scholarly journals Cloud-scale modelling of the impact of deep convection on the fate of oceanic bromoform in the troposphere: a case study over the west coast of Borneo

2021 ◽  
Vol 21 (22) ◽  
pp. 16955-16984
Author(s):  
Paul D. Hamer ◽  
Virginie Marécal ◽  
Ryan Hossaini ◽  
Michel Pirre ◽  
Gisèle Krysztofiak ◽  
...  

Abstract. This paper presents a modelling study on the fate of CHBr3 and its product gases in the troposphere within the context of tropical deep convection. A cloud-scale case study was conducted along the west coast of Borneo, where several deep convective systems were triggered on the afternoon and early evening of 19 November 2011. These systems were sampled by the Falcon aircraft during the field campaign of the SHIVA project and analysed using a simulation with the cloud-resolving meteorological model C-CATT-BRAMS at 2×2 km resolution that represents the emissions, transport by large-scale flow, convection, photochemistry, and washout of CHBr3 and its product gases (PGs). We find that simulated CHBr3 mixing ratios and the observed values in the boundary layer and the outflow of the convective systems agree. However, the model underestimates the background CHBr3 mixing ratios in the upper troposphere, which suggests a missing source at the regional scale. An analysis of the simulated chemical speciation of bromine within and around each simulated convective system during the mature convective stage reveals that >85 % of the bromine derived from CHBr3 and its PGs is transported vertically to the point of convective detrainment in the form of CHBr3 and that the remaining small fraction is in the form of organic PGs, principally insoluble brominated carbonyls produced from the photo-oxidation of CHBr3. The model simulates that within the boundary layer and free troposphere, the inorganic PGs are only present in soluble forms, i.e. HBr, HOBr, and BrONO2, and, consequently, within the convective clouds, the inorganic PGs are almost entirely removed by wet scavenging. We find that HBr is the most abundant PG in background lower-tropospheric air and that this prevalence of HBr is a result of the relatively low background tropospheric ozone levels at the regional scale. Contrary to a previous study in a different environment, for the conditions in the simulation, the insoluble Br2 species is hardly formed within the convective systems and therefore plays no significant role in the vertical transport of bromine. This likely results from the relatively small quantities of simulated inorganic bromine involved, the presence of HBr in large excess compared to HOBr and BrO, and the relatively efficient removal of soluble compounds within the convective column.

2020 ◽  
Author(s):  
Paul D. Hamer ◽  
Virginie Marécal ◽  
Ryan Hossaini ◽  
Michel Pirre ◽  
Gisèle Krysztofiak ◽  
...  

Abstract. Coastal oceans emit bromoform (CHBr3) that can be transported rapidly to the upper troposphere by deep convection. In the troposphere, the spatial and vertical distribution of CHBr3 and its product gases (PGs) depend on emissions, chemical processing, transport by large scale flow, convection, and associated washout. This paper presents a modelling study on the fate of CHBr3 and its PGs in the troposphere. A case study at cloud scale was conducted along the west coast of Borneo, when several deep convective systems triggered in the afternoon and early evening of November 19th 2011. These systems were sampled by the Falcon aircraft during the field campaign of the SHIVA project. We analyse these systems using a simulation with the cloud-resolving meteorological model C-CATT-BRAMS at 2 × 2 km resolution that describes transport, photochemistry, and washout of CHBr3. We find that simulated CHBr3 mixing ratios and the observed values in the boundary layer and the outflow of the convective systems agree. However, the model underestimates the background CHBr3 mixing ratios in the upper troposphere, which suggests a missing source. An analysis of the simulated chemical speciation of bromine within and around each simulated convective system during the mature convective stage reveals that > 85 % of the bromine derived from CHBr3 and its PGs is transported vertically to the point of convective detrainment in the form of CHBr3 and that the remaining small fraction is in the form of organic PGs, principally insoluble brominated carbonyls produced from the photo-oxidation of CHBr3. The model simulates that within the boundary layer and free troposphere, the inorganic PGs are only present in soluble forms, i.e., HBr, HOBr, and BrONO2, and consequently, within the convective clouds, the inorganic PGs are almost entirely removed by wet scavenging. For the conditions of the simulated case study Br2 plays no significant role in the vertical transport of bromine. This likely results from the small simulated quantities of inorganic bromine involved, the presence of HBr in large excess compared to HOBr and the less soluble BrO, and the relatively quick removal of soluble compounds within the convective column. This prevalence of HBr is a result of the wider simulated regional atmospheric composition whereby background tropospheric ozone levels are exceptionally low.


