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Search Results: 1 - 10 of 297563 matches for " J. Kazil "
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A semi-analytical method for calculating rates of new sulfate aerosol formation from the gas phase
J. Kazil,E. R. Lovejoy
Atmospheric Chemistry and Physics (ACP) & Discussions (ACPD) , 2007,
Abstract: The formation of new aerosol from the gas phase is commonly represented in atmospheric modeling with parameterizations of the steady state nucleation rate. Present parameterizations are based on classical nucleation theory or on nucleation rates calculated with a numerical aerosol model. These parameterizations reproduce aerosol nucleation rates calculated with a numerical aerosol model only imprecisely. Additional errors can arise when the nucleation rate is used as a surrogate for the production rate of particles of a given size. We discuss these errors and present a method which allows a more precise calculation of steady state sulfate aerosol formation rates. The method is based on the semi-analytical solution of an aerosol system in steady state and on parameterized rate coefficients for H2SO4 uptake and loss by sulfate aerosol particles, calculated from laboratory and theoretical thermodynamic data.
A semi-analytical method for calculating rates of new sulfate aerosol formation from the gas phase
J. Kazil,E. R. Lovejoy
Atmospheric Chemistry and Physics Discussions , 2007,
Abstract: The formation of new sulfate aerosol from the gas phase is commonly represented in atmospheric modeling with parameterizations of the steady state nucleation rate. Such parameterizations are based on classical nucleation theory or on aerosol nucleation rate tables, calculated with a numerical aerosol model. These parameterizations reproduce aerosol nucleation rates calculated with a numerical aerosol model only imprecisely. Additional errors can arise when the nucleation rate is used as a surrogate for the production rate of particles of a given size. We discuss these errors and present a method which allows a more precise calculation of steady state sulfate aerosol formation rates. The method is based on the semi-analytical solution of an aerosol system in steady state and on parameterized rate coefficients for H2SO4 uptake and loss by sulfate aerosol particles, calculated from laboratory and theoretical thermodynamic data.
Numerical issues associated with compensating and competing processes in climate models: an example from ECHAM-HAM
H. Wan,P. J. Rasch,K. Zhang,J. Kazil
Geoscientific Model Development Discussions , 2013, DOI: 10.5194/gmdd-6-685-2013
Abstract: The purpose of this paper is to draw attention to the need for appropriate numerical techniques to represent process interactions in climate models. In two versions of the ECHAM-HAM model, different time integration methods are used to solve the sulfuric acid (H2SO4) gas evolution equation, which lead to substantially different results in the H2SO4 gas concentration and the aerosol nucleation rate. Using convergence tests and sensitivity simulations performed with various time stepping schemes, it is confirmed that numerical errors in the second model version are significantly smaller than those in version one. The use of sequential operator splitting in combination with long time step is identified as the main reason for the large systematic biases in the old model. The remaining errors of nucleation rate in version two, related to the competition between condensation and nucleation, have a clear impact on the simulated concentration of cloud condensation nuclei (CCN) in the lower troposphere. These errors can be significantly reduced by employing an implicit solver that handles production, condensation and nucleation at the same time. Lessons learned in this work underline the need for more caution when treating multi-time-scale problems involving compensating and competing processes, a common occurrence in current climate models.
Modelling microphysical and meteorological controls on precipitation and cloud cellular structures in Southeast Pacific stratocumulus
H. Wang, G. Feingold, R. Wood,J. Kazil
Atmospheric Chemistry and Physics (ACP) & Discussions (ACPD) , 2010,
Abstract: Microphysical and meteorological controls on the formation of open and closed cellular structures in the Southeast Pacific are explored using model simulations based on aircraft observations during the VAMOS Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx). The effectiveness of factors such as boundary-layer moisture and temperature perturbations, surface heat and moisture fluxes, large-scale vertical motion and solar heating in promoting drizzle and open cell formation for prescribed aerosol number concentrations is explored. For the case considered, drizzle and subsequent open cell formation over a broad region are more sensitive to the observed boundary-layer moisture and temperature perturbations (+0.9 g kg 1; 1 K) than to a five-fold decrease in aerosol number concentration (150 vs. 30 mg 1). When embedding the perturbations in closed cells, local drizzle and pockets of open cell (POC) formation respond faster to the aerosol reduction than to the moisture increase, but the latter generates stronger and more persistent drizzle. A local negative perturbation in temperature drives a mesoscale circulation that prevents local drizzle formation but promotes it in a remote area where lower-level horizontal transport of moisture is blocked and converges to enhance liquid water path. This represents a potential mechanism for POC formation in the Southeast Pacific stratocumulus region whereby the circulation is triggered by strong precipitation in adjacent broad regions of open cells. A simulation that attempts to mimic the influence of a coastally induced upsidence wave results in an increase in cloud water but this alone is insufficient to initiate drizzle. An increase of surface sensible heat flux is also effective in triggering local drizzle and POC formation. Both open and closed cells simulated with observed initial conditions exhibit distinct diurnal variations in cloud properties. A stratocumulus deck that breaks up due solely to solar heating can recover at night. Precipitation in the open-cell cases depletes the aerosol to the extent that cloud formation is significantly suppressed within one diurnal cycle. A replenishment rate of cloud condensation nuclei of order 1 mg 1 h 1 is sufficient to maintain clouds and prevent the boundary layer from collapsing the following day, suggesting that some local and/or remote aerosol sources is necessary for POCs to be able to last for days.
