-
A double-moment bulk microphysics scheme for modelling cirrus clouds including explicit impact of aerosols on different types of nucleation mechanism is described. Process rates are formulated in terms of generalised moments of the underlying a priori size distributions in order to allow simple switching between various distribution types. The scheme has been implemented into a simple box model and into the anelastic non-hydrostatic model EULAG. The new microphysics is validated against simulations with detailed microphysics for idealised process studies and for a well documented case of arctic cirrostratus. Additionally, the formation of ice crystals with realistic background aerosol concentration is modelled and the effect of ambient pressure on homogeneous nucleation is investigated in the box model. <br><br> The model stands all tests and is thus suitable for cloud-resolving simulations of cirrus clouds.
-
Studies of secondary aerosol-particle formation depend on identifying days in which new particle formation occurs and, by comparing them to days with no signs of particle formation, identifying the conditions favourable for formation. Continuous aerosol size distribution data has been collected at the SMEAR II station in a boreal forest in Hyytiälä, Finland, since 1996, making it the longest time series of aerosol size distributions available worldwide. In previous studies, the data have been classified as particle-formation event, nonevent, and undefined days, with almost 40% of the dataset classified as undefined. In the present study, eleven years (1996–2006) of undefined days (1630 days) were reanalyzed and subdivided into three new classes: failed events (37% of all previously undefined days), ultrafine-mode concentration peaks (34%), and pollution-related concentration peaks (19%). Unclassified days (10%) comprised the rest of the previously undefined days. The failed events were further subdivided into tail events (21%), where a tail of a formation event presumed to be advected to Hyytiälä from elsewhere, and quasi events (16%) where new particles appeared at sizes 3–10 nm, but showed unclear growth, the mode persisted for less than an hour, or both. The ultrafine concentration peaks days were further subdivided into nucleation-mode peaks (24%) and Aitken-mode peaks (10%), depending on the size range where the particles occurred. The mean annual distribution of the failed events has a maximum during summer, whereas the two peak classes have maxima during winter. The summer minimum previously found in the seasonal distribution of event days partially offsets a summer maximum in failed-event days. Daily-mean relative humidity and condensation sink values are useful in discriminating the new classes from each other. Specifically, event days had low values of relative humidity and condensation sink relative to nonevent days. Failed-event days possessed intermediate condensation sink and relative humidity values, whereas both ultrafine-mode peaks and, to a greater extent, pollution-related peaks had high values of both, similar to nonevent days. Using 96-h back trajectories, particle-size concentrations were plotted as a function of time the trajectory spent over land. Increases in particle size and number concentration during failed-event days were similar to that during the later stages of event days, whereas the particle size and number concentration for both nonevent and peaks classes did not increase as fast as for event and failed events days.
-
A recently developed and validated bulk microphysics scheme for modelling cirrus clouds (Spichtinger and Gierens, 2009), implemented into the anelastic non-hydrostatic model EULAG is used for investigation of the impact of dynamics on the evolution of an arctic cirrostratus. Sensitivity studies are performed, using variation of large-scale updraughts as well as addition of small-scale temperature fluctuations and wind shear. The results show the importance of sedimentation of ice crystals on cloud evolution. Due to non-linear processes like homogeneous nucleation situations can arise where small changes in the outer parameters have large effects on the resulting cloud structure. In-cloud ice supersaturation is a common feature of all our simulations, and we show that dynamics is as least as important for its appearance than is microphysics.
-
Detrended fluctuation analysis is applied to the time series of the global tropopause height derived from the 1980–2004 daily radiosonde data, in order to detect long-range correlations in its time evolution. <br><br> Global tropopause height fluctuations in small time-intervals are found to be positively correlated to those in larger time intervals in a power-law fashion. The exponent of this dependence is larger in the tropics than in the middle and high latitudes in both hemispheres. Greater persistence is observed in the tropopause of the Northern than in the Southern Hemisphere. A plausible physical explanation of the fact that long-range correlations in tropopause variability decreases with increasing latitude is that the column ozone fluctuations (that are closely related with the tropopause ones) exhibit long range correlations, which are larger in tropics than in the middle and high latitudes at long time scales. <br><br> This finding for the tropopause height variability should reduce the existing uncertainties in assessing the climatic characteristics. More specifically the reliably modelled values of a climatic variable (i.e. past and future simulations) must exhibit the same scaling behaviour with that possibly existing in the real observations of the variable under consideration. An effort has been made to this end by applying the detrended fluctuation analysis to the global mean monthly land and sea surface temperature anomalies during the period January 1850–August 2008. The result obtained supports the findings presented above, notably: the correlations between the fluctuations in the global mean monthly land and sea surface temperature display scaling behaviour which must characterizes any projection.