2014 ◽  
Vol 14 (17) ◽  
pp. 8917-8931 ◽  
Author(s):  
H. Bozem ◽  
H. Fischer ◽  
C. Gurk ◽  
C. L. Schiller ◽  
U. Parchatka ◽  
...  

Abstract. Convective redistribution of ozone and its precursors between the boundary layer (BL) and the free troposphere (FT) influences photochemistry, in particular in the middle and upper troposphere (UT). We present a case study of convective transport during the GABRIEL campaign over the tropical rain forest in Suriname in October 2005. During one measurement flight the inflow and outflow regions of a cumulonimbus cloud (Cb) have been characterized. We identified a distinct layer between 9 and 11 km altitude with enhanced mixing ratios of CO, O3, HOx, acetone and acetonitrile. The elevated O3 contradicts the expectation that convective transport brings low-ozone air from the boundary layer to the outflow region. Entrainment of ozone-rich air is estimated to account for 62% (range: 33–91%) of the observed O3. Ozone is enhanced by only 5–6% by photochemical production in the outflow due to enhanced NO from lightning, based on model calculations using observations including the first reported HOx measurements over the tropical rainforest. The "excess" ozone in the outflow is most probably due to direct production by corona discharge associated with lightning. We deduce a production rate of 5.12 × 1028 molecules O3 flash−1 (range: 9.89 × 1026–9.82 × 1028 molecules O3 flash−1), which is at the upper limit of the range reported previously.


2014 ◽  
Vol 14 (4) ◽  
pp. 5233-5270 ◽  
Author(s):  
H. Bozem ◽  
H. Fischer ◽  
C. Gurk ◽  
C. L. Schiller ◽  
U. Parchatka ◽  
...  

Abstract. Convective redistribution of ozone and its precursors between the boundary layer (BL) and the free troposphere (FT) influences photochemistry, in particular that of the middle and upper troposphere (UT). We present a case study of convective transport during the GABRIEL campaign over the tropical rain forest in Suriname in October 2005. During a measurement flight on 12 October the inflow and outflow regions of a cumulonimbus cloud (Cb) have been characterized, providing evidence of convective transport. We identified a distinct layer between 9 and 11 km altitude with enhanced mixing ratios of CO, O3, HOx, acetone and acetonitrile. The elevated O3 contradicts the expectation that convective transport brings low ozone air from the boundary layer to the outflow region. The enhanced mixing ratio of ozone in the outflow was mainly of dynamical origin. Entrainment of ozone rich air at the outflow level into the convective outflow accounts for 62% (range: 33–91%) of the observed O3. Ozone is enhanced by only 5–6% by photochemical production in the outflow due to enhanced NO from lightning, based on steady state model calculations, using in-situ observations including the first reported HOx measurements over the tropical rainforest. The "excess" ozone in the outflow is most probably due to direct production by corona discharge associated with lightning. We deduce a production rate of 5.12 × 1028 molecules O3 flash−1 (range: 9.89 × 1026–9.82 × 1028 molecules O3 flash−1), which is at the upper limit of the range of the values reported previously.