Aerosol microphysics modules in the framework of the ECHAM5 climate model – intercomparison under stratospheric conditions
H. Kokkola,R. Hommel,J. Kazil,U. Niemeier
Geoscientific Model Development Discussions , 2009,
Abstract: In this manuscript, we present an intercomparison of three different aerosol microphysics modules that are implemented in the climate model ECHAM5. The comparison was done between the modal aerosol microphysics module M7, which is currently the default aerosol microphysical core in ECHAM5, and two sectional aerosol microphysics modules SALSA, and SAM2. A detailed aerosol microphycical model MAIA was used as a reference model to evaluate the results of the aerosol microphysics modules with respect to sulphate aerosol. The ability of the modules to describe the development of the aerosol size distribution was tested in a zero dimensional framework. We evaluated the strengths and weaknesses of different approaches under different types of stratospheric conditions. Also, we present an improved method for the time integration in M7 and study how the setup of the modal approach affects the evolution of the aerosol size distribution. Intercomparison simulations were carried out with varying SO2 concentrations from background conditions to extreme values arising from stratospheric injections of large volcanic eruptions. Under background conditions, all microphysics modules were in good agreement describing the shape of the size distribution but the scatter between the model results increased with increasing SO2 concentrations. In particular for the volcanic case the module setups have to be redefined to be applied in global model simulations capturing respective sulphate particle formation events. Summarized, this intercomparison serves as a review on the different aerosol microphysics modules which are currently available for the climate model ECHAM5.
In situ observations of new particle formation in the tropical upper troposphere: the role of clouds and the nucleation mechanism
R. Weigel,S. Borrmann,J. Kazil,A. Minikin
Atmospheric Chemistry and Physics (ACP) & Discussions (ACPD) , 2011, DOI: 10.5194/acp-11-9983-2011
Abstract: New particle formation (NPF), which generates nucleation mode aerosol, was observed in the tropical Upper Troposphere (UT) and Tropical Tropopause Layer (TTL) by in situ airborne measurements over South America (January–March 2005), Australia (November–December 2005), West Africa (August 2006) and Central America (2004–2007). Particularly intense NPF was found at the bottom of the TTL. Measurements with a set of condensation particle counters (CPCs) with different dp50 (50% lower size detection efficiency diameter or "cut-off diameter") were conducted on board the M-55 Geophysica in the altitude range of 12.0–20.5 km and on board the DLR Falcon-20 at up to 11.5 km altitude. On board the NASA WB-57F size distributions were measured over Central America in the 4 to 1000 nm diameter range with a system of nucleation mode aerosol spectrometers. Nucleation mode particle concentrations (NNM) were derived from these measurements which allow for identifying many NPF events with NNM in the range of thousands of particles per cm3. Over Australia and West Africa, we identified NPF in the outflow of tropical convection, in particular of a Mesoscale Convective System (MCS). Newly formed particles with NNM > 1000 cm 3 were found to coexist with ice cloud particles (dp > 2 μm) as long as cloud particle concentrations remained below 2 cm 3. The occurrence of NPF within the upper troposphere and the TTL was generally confined within 340 K to 380 K potential temperature, but NPF was of particular strength between 350 K and 370 K (i.e. ~1–4 km below the cold point tropopause). Analyses of the aerosol volatility (at 250 °C) show that in the TTL on average 75–90% of the particles were volatile, compared to typically only 50% in the extra-tropical UT, indicative for the particles to mainly consist of H2SO4-H2O and possibly organic compounds. Along two flight segments over Central and South America (24 February 2005 and 7 August 2006, at 12.5 km altitude) in cloud free air, above thin cirrus, particularly high NNM were observed. Recent lifting had influenced the probed air masses, and NNM reached up to 16 000 particles cm 3 (ambient concentration). A sensitivity study using an aerosol model, which includes neutral and ion induced nucleation processes, simulates NNM in reasonable agreement with the in situ observations of clear-air NPF. Based on new, stringent multi-CPC criteria, our measurements corroborate the hypothesis that the tropical UT and the TTL are regions supplying freshly nucleated particles. Our findings narrow the altitude of the main source region to the bottom
The global aerosol-climate model ECHAM-HAM, version 2: sensitivity to improvements in process representations
K. Zhang,D. O'Donnell,J. Kazil,P. Stier
Atmospheric Chemistry and Physics (ACP) & Discussions (ACPD) , 2012, DOI: 10.5194/acp-12-8911-2012