-
The eruption of Mt. Pinatubo in the Philippines in June 1991 was one of the strongest volcanic eruptions in the 20th century and this well observed eruption can serve as an important case study to understand the subsequent weather and climate changes. In this paper, the most comprehensive simulations to date of the climate impact of Mt. Pinatubo eruption are carried out with prescribed volcanic aerosols including observed SSTs, QBO and volcanically induced ozone anomalies. This is also the first attempt to include all the known factors for the simulation of such an experiment. Here, the climate response is evaluated under different boundary conditions including one at a time, thereby, investigating the radiative and dynamical responses to individual and combined forcings by observed SSTs, QBO and volcanic effects. Two ensembles of ten members each, for unperturbed and volcanically perturbed conditions were carried out using the middle atmosphere configuration of ECHAM5 general circulation model. Our results show that the simulated climate response that may arise solely from aerosol forcing in lower stratospheric temperature is insensitive to the boundary conditions in the tropics and does not show some observed features such as the temperature signature of the QBO phases. Also, statistically significant positive anomalies in the high latitudes in NH winter of 1991/92 seen in our model simulations with prescribed observed SST and QBO phases as boundary conditions are consistent with the observations. To simulate realistically the lower stratospheric temperature response, one must include all the known factors. The pure QBO and ocean signatures in lower stratospheric temperature are simulated consistently with earlier studies. The indirect effect of the volcanic aerosols manifested as the winter warming pattern is not simulated in the ensemble mean of the experiments. Our analysis also shows that the response to El Niño conditions is very strong in the model and that it partially masks the effects due to volcanic forcing.
-
2003 was a record year for wildfires worldwide. Severe forest fires killed four people, displaced 20 500 others and burnt 260 000 ha in South-East Australia in January 2003. The uncontrolled fires ignited in early January 2003 as a result of a prolonged El Niño drought in South-East Australia. Severe weather conditions resulted in a fast spread of the fires and poor air quality in a region where 70% of the population of Australia lives. We use state-of-art global chemistry and transport model GEOS-Chem in conjunction with ground- and space-based observations to study the ozone (O<sub>3</sub>) and aerosol enhancement due to fires. Firstly, the monthly mean surface O<sub>3</sub> and Aerosol Optical Depth (AOD) in January 2003 are compared to January 2004 and, secondly, from sensitivity model simulations, four episodes are isolated and an attempt is made to quantify the contribution of the fires to air quality in south and South-East Australia. <br><br> In January 2003 the observed monthly mean afternoon surface O<sub>3</sub> in Victoria (VIC) and South Australia (SA) reached 27.5 ppb, which is 6.5 ppb (i.e. 30%) higher than in 2004. The simulated O<sub>3</sub> is 29.5 ppb, which is 10 ppb higher than in 2004. While the model tends to overestimate the observed peak O<sub>3</sub>, it exhibits very good skill in reproducing the O<sub>3</sub> temporal variability in January 2003 with a correlation of 0.83. In VIC, the air quality 4-h ozone (O<sub>3</sub>) standard exceedences are reported on 17, 24 and 25 January. On 12, 17, 24–25 and 29 January 2003, the observed O<sub>3</sub> peaks above 40 ppb and the simulated fire contribution is higher than 10 ppb. During these 4 episodes, the range of observed O<sub>3</sub> enhancement due to fires is 20–35 ppb, which is a factor of 3 to 5 higher than the monthly mean. The simulated fire O<sub>3</sub> enhancement is in the range 15–50 ppb with a factor of 1.5 to 5 higher than the monthly mean. During two episodes, a well-formed surface wind channel stretches across the Tasman Sea facilitating the long range transport to New Zealand contributing to a 10% increase of surface O<sub>3</sub>. <br><br> During the four episodes in January 2003, the observed AOD was up to a factor of five higher that the monthly mean AOD. The simulated and observed AODs agree on the spatial structure. Despite the model tendency to underestimate the AOD, it proves a useful tool in reconstructing the mostly patchy observations.
