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Impacts of the January 2005 solar particle event on noctilucent clouds and water at the polar summer mesopause

The response of noctilucent clouds to the solar particle event in January 2005 is investigated by means of icy particle and ion chemistry simulations. It is shown that the decreasing occurrence rate of noctilucent clouds derived from measurements of the SCIAMACHY/Envisat instrument can be reproduced by one-dimensional model simulations if temperature data from the MLS/Aura instrument are used. The model calculations indicate that the sublimation of noctilucent clouds leads to significant changes of the water distribution in the mesopause region. These model results are compared with H2O measurements from the MLS and the MIPAS/Envisat satellite instruments. The pronounced modelled water enhancement below the icy particle layer and its decrease during the SPE are not observed by the satellite instruments. At altitudes >85 km the satellite measurements show an increase of H2O during the SPE in qualitative agreement with the model predictions. The discrepancies between model H2O and observations at lower altitudes might be attributed to the one-dimensional model approach which in particular neglects inhomogeneities and horizontal transport processes. Additionally, it is revealed that the water depletion due to reactions of proton hydrates during the considered solar particle event has only a minor impact on the icy particles.
Semi-continuous gas and inorganic aerosol measurements at a Finnish urban site: comparisons with filters, nitrogen in aerosol and gas phases, and aerosol acidity

Concentrations of 5 gases (HCl, HNO3, HONO, NH3, SO2) and 8 major inorganic ions in particles (Cl−, NO3−, SO42−, NH4+, Na+, K+, Mg2+, Ca2+) were measured with an online monitor MARGA 2S in two size ranges, Dp <2.5 μm and Dp < 10 μm, in Helsinki, Finland from November 2009 to May 2010. The results were compared with filter sampling, mass concentrations obtained from particle number size distributions, and a conventional SO2 monitor. The MARGA yielded lower concentrations than those analyzed from the filter samples for most ions. Linear regression yielded the following MARGA vs. filter slopes: 0.72 for Cl−, 0.90 for NO3−, 0.85 for SO42−, 0.91 for NH4+ , 0.49 for Na+, 3.0 for Mg2+, and 3.0 for Ca2+ and 0.90 for the MARGA vs. SO2 monitor. For K+ there were not enough data points to calculate a statistically significant linear regression. There were clear seasonal cycles in the concentrations of the nitrogen-containing gases: the median concentrations of HNO3, HONO, and NH3 were 0.09 ppb, 0.37 ppb, and 0.01 ppb in winter, respectively, and 0.15, 0.15, and 0.14 in spring, respectively. The gas-phase fraction of nitrogen decreased roughly with decreasing temperature, so that in the coldest period from January to February the median contribution was 28% but in April to May was 53%. There were also large fractionation variations that temperature alone cannot explain. HONO correlated well with NOx but a large fraction of the HONO-to-NOx ratios were larger than published ratios in a road traffic tunnel, suggesting that a large amount of HONO had other sources than vehicle exhaust. Aerosol acidity was estimated by calculating ion equivalent ratios. The sources of acidic aerosols were studied with trajectory statistics that showed that continental aerosol is mainly neutralized and marine aerosol acidic.
A multi-sensor upper tropospheric ozone product (MUTOP) based on TES ozone and GOES water vapor: validation with ozonesondes