Abstract: This paper introduces and evaluates the second version of the global aerosol-climate model ECHAM-HAM. Major changes have been brought into the model, including new parameterizations for aerosol nucleation and water uptake, an explicit treatment of secondary organic aerosols, modified emission calculations for sea salt and mineral dust, the coupling of aerosol microphysics to a two-moment stratiform cloud microphysics scheme, and alternative wet scavenging parameterizations. These revisions extend the model's capability to represent details of the aerosol lifecycle and its interaction with climate. Nudged simulations of the year 2000 are carried out to compare the aerosol properties and global distribution in HAM1 and HAM2, and to evaluate them against various observations. Sensitivity experiments are performed to help identify the impact of each individual update in model formulation. Results indicate that from HAM1 to HAM2 there is a marked weakening of aerosol water uptake in the lower troposphere, reducing the total aerosol water burden from 75 Tg to 51 Tg. The main reason is the newly introduced κ-K hler-theory-based water uptake scheme uses a lower value for the maximum relative humidity cutoff. Particulate organic matter loading in HAM2 is considerably higher in the upper troposphere, because the explicit treatment of secondary organic aerosols allows highly volatile oxidation products of the precursors to be vertically transported to regions of very low temperature and to form aerosols there. Sulfate, black carbon, particulate organic matter and mineral dust in HAM2 have longer lifetimes than in HAM1 because of weaker in-cloud scavenging, which is in turn related to lower autoconversion efficiency in the newly introduced two-moment cloud microphysics scheme. Modification in the sea salt emission scheme causes a significant increase in the ratio (from 1.6 to 7.7) between accumulation mode and coarse mode emission fluxes of aerosol number concentration. This leads to a general increase in the number concentration of smaller particles over the oceans in HAM2, as reflected by the higher ngstr m parameters. Evaluation against observation reveals that in terms of model performance, main improvements in HAM2 include a marked decrease of the systematic negative bias in the absorption aerosol optical depth, as well as smaller biases over the oceans in ngstr m parameter and in the accumulation mode number concentration. The simulated geographical distribution of aerosol optical depth (AOD) is better correlated with the MODIS data, while the surface aeros
Modelling microphysical and meteorological controls on precipitation and cloud cellular structures in Southeast Pacific stratocumulus
H. Wang,G. Feingold,R. Wood,J. Kazil
Atmospheric Chemistry and Physics (ACP) & Discussions (ACPD) , 2010, DOI: 10.5194/acp-10-6347-2010
Abstract: Microphysical and meteorological controls on the formation of open and closed cellular structures in the Southeast Pacific are explored using model simulations based on aircraft observations during the VAMOS Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx). The effectiveness of factors such as boundary-layer moisture and temperature perturbations, surface heat and moisture fluxes, large-scale vertical motion and solar heating in promoting drizzle and open cell formation for prescribed aerosol number concentrations is explored. For the case considered, drizzle and subsequent open cell formation over a broad region are more sensitive to the observed boundary-layer moisture and temperature perturbations (+0.9 g kg 1; 1 K) than to a five-fold decrease in aerosol number concentration (150 vs. 30 mg 1). When embedding the perturbations in closed cells, local drizzle and pockets of open cell (POC) formation respond faster to the aerosol reduction than to the moisture increase, but the latter generates stronger and more persistent drizzle. A local negative perturbation in temperature drives a mesoscale circulation that prevents local drizzle formation but promotes it in a remote area where lower-level horizontal transport of moisture is blocked and converges to enhance liquid water path. This represents a potential mechanism for POC formation in the Southeast Pacific stratocumulus region whereby the circulation is triggered by strong precipitation in adjacent broad regions of open cells. A simulation that attempts to mimic the influence of a coastally induced upsidence wave results in an increase in cloud water but this alone is insufficient to initiate drizzle. An increase of surface sensible heat flux is also effective in triggering local drizzle and POC formation. Both open and closed cells simulated with observed initial conditions exhibit distinct diurnal variations in cloud properties. A stratocumulus deck that breaks up due solely to solar heating can recover at night. Precipitation in the open-cell cases depletes the aerosol to the extent that cloud formation is significantly suppressed within one diurnal cycle. A replenishment rate of cloud condensation nuclei of order 1 mg 1 h 1 is sufficient to maintain clouds and prevent the boundary layer from collapsing the following day, suggesting that some local and/or remote aerosol sources is necessary for POCs to be able to last for days.
