Model Accumulation Mode of Atmospheric Aerosol Including Photochemical Aerosol Formation, Coagulation, Dynamics of the Atmospheric Boundary Layer and Relative Humidity

Author(s):  
P. Koutsenogii
2011 ◽  
Vol 11 (12) ◽  
pp. 5591-5601 ◽  
Author(s):  
J. Lauros ◽  
A. Sogachev ◽  
S. Smolander ◽  
H. Vuollekoski ◽  
S.-L. Sihto ◽  
...  

Abstract. We carried out column model simulations to study particle fluxes and deposition and to evaluate different particle formation mechanisms at a boreal forest site in Finland. We show that kinetic nucleation of sulphuric acid cannot be responsible for new particle formation alone as the simulated vertical profile of particle number concentration does not correspond to observations. Instead organic induced nucleation leads to good agreement confirming the relevance of the aerosol formation mechanism including organic compounds emitted by the biosphere. The simulation of aerosol concentration within the atmospheric boundary layer during nucleation event days shows a highly dynamical picture, where particle formation is coupled with chemistry and turbulent transport. We have demonstrated the suitability of our turbulent mixing scheme in reproducing the most important characteristics of particle dynamics within the boundary layer. Deposition and particle flux simulations show that deposition affects noticeably only the smallest particles in the lowest part of the atmospheric boundary layer.


2008 ◽  
Vol 3 (Special Issue No. 1) ◽  
pp. S89-S94 ◽  
Author(s):  
A. Kleidon

The hydrologic cycle is a system far from thermodynamic equilibrium that is characterized by its rate of entropy production in the climatological mean steady state. Over land, the hydrologic cycle is strongly affected by the presence of terrestrial vegetation. In order to investigate the role of the biota in the hydrologic cycle, it is critical to investigate the consequences of biotic effects from this thermodynamic perspective. Here I quantify entropy production by evapotranspiration with a climate system model of intermediate complexity and estimate its sensitivity to vegetation cover. For present-day conditions, the global mean entropy production of evaporation is 8.4 mW/m<sup>2</sup>/K, which is about 1/3 of the estimated entropy production of the whole hydrologic cycle. On average, ocean surfaces generally produce more than twice as much entropy as land surfaces. On land, high rates of entropy production of up to 16 mW/m<sup>2</sup>/K are found in regions of high evapotranspiration, although relative humidity of the atmospheric boundary layer is also an important factor. With an additional model simulation of a “Desert” simulation, where the effects of vegetation on land surface functioning is removed, I estimate the sensitivity of these entropy production rates to the presence of vegetation. Land averaged evapotranspiration decreases from 2.4 to 1.4 mm/d, while entropy production is reduced comparatively less from 4.2 to 3.1 mW/m<sup>2</sup>/K. This is related to the reduction in relative humidity of the atmospheric boundary layer as a compensatory effect, and points out the importance of a more complete treatment of entropy production calculations to investigate the role of biotic effects on Earth system functioning.


2021 ◽  
Vol 21 (15) ◽  
pp. 12091-12111
Author(s):  
Rebecca D. Kutzner ◽  
Juan Cuesta ◽  
Pascale Chelin ◽  
Jean-Eudes Petit ◽  
Mokhtar Ray ◽  
...  