Accurate representation of ozone in the extratropical upper troposphere (UT) remains a challenge. However, the implementation of hyper-spectral remote sensing using satellite instruments such as the Tropospheric Emission Spectrometer (TES) provides an avenue for mapping ozone in this region, from 500 to 300 hPa. As a polar orbiting satellite TES observations are limited, but in this paper they are combined with geostationary satellite observations of water vapor. This paper describes a validation of the Multi-sensor UT Ozone Product (MUTOP). MUTOP, based on a statistical retrieval method, is an image product derived from the multiple regression of remotely sensed TES ozone, against geostationary (GOES) specific humidity (remotely sensed) and potential vorticity (a modeled dynamical tracer in the UT). These TES-derived UT ozone mixing ratios are compared to coincident ozonesonde measurements of layer-average UT ozone mixing ratios made during the NASA INTEX/B field campaign in the spring of 2006; the region for this study is effectively the GOES west domain covering the eastern North Pacific Ocean and the western United States. This intercomparison evaluates MUTOP skill at representing ozone magnitude and variability in this region of complex dynamics. In total, 11 ozonesonde launch sites were available for this study, providing 127 individual sondes for comparison; the overall mean ozone of the 500–300 hPa layer for these sondes was 78.0 ppbv. MUTOP reproduces in~situ measurements reasonably well, producing an UT mean of 82.3 ppbv, with a mean absolute error of 12.2 ppbv and a root mean square error of 16.4 ppbv relative to ozonesondes across all sites. An overall UT mean bias of 4.3 ppbv relative to sondes was determined for MUTOP. Considered in the context of past TES validation studies, these results illustrate that MUTOP is able to maintain accuracy similar to TES while expanding coverage to the entire GOES-West satellite domain. In addition MUTOP provides six-hour temporal resolution throughout the INTEX-B study period, making the visualization of UT ozone dynamics possible. This paper presents the overall statistical validation as well as a selection of ozonesonde case studies. The case studies illustrate that error may not always represent a lack of TES-derived product skill, but often results from discrepancies driven by observations made in the presence of strong meteorological gradients.
Effect of bacterial ice nuclei on the frequency and intensity of lightning activity inferred by the BRAMS model

Many studies from the last decades have shown that airborne microorganisms can be intrinsically linked to atmospheric processes. Certain bacteria may constitute the most active ice nuclei found in the atmosphere and might have some influence on the formation of ice crystals in clouds. This study deals with the ice nucleation activity of Pseudomonas syringae inside of thunderstorms through numerical simulations using BRAMS (Brazilian Regional Atmospheric Model System). The numerical simulations were developed in order to investigate the effect on the total amount of rainwater as a function of ice nuclei (IN) P. syringae concentrations with different scenarios (classified as S2 to S4 scenarios) corresponding to a maximum of 102 to 104 IN bacteria per liter of cloud water plus the BRAMS default (classified as S5 scenario). Additionally, two other scenarios were included without any IN (S1) and the sum of RAMS default and S4 scenario (classified as S6). The chosen radiosonde data is for 3 March 2003, typical summertime in São Paulo City which presents a strong convective cell. The objective of the simulations was to analyze the effect of the IN concentrations on the BRAMS modeled cloud properties and precipitation. The simulated electrification of the cloud permitted analysis of the total flashes estimated from precipitable and non-precipitable ice mass fluxes in two different lightning frequencies. Among all scenarios, only S4 and S6 presented a tendency to decrease the total cloud water, and all bacteria scenarios presented a tendency to decrease the total amount of rain (−8%), corroborating other reports in the literature. All bacteria scenarios also present higher precipitable ice concentrations compared to S5 scenario, the RAMS default. The main results present the total flash number per simulation as well. From the results, the total flash numbers, from both lightning frequencies, in S4 and S6 scenarios, are from 3.1 to 3.7 higher than the BRAMS default. Even the lower bacterial concentrations (scenarios S2 and S3) produced 3 time higher number of flashes, compared to S5 scenario. This result is a function of the hydrometeors in each simulation. In conclusion, IN bacteria could affect directly the thunderstorm structure and lightning formation with many other microphysical implications.
Regional and global modeling of aerosol optical properties with a size, composition, and mixing state resolved particle microphysics model

