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A decadal satellite analysis of the origins and impacts of smoke in Colorado

We analyze the record of aerosol optical depth (AOD) measured by the MODerate resolution Imaging Spectroradiometer (MODIS) aboard the Terra satellite in combination with surface PM2.5 to investigate the impact of fires on aerosol loading and air quality over Colorado from 2000 to 2012, and to evaluate the contribution of local versus transported smoke. Fire smoke contributed significantly to the AOD levels observed over Colorado. During the worst fire seasons of 2002 and 2012, average MODIS AOD over the Colorado Front Range corridor were 20–50% larger than the other 11 yr studied. Surface PM2.5 was also unusually elevated during fire events and concentrations were in many occasions above the daily National Ambient Air Quality Standard (35 μg m−3) and even reached locally unhealthy levels (> 100 μg m−3) over populated areas during the 2012 High Park fire and the 2002 Hayman fire. Over the 13 yr examined, long-range transport of smoke from northwestern US and even California (> 1500 km distance) occurred often and affected AOD and surface PM2.5. During most of the transport events, MODIS AOD and surface PM2.5 were reasonable correlated (r2 = 0.2–0.9), indicating that smoke subsided into the Colorado boundary layer and reached surface levels. However, that is not always the case since at least one event of AOD enhancement was disconnected from the surface (r2<0.01 and low PM2.5 levels). Observed plume heights from the Multi-angle Imaging SpectroRadiometer (MISR) satellite instrument and vertical aerosol profiles measured by the space-based Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) showed a complex vertical distribution of smoke emitted by the High Park fire in 2012. Smoke was detected from a range of 1.5 to 7.5 km altitude at the fire origin and from ground levels to 12.3 km altitude far away from the source. The variability of smoke altitude as well as the local meteorology were key in determining the aerosol loading and air quality over the Colorado Front Range region. Our results underline the importance of accurate characterization of the vertical distribution of smoke for estimating the air quality degradation associated with fire activity and its link to human health.
European atmosphere in 2050, a regional air quality and climate perspective under CMIP5 scenarios

To quantify changes in air pollution over Europe at the 2050 horizon, we designed a comprehensive modelling system that captures the external factors considered to be most relevant, and that relies on up-to-date and consistent sets of air pollution and climate policy scenarios. Global and regional climate as well as global chemistry simulations are based on the recent representative concentration pathways (RCP) produced for the Fifth Assessment Report (AR5) of the IPCC (Intergovernmental Panel on Climate Change) whereas regional air quality modelling is based on the updated emissions scenarios produced in the framework of the Global Energy Assessment. We explored two diverse scenarios: a reference scenario where climate policies are absent and a mitigation scenario which limits global temperature rise to within 2 °C by the end of this century. This first assessment of projected air quality and climate at the regional scale based on CMIP5 (5th Coupled Model Intercomparison Project) climate simulations is in line with the existing literature using CMIP3. The discrepancy between air quality simulations obtained with a climate model or with meteorological reanalyses is pointed out. Sensitivity simulations show that the main factor driving future air quality projections is air pollutant emissions, rather than climate change or intercontinental transport of pollution. Whereas the well documented "climate penalty" that weights upon ozone (increase of ozone pollution with global warming) over Europe is confirmed, other features appear less robust compared to the literature, such as the impact of climate on PM2.5. The quantitative disentangling of external factors shows that, while several published studies focused on the climate penalty bearing upon ozone, the contribution of the global ozone burden is somewhat overlooked in the literature.
Free troposphere as a major source of CCN for the equatorial pacific boundary layer: long-range transport and teleconnections

Airborne aerosol measurements in the central equatorial Pacific during PASE (Pacific Atmospheric Sulfur Experiment) revealed that cloud condensation nuclei (CCN) activated in marine boundary layer (MBL) clouds were strongly influenced by entrainment from the free troposphere (FT). About 65% entered at sizes effective as CCN in MBL clouds, while ~25% entered the MBL too small to activate but subsequently grew via gas to particle conversion. The remaining ~10% were inferred to be sea salt aerosol. FT aerosols at low carbon monoxide (CO) mixing ratios (< 63 ppbv) were mostly volatile at 360 °C with a number mode peak of around 30–40 nm dry diameter and tended to be associated with cloud outflow from distant (3000 km or more) deep convection. Higher CO concentrations were commonly associated with trajectories from South America and the Amazon region (ca. ~10 000 km away) and occurred in layers indicative of combustion sources (biomass burning season) partially scavenged by precipitation. These had number modes near 60–80 nm dry diameter with a large fraction of CCN.2 (those activated at 0.2% supersaturation and representative of MBL clouds) prior to entrainment into the MBL. Flight averaged concentrations of CCN.2 were similar for measurements near the surface, below the inversion and in the FT just above the inversion, confirming that subsidence and entrainment of FT aerosol strongly influenced MBL CCN.2. Concurrent flight-to-flight variations of CCN.2 at all altitudes below 3 km also imply MBL CCN.2 concentrations were in quasi-equilibrium with the FT over a 2–3 day timescale. The observed FT transport over thousands of kilometers indicates teleconnections between MBL CCN and cloud-scavenged sources of both natural and/or residual combustion origin. Nonetheless, in spite of its importance, this source of CCN number is not well represented in most current models and is generally not detectable by satellite because of the low aerosol scattering in such layers as a result of cloud scavenging. In addition, our measurements confirm nucleation in the MBL was not evident during PASE and argue against a localized linear relation in the MBL between dimethyl sulfide (DMS) and CCN suggested by the CLAW hypothesis. However, when the FT is not impacted by long-range transport, sulfate aerosol derived from DMS pumped aloft in the ITCZ (Inter-Tropical Convergence Zone) can provide a source of CCN to the boundary layer via FT teleconnections involving more complex non-linear processes.
Diurnal variation of stratospheric and lower mesospheric HOCl, ClO and HO2 at the equator: comparison of 1-D model calculations with measurements by satellite instruments