Abstract. Ammonia (NH3) is a key precursor for the formation of atmospheric secondary inorganic particles, such as ammonium nitrate and sulfate. Although the chemical processes associated with the gas-to-particle conversion are well known, atmospheric concentrations of gaseous ammonia are still scarcely characterized. However, this information is critical, especially for processes concerning the equilibrium between ammonia and ammonium nitrate, due to the semivolatile character of the latter. This study presents an analysis of the diurnal cycle of atmospheric ammonia during a pollution event over the Paris megacity region in spring 2012 (5 d in late March 2012). Our objective is to analyze the link between the diurnal evolution of surface NH3 concentrations and its integrated column abundance, meteorological variables and relevant chemical species involved in gas–particle partitioning. For this, we implement an original approach based on the combined use of surface and total column ammonia measurements. These last ones are derived from ground-based remote sensing measurements performed by the Observations of the Atmosphere by Solar Infrared Spectroscopy (OASIS) Fourier transform infrared observatory at an urban site over the southeastern suburbs of the Paris megacity. This analysis considers the following meteorological variables and processes relevant to the ammonia pollution event: temperature, relative humidity, wind speed and direction, and the atmospheric boundary layer height (as indicator of vertical dilution during its diurnal development). Moreover, we study the partitioning between ammonia and ammonium particles from concomitant measurements of total particulate matter (PM) and ammonium (NH4+) concentrations at the surface. We identify the origin of the pollution event as local emissions at the beginning of the analyzed period and advection of pollution from Benelux and western Germany by the end. Our results show a clearly different diurnal behavior of atmospheric ammonia concentrations at the surface and those vertically integrated over the total atmospheric column. Surface concentrations remain relatively stable during the day, while total column abundances show a minimum value in the morning and rise steadily to reach a relative maximum in the late afternoon during each day of the spring pollution event. These differences are mainly explained by vertical mixing within the boundary layer, provided that this last one is considered well mixed and therefore homogeneous in ammonia concentrations. This is suggested by ground-based measurements of vertical profiles of aerosol backscatter, used as tracer of the vertical distribution of pollutants in the atmospheric boundary layer. Indeed, the afternoon enhancement of ammonia clearly seen by OASIS for the whole atmospheric column is barely depicted by surface concentrations, as the surface concentrations are strongly affected by vertical dilution within the rising boundary layer. Moreover, the concomitant occurrence of a decrease in ammonium particle concentrations and an increase in gaseous ammonia abundance suggests the volatilization of particles for forming ammonia. Furthermore, surface observations may also suggest nighttime formation of ammonium particles from gas-to-particle conversion, for relative humidity levels higher than the deliquescence point of ammonium nitrate.


2005 ◽  
Vol 5 (12) ◽  
pp. 3345-3356 ◽  
Author(s):  
S. Hyvönen ◽  
H. Junninen ◽  
L. Laakso ◽  
M. Dal Maso ◽  
T. Grönholm ◽  
...  

Abstract. Atmospheric aerosol particle formation is frequently observed throughout the atmosphere, but despite various attempts of explanation, the processes behind it remain unclear. In this study data mining techniques were used to find the key parameters needed for atmospheric aerosol particle formation to occur. A dataset of 8 years of 80 variables collected at the boreal forest station (SMEAR II) in Southern Finland was used, incorporating variables such as radiation, humidity, SO2, ozone and present aerosol surface area. This data was analyzed using clustering and classification methods. The aim of this approach was to gain new parameters independent of any subjective interpretation. This resulted in two key parameters, relative humidity and preexisting aerosol particle surface (condensation sink), capable in explaining 88% of the nucleation events. The inclusion of any further parameters did not improve the results notably. Using these two variables it was possible to derive a nucleation probability function. Interestingly, the two most important variables are related to mechanisms that prevent the nucleation from starting and particles from growing, while parameters related to initiation of particle formation seemed to be less important. Nucleation occurs only with low relative humidity and condensation sink values. One possible explanation for the effect of high water content is that it prevents biogenic hydrocarbon ozonolysis reactions from producing sufficient amounts of low volatility compounds, which might be able to nucleate. Unfortunately the most important biogenic hydrocarbon compound emissions were not available for this study. Another effect of water vapour may be due to its linkage to cloudiness which may prevent the formation of nucleating and/or condensing vapours. A high number of preexisting particles will act as a sink for condensable vapours that otherwise would have been able to form sufficient supersaturation and initiate the nucleation process.