There exist large uncertainties in the present modeling of physical, chemical, and optical properties of atmospheric particles. We have recently incorporated an advanced particle microphysics (APM) model into a global chemistry transport model (GEOS-Chem) and a regional weather forecasting and chemistry model (WRF-Chem). Here we develop a scheme for calculating regional and global aerosol optical depth (AOD) from detailed aerosol information resolved by the APM model. According to GEOS-Chem-APM simulations, in most parts of the globe, the mass of secondary species resides mainly within secondary particles (60–90%), but in certain regions a large fraction (up to 50–80%) can become coated on various primary particles. Secondary species coated on black carbon and primary organic carbon particles significantly increase the size and hygroscopicity of these particles and thus impact their optical properties. The GEOS-Chem-APM model captures the global spatial distributions of AOD derived from AERONET, MODIS, and MISR measurements, generally within a factor of ~2. Our analysis indicates that modeled annual mean AODs at all sky and clear sky conditions differ by ~20% globally averaged and by >50% in some regions. The time series of WRF-Chem-APM predicted AOD over the northeastern United States in June 2008 have been compared to those from seven AERONET sites. Overall, the model mostly captures the absolute values as well as the variations of AOD at the AERONET sites (including dramatic changes associated with the crossing of high AOD plumes). Both GEOS-Chem and WRF-Chem simulations indicate that AOD over the northeastern US is dominated by secondary particles and have large spatiotemporal variations.
Understanding and forecasting polar stratospheric variability with statistical models

The variability of the north-polar stratospheric vortex is a prominent aspect of the middle atmosphere. This work investigates a wide class of statistical models with respect to their ability to model geopotential and temperature anomalies, representing variability in the polar stratosphere. Four partly nonstationary, nonlinear models are assessed: linear discriminant analysis (LDA); a cluster method based on finite elements (FEM-VARX); a neural network, namely the multi-layer perceptron (MLP); and support vector regression (SVR). These methods model time series by incorporating all significant external factors simultaneously, including ENSO, QBO, the solar cycle, volcanoes, to then quantify their statistical importance. We show that variability in reanalysis data from 1980 to 2005 is successfully modeled. The period from 2005 to 2011 can be hindcasted to a certain extent, where MLP performs significantly better than the remaining models. However, variability remains that cannot be statistically hindcasted within the current framework, such as the unexpected major warming in January 2009. Finally, the statistical model with the best generalization performance is used to predict a winter 2011/12 with warm and weak vortex conditions. A vortex breakdown is predicted for late January, early February 2012.
Assessing large-scale weekly cycles in meteorological variables: a review

Several studies have claimed to have found significant weekly cycles of meteorological variables appearing over large domains, which can hardly be related to urban effects exclusively. Nevertheless, there is still an ongoing scientific debate whether these large-scale weekly cycles exist or not, and some other studies fail to reproduce them with statistical significance. In addition to the lack of the positive proof for the existence of these cycles, their possible physical explanations have been controversially discussed during the last years. In this work we review the main results about this topic published during the recent two decades, including a summary of the existence or non-existence of significant weekly weather cycles across different regions of the world, mainly over the US, Europe and Asia. In addition, some shortcomings of common statistical methods for analyzing weekly cycles are listed. Finally, a brief summary of supposed causes of the weekly cycles, focusing on the aerosol-cloud-radiation interactions and their impact on meteorological variables as a result of the weekly cycles of anthropogenic activities, and possible directions for future research, is presented.
Development of a climate record of tropospheric and stratospheric column ozone from satellite remote sensing: evidence of an early recovery of global stratospheric ozone

