively) in the cloud layer because the reaction rate is lower. Aqueous-phase reactions can modify the segregation between OH and BVOC by changing the sign of the segregation intensity, causing up to 55% reduction in the isoprene-OH reaction rate and 40% reduction for the MACR-OH reaction when clouds are present. Analysis of the isoprene-OH covariance budget shows the chemistry term is the primary driver of the strong segregation in clouds, triggered by the decrease in OH. All organic acids except acetic acid are formed only through aqueous-phase reactions. For acids formed in the aqueous phase, turbulence mixes these compounds on short time scales, with the near-surface mixing ratios of these acids reaching 20% of the mixing ratios in the cloud layer within one hour of cloud formation.

Description: [1]  This study investigates the responses of the direct radiative effect of light absorbing and scattering carbonaceous and sulfate aerosols on cloudiness and associated radiative fluxes using an interactive aerosol-climate model based on the NCAR Community Atmospheric Model (CAM-MIT aerosol model) coupled with a slab ocean model. Three simulations that include respectively the radiative effect of only light-scattering aerosols, only absorbing aerosols, and both absorbing and scattering aerosols are compared to a simulation that excludes the radiative effects of these aerosols. We find that without including the impact of aerosols on cloud microphysics in the model (indirect effect), the direct radiative effect of aerosols alone can cause a change in cloud coverage and thus in cloud flux change which is consistent with several previous studies. More notably, our result indicates that the direct radiative effect of absorbing aerosols can cause changes in both low-level and high-level clouds with opposite signs. As a result, the global mean cloud radiation response to absorbing aerosols has a rather small value. The change of cloud solar radiative response (all-sky effect minus clear-sky effect) at the top of the atmosphere due to the existence of direct radiative effect of scattering, absorbing, and both types of aerosols is 0.72, 0.08, and 0.81 Wm -2 , respectively, all are comparable in quantity to the current estimation of aerosol direct radiative forcing. The cloud response due to the longwave radiative effect is 0.09, 0.18, and 0.27 Wm -2 , respectively. The global means of the radiative flux and cloud radiative responses appear to be linearly additive, however, this is definitely not the case for the zonal mean or at the regional scale.

Description: [1]  Simulations of observed convective systems with the Advanced Research Weather Research and Forecasting (ARW-WRF) model are used to test the influence of the large-scale lower stratosphere stability environment on the vertical extent of convective overshooting and transport above the extratropical tropopause. Three unique environments are identified (double tropopause, stratospheric intrusion, and single tropopause), and representative cases with comparable magnitudes of convective available potential energy are selected for simulation. Convective injection into the extratropical lower stratosphere is found to be deepest for the double tropopause case (up to 4 km above the lapse-rate tropopause), and at comparable altitudes for the remaining cases (up to 2 km above the lapse-rate tropopause). All simulations show evidence of gravity wave breaking near the overshooting convective top, consistent with the identification of its role as a transport mechanism in previous studies. Simulations for thedouble tropopause case, however, also show evidence of direct mixing of the overshooting top into the lower stratosphere, which is responsible for the highest levels of injection in that case. In addition, the choice of bulk microphysical parameterization for ARW-WRF simulations is found to have little impact on the transport characteristics for each case.