2015 ◽  
Vol 8 (3) ◽  
pp. 453-471 ◽  
Author(s):  
R. H. H. Janssen ◽  
A. Pozzer

Abstract. We present a new submodel for the Modular Earth Submodel System (MESSy): the MiXed Layer (MXL) model for the diurnal dynamics of the convective boundary layer, including explicit representations of entrainment and surface fluxes. This submodel is embedded in a new MESSy base model (VERTICO), which represents a single atmospheric column. With the implementation of MXL in MESSy, MXL can be used in combination with other MESSy submodels that represent processes related to atmospheric chemistry. For instance, the coupling of MXL with more advanced modules for gas-phase chemistry (such as the Mainz Isoprene Mechanism 2 (MIM2)), emissions, dry deposition and organic aerosol formation than in previous versions of the MXL code is possible. Since MXL is now integrated in the MESSy framework, it can take advantage of future developments of this framework, such as the inclusion of new process submodels. The coupling of MXL with submodels that represent other processes relevant to chemistry in the atmospheric boundary layer (ABL) yields a computationally inexpensive tool that is ideally suited for the analysis of field data, for evaluating new parametrizations for 3-D models, and for performing systematic sensitivity analyses. A case study for the DOMINO campaign in southern Spain is shown to demonstrate the use and performance of MXL/MESSy in reproducing and analysing field observations.


2010 ◽  
Vol 10 (8) ◽  
pp. 20005-20033
Author(s):  
J. Lauros ◽  
A. Sogachev ◽  
S. Smolander ◽  
H. Vuollekoski ◽  
S.-L. Sihto ◽  
...  

Abstract. We carried out column model simulations to study particle fluxes and deposition and to evaluate different particle formation mechanisms at a boreal forest site in Finland. We show that kinetic nucleation of sulphuric acid cannot be responsible for new particle formation alone as the vertical profile of particle number distribution does not correspond to observations. Instead organic induced nucleation leads to good agreement confirming the relevance of the aerosol formation mechanism including organic compounds emitted by biosphere. Simulation of aerosol concentration inside the atmospheric boundary layer during nucleation days shows highly dynamical picture, where particle formation is coupled with chemistry and turbulent transport. We have demonstrated suitability of our turbulent mixing scheme in reproducing most important characteristics of particle dynamics inside the atmospheric boundary layer. Deposition and particle flux simulations show that deposition affects noticeably only the smallest particles at the lowest part of the atmospheric boundary layer.


2021 ◽  
Vol 38 (1) ◽  
pp. 47-61
Author(s):  
Temple R. Lee ◽  
Sandip Pal

AbstractRawinsonde observations have long been used to estimate the atmospheric boundary layer depth (BLD), which is an important parameter for monitoring air quality, dispersion studies, weather forecast models, and inversion systems for estimating regional surface–atmosphere fluxes of tracers. Although many approaches exist for deriving the BLDs from rawinsonde observations, the bulk Richardson approach has been found to be most appropriate. However, the impact of errors in the measured thermodynamic and kinematic fields on the estimated BLDs remains unexplored. We argue that quantifying BLD error (δBLD) estimates is equally as important as the BLDs themselves. Here we quantified δBLD by applying the bulk Richardson method to 35 years of rawinsonde data obtained from three stations in the United States: Sterling, Virginia; Amarillo, Texas; and Salt Lake City, Utah. Results revealed similar features in terms of their respective errors. A −2°C bias in temperature yielded a mean δBLD ranging from −15 to 200 m. A +2°C bias in temperature yielded a mean δBLD ranging from −214 to +18 m. For a −5% relative humidity bias, the mean δBLD ranged from −302 to +7 m. For a +5% relative humidity bias, the mean δBLD ranged from +2 to +249 m. Differences of ±2 m s−1 in the winds yielded BLD errors of ~±300 m. The δBLD increased as a function of BLD when introducing errors to the thermodynamic fields and decreased as a function of BLD when introducing errors to the kinematic fields. These findings expand upon previous work evaluating rawinsonde-derived δBLD by quantifying δBLD arising from rawinsonde-derived thermodynamic and kinematic measurements. Knowledge of δBLD is critical in, for example, intercomparison studies where rawinsonde-derived BLDs are used as references.