Ozone data beginning October 2004 from the Aura Ozone Monitoring Instrument (OMI) and Aura Microwave Limb Sounder (MLS) are used to evaluate the accuracy of the Cloud Slicing technique in effort to develop long data records of tropospheric and stratospheric ozone and for studying their long-term changes. Using this technique, we have produced a 32-yr (1979–2010) long record of tropospheric and stratospheric column ozone from the combined Total Ozone Mapping Spectrometer (TOMS) and OMI. Analyses of these time series suggest that the quasi-biennial oscillation (QBO) is the dominant source of inter-annual variability of stratospheric ozone and is clearest in the Southern Hemisphere during the Aura time record with related inter-annual changes of 30–40 Dobson Units. Tropospheric ozone for the long record also indicates a QBO signal in the tropics with peak-to-peak changes varying from 2 to 7 DU. The most important result from our study is that global stratospheric ozone indicates signature of a recovery occurring with ozone abundance now approaching the levels of year 1980 and earlier. The negative trends in stratospheric ozone in both hemispheres during the first 15 yr of the record are now positive over the last 15 yr and with nearly equal magnitudes. This turnaround in stratospheric ozone loss is occurring about 20 yr earlier than predicted by many chemistry climate models. This suggests that the Montreal Protocol which was first signed in 1987 as an international agreement to reduce ozone destroying substances is working well and perhaps better than anticipated.
Importance of biogenic precursors to the budget of organic nitrates: observations of multifunctional organic nitrates by CIMS and TD-LIF during BEARPEX 2009

Alkyl and multifunctional organic nitrates, molecules of the chemical form RONO2, are products of chain terminating reactions in the tropospheric HOx and NOx catalytic cycles and thereby impact ozone formation locally. Many of the molecules in the class have lifetimes that are long enough that they can be transported over large distances. If the RONO2 then decompose to deliver NOx to remote regions they affect ozone production rates in locations distant from the original NOx source. While measurements of total RONO2 (ΣANs) and small straight chain alkyl nitrates are routine, measurements of the specific multifunctional RONO2 molecules that are believed to dominate the total have rarely been reported and never reported in coincidence with ambient ΣANs measurements. Here we describe observations obtained during the BEARPEX 2009 experiment including ΣANs and a suite of multifunctional nitrates including isoprene derived hydroxynitrates, oxidation products of those nitrates, 2-methyl-3-buten-2-ol (MBO) derived hydroxynitrates, and monoterpene nitrates. At the BEARPEX field site, the sum of the individual biogenically derived nitrates account for two-thirds of the ΣANs, confirming predictions of the importance of biogenic nitrates to the NOy budget. Isoprene derived nitrates, transported to the site, are a much larger fraction of the ΣANs at the site than the nitrates derived from the locally emitted MBO. Evidence for additional nitrates, possibly from nocturnal chemistry of isoprene and α-pinene, is presented.
Climatological perspectives of air transport from atmospheric boundary layer to tropopause layer over Asian monsoon regions during boreal summer inferred from Lagrangian approach

The Asian Summer Monsoon (ASM) region has been recognized as a key region that plays a vital role in troposphere-to-stratosphere transport (TST), which can significant impact the budget of global atmospheric constituents and climate change. However, the details of transport from the boundary layer (BL) to tropopause layer (TL) over these regions, particularly from a climatological perspective, remain an issue of uncertainty. In this study, we present the climatological properties of BL-to-TL transport over the ASM region during boreal summer season (June-July-August) from 2001 to 2009. A comprehensive tracking analysis is conducted based on a large ensemble of TST-trajectories departing from the atmospheric BL and arriving at TL. Driven by the winds fields from NCEP/NCAR Global Forecast System, all the TST-trajectories are selected from the high resolution datasets generated by the Lagrangian particle transport model FLEXPART using a domain-filling technique. Three key atmospheric boundary layer sources for BL-to-TL transport are identified with their contributions: (i) 38% from the region between tropical Western Pacific region and South China Seas (WP) (ii) 21% from Bay of Bengal and South Asian subcontinent (BOB), and (iii) 12% from the Tibetan Plateau, which includes the South Slope of the Himalayas (TIB). Controlled by the different patterns of atmospheric circulation, the air masses originated from these three source regions are transported along the different tracks into the TL. The spatial distributions of three source regions keep similarly from year to year. The timescales of transport from BL to TL by the large-scale ascents r-range from 1 to 7 weeks contributing up to 60–70% of the overall TST, whereas the transport governed by the deep convection overshooting become faster on a timescales of 1–2 days with the contributions of 20–30%. These results provide clear policy implications for the control of very short lived substances, especially for the source regions over Indian subcontinent with increasing populations and developing industries.