-
Very dry high-ozone layers have been repeatedly observed with the ozone lidar in Garmisch-Partenkirchen (Germany) starting one or two days after the onset of high-pressure periods during the warm season. These episodes have been analysed by trajectory calculations and extended simulations with the FLEXPART particle dispersion model. Mixed contributions from the stratosphere over the Pacific Ocean and the boundary layers of East Asia and North America were found. The stratospheric influence is mostly dominating and caused by a rather shallow transfer from the stratosphere into these rapid upper- and mid-tropospheric air streams. The considerable vertical extent of these layers and peak ozone mixing ratios between 80 and 150 ppb suggest an important mechanism for stratosphere-to-troposphere transport.
-
Satellite retrievals of methane (CH<sub>4</sub>) using the Atmospheric Infrared Sounder (AIRS) on the EOS/Aqua platform from 2003–2007 show a strong, plume-like enhancement of CH<sub>4</sub> in the middle to upper troposphere over South Asia during July, August and September, with the maximum occurring in early September. Simulations using the global tracer model version 3 (TM3) also show similar seasonal enhancement of CH<sub>4</sub> in the same region. The model results also suggest that this enhancement is associated with transport processes and local surface emissions, thus the observations of tropospheric CH<sub>4</sub> during the monsoon season may be used to constrain the models for a better estimation of Asian CH<sub>4</sub> sources. Further comparisons between the AIRS retrievals and the model simulations suggest a possible overestimate of emissions from rice paddies in Southeast Asia in the scenario with the global emissions from rice of 60 Tg yr<sup>−1</sup>. Moreover, the observed tropospheric CH<sub>4</sub> enhancement from AIRS provides evidence for the strong transport of atmospheric pollutants from the lower to the upper troposphere in Asia during the monsoon season. The observed rapid disappearance of the local CH<sub>4</sub> maximum in September may provide valuable information for studying the dissipation of the Tibetan anticyclone and the withdrawal of monsoon.
-
This study investigates the droplet formation characteristics of secondary organic aerosol (SOA) formed during the ozonolysis of sesquiterpene β-caryophyllene (with and without hydroxyl radicals present). Emphasis is placed on understanding the role of semi-volatile material on Cloud Condensation Nucleus (CCN) activity and droplet growth kinetics. Aging of β-caryophyllene SOA significantly affects all CCN-relevant properties measured throughout the experiments. Using a thermodenuder and two CCN instruments, we find that CCN activity is a strong function of temperature (activation diameter at ~0.6% supersaturation: 100±10 nm at 20°C and 130±10 nm at 35°C), suggesting that the hygroscopic fraction of the SOA is volatile. The water-soluble organic carbon (WSOC) is extracted from the SOA and characterized with Köhler Theory Analysis (KTA); the results suggest that the WSOC is composed of low molecular weight (<200 g mol<sup>−1</sup>) slightly surface-active material that constitute 5–15% of the SOA mass. These properties are similar to the water-soluble fraction of monoterpene SOA, suggesting that predictive understanding of SOA CCN activity requires knowledge of the WSOC fraction but not its exact speciation. Droplet growth kinetics of the CCN are found to be strongly anticorrelated with WSOC fraction, suggesting that the insoluble material in the SOA forms a kinetic barrier that delays droplet growth. Overall, volatilization effects can increase activation diameters by 30%, and depress droplet growth rate by a factor of two; these results may have important implications for the droplet formation characteristics of SOA, and the atmospheric relevance of CCN measurements carried out at temperatures different from ambient.
-
Comparisons of cloud liquid water path (LWP) retrievals are presented from the Moderate Resolution Imaging Spectroradiometer (MODIS) and the Advanced Microwave Scanning Radiometer (AMSR-E) located aboard the Aqua spacecraft. LWP differences as a function of cloud top height, cloud fraction, cloud top temperature, LWP, cloud effective radius and cloud optical thickness are quantified in most geophysical conditions. The assumption of vertically homogeneous distributions of cloud water content in the MODIS LWP retrieval yields a slightly poorer agreement than the assumption of stratified cloud liquid water. Furthermore, for a fixed cloud top pressure, the cloud top temperature can lead to sign changes in the LWP difference. In general, AMSR-E LWP is larger than MODIS for small cloud fractions, low values of LWP, and warmer cloud top temperatures. On the other hand, clouds with optical thicknesses above 20 lead to larger MODIS LWP. Using cloud optical thickness as a proxy for cloud type, deep convective clouds and stratus are shown to have the poorest agreement between AMSR-E and MODIS LWP. Particularly large differences are also found at latitudes poleward of 50°. The results of this work help characterize the scene- and cloud-dependent performance of microwave and visible/near infrared retrievals of LWP.
