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Diurnal tracking of anthropogenic CO2 emissions in the Los Angeles basin megacity during spring 2010

Attributing observed CO2 variations to human or natural cause is critical to deducing and tracking emissions from observations. We have used in situ CO2, CO, and planetary boundary layer height (PBLH) measurements recorded during the CalNex-LA (CARB et al., 2008) ground campaign of 15 May–15 June 2010, in Pasadena, CA, to deduce the diurnally varying anthropogenic component of observed CO2 in the megacity of Los Angeles (LA). This affordable and simple technique, validated by carbon isotope observations and WRF-STILT (Weather Research and Forecasting model – Stochastic Time-Inverted Lagrangian Transport model) predictions, is shown to robustly attribute observed CO2 variation to anthropogenic or biogenic origin over the entire diurnal cycle. During CalNex-LA, local fossil fuel combustion contributed up to ~50% of the observed CO2 enhancement overnight, and ~100% of the enhancement near midday. This suggests that sufficiently accurate total column CO2 observations recorded near midday, such as those from the GOSAT or OCO-2 satellites, can potentially be used to track anthropogenic emissions from the LA megacity.
Cold trap dehydration in the Tropical Tropopause Layer characterised by SOWER chilled-mirror hygrometer network data in the Tropical Pacific

A network of balloon-borne radiosonde observations employing chilled-mirror hygrometers for water and electrochemical concentration cells for ozone has been operated since the late 1990s in the Tropical Pacific to capture the evolution of dehydration of air parcels advected quasi-horizontally in the Tropical Tropopause Layer (TTL). The analysis of this dataset is made on isentropes taking advantage of the conservative properties of tracers moving adiabatically. The existence of ice particles is diagnosed by lidars simultaneously operated with sonde flights. Characteristics of the TTL dehydration are presented on the basis of individual soundings and statistical features. Supersaturations close to 80% in relative humidity with respect to ice (RHice) have been observed in subvisible cirrus clouds located near the cold point tropopause at extremely low temperatures around 180 K. Although further observational evidence is needed to confirm the credibility of such high values of RHice, the evolution of TTL dehydration is evident from the data in isentropic scatter plots between the sonde-observed mixing ratio (OMR) and the minimum saturation mixing ratio (SMRmin) along the back trajectories associated with the observed air mass. Supersaturation exceeding the critical value of homogeneous ice nucleation (OMR > 1.6 × SMRmin) is frequently observed on the 360 and 365 K surfaces indicating that cold trap dehydration is in progress in the TTL. The near correspondence between the two (OMR ~ SMRmin) at 380 K on the other hand implies that this surface is not sufficiently cold for the advected air parcels to be dehydrated. Above 380 K, cold trap dehydration would scarcely function while some moistening occurs before the air parcels reach the lowermost stratosphere at around 400 K where OMR is generally smaller than SMRmin.
The effects of hygroscopicity on ice nucleation of fossil fuel combustion aerosols in mixed-phase clouds

Fossil fuel black carbon and organic matter (ffBC/OM) are often emitted together with sulfate, which coats the surface of these particles and changes their hygroscopicity. Observational studies at cirrus temperatures (≈−40 °C) show that the hygroscopicity of soot particles can modulate their ice nucleation ability. Here, we implement a scheme for 3 categories of soot (hydrophobic, hydrophilic and hygroscopic) on the basis of laboratory data and specify their ability to act as ice nuclei at mixed-phase temperatures by extrapolating the observations using a published deposition/condensation/immersion freezing parameterization. The new scheme results in significant changes to anthropogenic forcing in mixed-phase clouds. The net forcing in our offline model studies varies from 0.111 to 1.059 W m−2 depending on the ice nucleation capability of hygroscopic soot particles. The total anthropogenic cloud forcing and whole-sky forcing with the new scheme are 0.06 W m−2 and −2.45 W m−2, respectively, but could be more positive (by about 1.17 W m−2) if hygroscopic soot particles are allowed to nucleate ice particles. The change in liquid water path dominates the anthropogenic forcing in mixed-phase clouds.
Corrigendum to "The Australian bushfires of February 2009: MIPAS observations and GEM-AQ model results" published in Atmos. Chem. Phys., 13, 1637–1658, 2013
Stratospheric SO2 and sulphate aerosol, model simulations and satellite observations