Modeling chemical and aerosol processes in the transition from closed to open cells during VOCALS-REx
J. Kazil, H. Wang, G. Feingold, A. D. Clarke, J. R. Snider,A. R. Bandy
Atmospheric Chemistry and Physics (ACP) & Discussions (ACPD) , 2011,
Abstract: Chemical and aerosol processes in the transition from closed- to open-cell circulation in the remote, cloudy marine boundary layer are explored. It has previously been shown that precipitation can initiate a transition from the closed- to the open-cellular state, but that the boundary layer cannot maintain this open-cell state without a resupply of cloud condensation nuclei (CCN). Potential sources of CCN include wind-driven production of sea salt from the ocean, nucleation from the gas phase, and entrainment from the free troposphere. In order to investigate CCN sources in the marine boundary layer and their role in supplying new particles, we have coupled in detail chemical, aerosol, and cloud processes in the WRF/Chem model, and added state-of-the-art representations of sea salt emissions and aerosol nucleation. We conduct numerical simulations of the marine boundary layer in the transition from a closed- to an open-cell state. Results are compared with observations in the Southeast Pacific boundary layer during the VAMOS Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx). The transition from the closed- to the open-cell state generates conditions that are conducive to nucleation by forming a cloud-scavenged, ultra-clean layer below the inversion base. Open cell updrafts loft dimethyl sulfide from the ocean surface into the ultra-clean layer, where it is oxidized during daytime to SO2 and subsequently to H2SO4. Low H2SO4 condensation sink values in the ultra-clean layer allow H2SO4 to rise to concentrations at which aerosol nucleation produces new aerosol in significant numbers. The existence of the ultra-clean layer is confirmed by observations. We find that the observed DMS flux from the ocean in the VOCALS-REx region can support a nucleation source of aerosol in open cells that exceeds sea salt emissions in terms of the number of particles produced. The freshly nucleated, nanometer-sized aerosol particles need, however, time to grow to sizes large enough to act as CCN. In contrast, mechanical production of particles from the ocean surface by near-surface winds provides a steady source of larger particles that are effective CCN at a rate exceeding a threshold for maintenance of open-cell circulation. Entrainment of aerosol from the free troposphere contributes significantly to boundary layer aerosol for the considered VOCALS-REx case, but less than sea salt aerosol emissions.
Aerosol microphysics modules in the framework of the ECHAM5 climate model – intercomparison under stratospheric conditions
H. Kokkola, R. Hommel, J. Kazil, U. Niemeier, A.-I. Partanen, J. Feichter,C. Timmreck
Geoscientific Model Development (GMD) & Discussions (GMDD) , 2009, DOI: 10.5194/gmd-2-97-2009
Abstract: In this manuscript, we present an intercomparison of three different aerosol microphysics modules that are implemented in the climate model ECHAM5. The comparison was done between the modal aerosol microphysics module M7, which is currently the default aerosol microphysical core in ECHAM5, and two sectional aerosol microphysics modules SALSA, and SAM2. The detailed aerosol microphysical model MAIA was used as a reference to evaluate the results of the aerosol microphysics modules with respect to sulphate aerosol. The ability of the modules to describe the development of the aerosol size distribution was tested in a zero dimensional framework. We evaluated the strengths and weaknesses of different approaches under different types of stratospheric conditions. Also, we present an improved method for the time integration in M7 and study how the setup of the modal aerosol modules affects the evolution of the aerosol size distribution. Intercomparison simulations were carried out with varying SO2 concentrations from background conditions to extreme values arising from stratospheric injections by large volcanic eruptions. Under background conditions, all microphysics modules were in good agreement describing the shape of the aerosol size distribution, but the scatter between the model results increased with increasing SO2 concentrations. In particular in the volcanic case the setups of the aerosol modules have to be adapted in order to dependably capture the evolution of the aerosol size distribution, and to perform in global model simulations. In summary, this intercomparison serves as a review of the different aerosol microphysics modules which are currently available for the climate model ECHAM5.
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