Atmosphere ◽  
2020 ◽  
Vol 11 (11) ◽  
pp. 1142
Author(s):  
Kyung-Hwan Kwak ◽  
Seung-Hyeop Lee ◽  
A-Young Kim ◽  
Kwon-Chan Park ◽  
Sang-Eun Lee ◽  
...  

A 307-m tall meteorological tower was used to evaluate meteorological observation data obtained using a rotary-wing unmanned aerial vehicle (UAV). A comparative study between the tower and UAV observations was conducted during the daytime (06:00 to 19:00 local time (LT)) in the summer of 2017 (16–18th August). Hourly vertical profiles of air temperature, relative humidity, black carbon (BC), and ozone (O3) concentrations were obtained for up to 300 m height. Statistical metrics for evaluating the accuracy of UAV observations against the tower observation showed positive (potential temperature) and negative (relative humidity) biases, which were within acceptable ranges. The daytime evolution of the lower atmospheric boundary layer (ABL) was successfully captured by the hourly UAV observations. During the early morning, a large vertical slope of potential temperature was observed between 100 and 140 m, corresponding to the stable ABL height. The large vertical slope coincided with the large differences in BC and O3 concentrations between altitudes below and above the height. The transition from stable to convective ABL was observed at 10–11 LT, indicated by the ABL height higher than 300 m in the convective ABL. Finally, we provide several recommendations to reduce uncertainties of UAV observation.


2020 ◽  
Author(s):  
Rebecca D. Kutzner ◽  
Juan Cuesta ◽  
Pascale Chelin ◽  
Jean-Eudes Petit ◽  
Mokhtar Ray ◽  
...  

Abstract. Ammonia (NH3) is a key precursor for the formation of atmospheric secondary inorganic particles, such as ammonium nitrate and sulfate. Although the chemical processes associated with the gas-to-particle conversion are well known, atmospheric concentrations of gaseous ammonia are still scarcely characterized. This information is however critical especially for processes concerning the equilibrium between ammonia and ammonium nitrate, due to the semi-volatile character of the latter one. This study presents an analysis of the diurnal cycle of atmospheric ammonia during a pollution event over the Paris megacity region in spring 2012 (five days in late March 2012). Our objective is to analyze the link between the diurnal evolution of surface NH3 concentrations and its integrated column abundance, meteorological variables and relevant chemical species involved in gas/particle partitioning. For this, we implement an original approach based on the combined use of surface and total column ammonia measurements. These last ones are derived from ground-based remote-sensing measurements performed by the Observations of the Atmosphere by Solar Infrared Spectroscopy (OASIS) Fourier transform infrared observatory at an urban site over the southeastern suburbs of the Paris megacity. This analysis considers the following meteorological variables relevant to the ammonia pollution event: temperature, relative humidity, wind speed and direction and vertical dilution in the atmospheric boundary layer. Moreover, we study the partitioning between ammonia and ammonium particles from concomitant measurements of total particulate matter (PM) and ammonium (NH4+) concentrations at the surface. We identify the origin of the pollution event as local emissions at the beginning of the analyzed period and advection of pollution from the Benelux and west Germany region by the end. Our results show a clearly different diurnal behavior of atmospheric ammonia concentrations at the surface and those vertically integrated over the total atmospheric column. Surface concentrations remain relatively stable during the day, while total column abundances show a minimum value in the morning and rise steadily to reach a relative maximum in the late afternoon during the spring pollution event. These differences are mainly explained by vertical mixing within the boundary layer, as suggested by ground-based measurements of vertical profiles of aerosol backscatter, used as tracer of the vertical distribution of pollutants in the atmospheric boundary layer. Indeed, the afternoon enhancement of ammonia clearly seen by OASIS for the whole atmospheric column is barely depicted by surface concentrations, as the latter are strongly affected by vertical dilution within the rising boundary layer. Moreover, the concomitant occurrence of a decrease of ammonium particle concentrations and an increase of gaseous ammonia abundance suggests the volatilization of particles for forming ammonia. Furthermore, surface observations may also suggest night-time formation of ammonium particles from gas-to-particle conversion, for relative humidity levels higher than the deliquescence point of ammonium nitrate.


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