A multiyear study with the atmospheric chemistry general circulation model EMAC with the aerosol module GMXe at high altitude resolution demonstrates that the sulfur gases COS and SO2, the latter from low-latitude volcanic eruptions, predominantly control the formation of stratospheric aerosol. The model consistently uses the same parameters in the troposphere and stratosphere for 7 aerosol modes applied. Lower boundary conditions for COS and other long-lived trace gases are taken from measurement networks, while estimates of volcanic SO2 emissions are based on satellite observations. We show comparisons with satellite data for aerosol extinction (e.g. SAGE) and SO2 in the middle atmosphere (MIPAS on ENVISAT). This corroborates the interannual variability induced by the Quasi-Biennial Oscillation, which is internally generated by the model. The model also realistically simulates the radiative effects of stratospheric and tropospheric aerosol including the effects on the model dynamics. The medium strength volcanic eruptions of 2005 and 2006 exerted a nonnegligible radiative forcing of up to −0.6 W m−2 in the tropics, while the large Pinatubo eruption caused a maximum though short term tropical forcing of about −10 W m−2. The study also shows that observed upper stratospheric SO2 can be simulated accurately only when a sulphur sink on meteoritic dust is included and the photolysis of gaseous H2SO4 in the near infrared is higher than assumed previously.
Evolution of Antarctic ozone in September–December predicted by CCMVal-2 model simulations for the 21st century

Chemistry-Climate Model Validation phase 2 (CCMVal-2) model simulations are used to analyze Antarctic ozone increases in 2000–2100 during local spring and early summer, both vertically integrated and at several pressure levels in the lower stratosphere. Multi-model median trends of monthly zonal mean total ozone column (TOC), ozone volume mixing ratio (VMR), wind speed and temperature poleward of 60° S are investigated. Median values are used to account for large variability in models, and the associated uncertainty is calculated using a bootstrapping technique. According to the trend derived from the twelve CCMVal-2 models selected, Antarctic TOC will not return to a 1965 baseline, an average of 1960–1969 values, by the end of the 21st century in September–November, but will return in ~2080 in December. The speed of December ozone depletion before 2000 was slower compared to spring months, and thus the decadal rate of December TOC increase after 2000 is also slower. Projected trends in December ozone VMR at 20–100 hPa show a much slower rate of ozone recovery, particularly at 50–70 hPa, than for spring months. Trends in temperature and winds at 20–150 hPa are also analyzed in order to attribute the projected slow increase of December ozone and to investigate future changes in the Antarctic atmosphere in general, including some aspects of the polar vortex breakup.
Mineral dust indirect effects and cloud radiative feedbacks of a simulated idealized nocturnal squall line

Mineral dust is arguably the most abundant aerosol species in the world and as such potentially plays a large role in aerosol indirect effects (AIEs). This study assesses and isolates the individual responses in a squall line that arise (1) from radiation, (2) from dust altering the microphysics, as well as (3) from the synergistic effects between (1) and (2). To accomplish these tasks, we use the Regional Atmospheric Modeling System (RAMS) set up as a cloud-resolving model (CRM). The CRM contains aerosol and microphysical schemes that allow mineral dust particles to nucleate as cloud drops and ice crystals, replenish upon evaporation and sublimation, be tracked throughout hydrometeor transition, and be scavenged by precipitation and dry sedimentation. Factor separation is used on four simulations of the squall line in order to isolate the individual roles of radiation (RADIATION), microphysically active dust (DUST MICRO), and the nonlinear interactions of those factors (SYNERGY). Results indicate that RADIATION acts to increase precipitation, intensify the cold pool, and enhance the mesoscale organization of the squall line due to changes in microphysics originating from cloud top cooling. Conversely, DUST MICRO decreases precipitation, weakens the cold pool, and weakens the mesoscale organization of the squall line due to an enhancement of the warm rain process. SYNERGY shows little impact on the squall line, except near the freezing level, where an increase in mesoscale organization takes place. The combined effect of the mineral dust AIE due to both DUST MICRO and SYNERGY is to weaken the squall line.
Observations of total RONO2 over the boreal forest: NOx sinks and HNO3 sources