2018 ◽  
Vol 133 ◽  
pp. 53-64 ◽  
Author(s):  
Linus Hasselström ◽  
Wouter Visch ◽  
Fredrik Gröndahl ◽  
Göran M. Nylund ◽  
Henrik Pavia

2005 ◽  
Vol 5 (4) ◽  
pp. 603-612 ◽  
Author(s):  
M. Zampieri ◽  
P. Malguzzi ◽  
A. Buzzi

Abstract. The "Montserrat-2000" severe flash flood event which occurred over Catalonia on 9 and 10 June 2000 is analyzed. Strong precipitation was generated by a mesoscale convective system associated with the development of a cyclone. The location of heavy precipitation depends on the position of the cyclone, which, in turn, is found to be very sensitive to various model characteristics and initial conditions. Numerical simulations of this case study using the hydrostatic BOLAM and the non-hydrostatic MOLOCH models are performed in order to test the effects of different formulations of the boundary layer parameterization: a modified version of the Louis (order 1) model and a custom version of the E-ℓ (order 1.5) model. Both of them require a diagnostic formulation of the mixing length, but the use of the turbulent kinetic energy equation in the E-ℓ model allows to represent turbulence history and non-locality effects and to formulate a more physically based mixing length. The impact of the two schemes is different in the two models. The hydrostatic model, run at 1/5 degree resolution, is less sensitive, but the quantitative precipitation forecast is in any case unsatisfactory in terms of localization and amount. Conversely, the non-hydrostatic model, run at 1/50 degree resolution, is capable of realistically simulate timing, position and amount of precipitation, with the apparently superior results obtained with the E-ℓ parameterization model.


Tellus B ◽  
2021 ◽  
Vol 73 (1) ◽  
pp. 1-26
Author(s):  
Piotr Sekuła ◽  
Anita Bokwa ◽  
Zbigniew Ustrnul ◽  
Mirosław Zimnoch ◽  
Bogdan Bochenek

2008 ◽  
Vol 21 (1) ◽  
pp. 22-39 ◽  
Author(s):  
Siegfried D. Schubert ◽  
Yehui Chang ◽  
Max J. Suarez ◽  
Philip J. Pegion

Abstract In this study the authors examine the impact of El Niño–Southern Oscillation (ENSO) on precipitation events over the continental United States using 49 winters (1949/50–1997/98) of daily precipitation observations and NCEP–NCAR reanalyses. The results are compared with those from an ensemble of nine atmospheric general circulation model (AGCM) simulations forced with observed SST for the same time period. Empirical orthogonal functions (EOFs) of the daily precipitation fields together with compositing techniques are used to identify and characterize the weather systems that dominate the winter precipitation variability. The time series of the principal components (PCs) associated with the leading EOFs are analyzed using generalized extreme value (GEV) distributions to quantify the impact of ENSO on the intensity of extreme precipitation events. The six leading EOFs of the observations are associated with major winter storm systems and account for more than 50% of the daily precipitation variability along the West Coast and over much of the eastern part of the country. Two of the leading EOFs (designated GC for Gulf Coast and EC for East Coast) together represent cyclones that develop in the Gulf of Mexico and occasionally move and/or redevelop along the East Coast producing large amounts of precipitation over much of the southern and eastern United States. Three of the leading EOFs represent storms that hit different sections of the West Coast (designated SW for Southwest coast, WC for the central West Coast, and NW for northwest coast), while another represents storms that affect the Midwest (designated by MW). The winter maxima of several of the leading PCs are significantly impacted by ENSO such that extreme GC, EC, and SW storms that occur on average only once every 20 years (20-yr storms) would occur on average in half that time under sustained El Niño conditions. In contrast, under La Niña conditions, 20-yr GC and EC storms would occur on average about once in 30 years, while there is little impact of La Niña on the intensity of the SW storms. The leading EOFs from the model simulations and their connections to ENSO are for the most part quite realistic. The model, in particular, does very well in simulating the impact of ENSO on the intensity of EC and GC storms. The main model discrepancies are the lack of SW storms and an overall underestimate of the daily precipitation variance.


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