In contrast with the textbook view of remote chemistry where HNO3 formation is the primary sink of nitrogen oxides, recent theoretical analyses show that formation of RONO2 (ΣANs) from isoprene and other terpene precursors is the primary net chemical loss of nitrogen oxides over the remote continents where the concentration of nitrogen oxides is low. This then increases the prominence of questions concerning the chemical lifetime and ultimate fate of ΣANs. We present observations of nitrogen oxides and organic molecules collected over the Canadian boreal forest during the summer which show that ΣANs account for ~20% of total oxidized nitrogen and that their instantaneous production rate is larger than that of HNO3. This confirms the primary role of reactions producing ΣANs as a control over the lifetime of NOx (NOx = NO + NO2) in remote, continental environments. However, HNO3 is generally present in larger concentrations than ΣANs indicating that the atmospheric lifetime of ΣANs is shorter than the HNO3 lifetime. We investigate a range of proposed loss mechanisms that would explain the inferred lifetime of ΣANs finding that in combination with deposition, two processes are consistent with the observations: (1) rapid ozonolysis of isoprene nitrates where at least ~40% of the ozonolysis products release NOx from the carbon backbone and/or (2) hydrolysis of particulate organic nitrates with HNO3 as a product. Implications of these ideas for our understanding of NOx and NOy budget in remote and rural locations are discussed.
Variability in the speed of the Brewer–Dobson circulation as observed by Aura/MLS

We use Aura/MLS stratospheric water vapour (H2O) measurements as tracer for dynamics and infer interannual variations in the speed of the Brewer–Dobson circulation (BDC) from 2004 to 2011. We correlate one-year time series of H2O in the lower stratosphere at two subsequent pressure levels (68 hPa, ~18.8 km and 56 hPa, ~19.9 km at the Equator) and determine the time lag for best correlation. The same calculation is made on the horizontal on the 100 hPa (~16.6 km) level by correlating the H2O time series at the Equator with the ones at 40° N and 40° S. From these lag coefficients we derive the vertical and horizontal speeds of the BDC in the tropics and extra-tropics, respectively. We observe a clear interannual variability of the vertical and horizontal branch. The variability reflects signatures of the Quasi Biennial Oscillation (QBO). Our measurements confirm the QBO meridional circulation anomalies and show that the speed variations in the two branches of the BDC are out of phase and fairly well anti-correlated. Maximum ascent rates are found during the QBO easterly phase. We also find that transport of H2O towards the Northern Hemisphere (NH) is on the average two times faster than to the Southern Hemisphere (SH) with a mean speed of 1.15 m s−1 at 100 hPa. Furthermore, the speed towards the NH shows much more interannual variability with an amplitude of about 21% whilst the speed towards the SH varies by only 10%. An amplitude of 21% is also observed in the variability of the ascent rate at the Equator which is on the average 0.2 mm s−1.
Aerosol composition, sources and processes during wintertime in Beijing, China

Air pollution is a major environmental concern during all seasons in the megacity of Beijing, China. Here we present the results from a winter study that was conducted from 21 November 2011 to 20 January 2012 with an Aerodyne Aerosol Chemical Speciation Monitor (ACSM) and various collocated instruments. The non-refractory submicron aerosol (NR-PM1) species vary dramatically with clean periods and pollution episodes alternating frequently. Compared to summer, wintertime submicron aerosols show much enhanced organics and chloride, which on average account for 52% and 5%, respectively, of the total NR-PM1 mass. All NR-PM1 species show quite different diurnal behaviors between summer and winter. For example, the wintertime nitrate presents a gradual increase during daytime and correlates well with secondary organic aerosol (OA), indicating a dominant role of photochemical production over gas–particle partitioning. Positive matrix factorization was performed on ACSM OA mass spectra, and identified three primary OA (POA) factors, i.e., hydrocarbon-like OA (HOA), cooking OA (COA), and coal combustion OA (CCOA), and one secondary factor, i.e., oxygenated OA (OOA). The POA dominates OA during wintertime, contributing 69%, with the other 31% being SOA. Further, all POA components show pronounced diurnal cycles with the highest concentrations occurring at nighttime. CCOA is the largest primary source during the heating season, on average accounting for 33% of OA and 17% of NR-PM1. CCOA also plays a significant role in chemically resolved particulate matter (PM) pollution as its mass contribution increases linearly as a function of NR-PM1 mass loadings. The SOA, however, presents a reverse trend, which might indicate the limited SOA formation during high PM pollution episodes in winter. The effects of meteorology on PM pollution and aerosol processing were also explored. In particular, the sulfate mass is largely enhanced during periods with high humidity because of fog processing of high concentration of precursor SO2. In addition, the increased traffic-related HOA emission at low temperature is also highlighted.