The diurnal variation of HOCl and the related species ClO, HO2 and HCl measured by satellites has been compared with the results of a one-dimensional photochemical model. The study compares the data from various limb-viewing instruments with model simulations from the middle stratosphere to the lower mesosphere. Data from three sub-millimetre instruments and two infrared spectrometers are used, namely from the Sub-Millimetre Radiometer (SMR) on board Odin, the Microwave Limb Sounder (MLS) on board Aura, the Superconducting Submillimeter-wave Limb-Emission Sounder (SMILES) on the International Space Station, the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on board ENVISAT, and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) on board SCISAT. Inter-comparison of the measurements from instruments on sun-synchronous satellites (SMR, MLS, MIPAS) and measurements from solar occultation instruments (ACE-FTS) is challenging since the measurements correspond to different solar zenith angles (or local times). However, using a model which covers all solar zenith angles and data from the SMILES instrument which measured at all local times over a period of several months provides the possibility to verify the model and to indirectly compare the diurnally variable species. The satellite data were averaged for latitudes of 20° S to 20° N for the SMILES observation period from November 2009 to April 2010 and were compared at three altitudes: 35, 45 and 55 km. Besides presenting the SMILES data, the study also shows a first comparison of the latest MLS data (version 3.3) of HOCl, ClO, and HO2 with other satellite observations, as well as a first evaluation of HO2 observations made by Odin/SMR. The MISU-1D model has been carefully initialised and run for conditions and locations of the observations. The diurnal cycle features for the species investigated here are generally well reproduced by the model. The satellite observations and the model agree well in terms of absolute mixing ratios. The differences between the day and night values of the model are in good agreement with the observations although the amplitude of the HO2 diurnal variation is 10–20% lower in the model than in the observations. In particular, the data offered the opportunity to study the reaction ClO+HO2 → HOCl+O2 in the lower mesosphere at 55 km. At this altitude the HOCl night-time variation depends only on this reaction. The result of this analysis points towards a value of the rate constant within the range of the JPL 2006 recommendation and the upper uncertainty limit of the JPL 2011 recommendation at 55 km.
Monte Carlo-based subgrid parameterization of vertical velocity and stratiform cloud microphysics in ECHAM5.5-HAM2

A new method for parameterizing the subgrid variations of vertical velocity and cloud droplet number concentration (CDNC) is presented for general circulation models (GCMs). These parameterizations build on top of existing parameterizations that create stochastic subgrid cloud columns inside the GCM grid cells, which can be employed by the Monte Carlo independent column approximation approach for radiative transfer. The new model version adds a description for vertical velocity in individual subgrid columns, which can be used to compute cloud activation and the subgrid distribution of the number of cloud droplets explicitly. Autoconversion is also treated explicitly in the subcolumn space. This provides a consistent way of simulating the cloud radiative effects with two-moment cloud microphysical properties defined at subgrid scale. The primary impact of the new parameterizations is to decrease the CDNC over polluted continents, while over the oceans the impact is smaller. Moreover, the lower CDNC induces a stronger autoconversion of cloud water to rain. The strongest reduction in CDNC and cloud water content over the continental areas promotes weaker shortwave cloud radiative effects (SW CREs) even after retuning the model. However, compared to the reference simulation, a slightly stronger SW CRE is seen e.g. over mid-latitude oceans, where CDNC remains similar to the reference simulation, and the in-cloud liquid water content is slightly increased after retuning the model.
Modelling the chemistry and transport of bromoform within a sea breeze driven convective system during the SHIVA Campaign

We carry out a case study of the transport and chemistry of bromoform and its product gases (PGs) in a sea breeze driven convective episode on 19 November 2011 along the North West coast of Borneo during the "Stratospheric ozone: Halogen Impacts in a Varying Atmosphere" (SHIVA) campaign. We use ground based, ship, aircraft and balloon sonde observations made during the campaign, and a 3-D regional online transport and chemistry model capable of resolving clouds and convection explicitly that includes detailed bromine chemistry. The model simulates the temperature, wind speed, wind direction fairly well for the most part, and adequately captures the convection location, timing, and intensity. The simulated transport of bromoform from the boundary layer up to 12 km compares well to aircraft observations to support our conclusions. The model makes several predictions regarding bromine transport from the boundary layer to the level of convective detrainment (11 to 12 km). First, the majority of bromine undergoes this transport as bromoform. Second, insoluble organic bromine carbonyl species are transported to between 11 and 12 km, but only form a small proportion of the transported bromine. Third, soluble bromine species, which include bromine organic peroxides, hydrobromic acid (HBr), and hypobromous acid (HOBr), are washed out efficiently within the core of the convective column. Fourth, insoluble inorganic bromine species (principally Br2) are not washed out of the convective column, but are also not transported to the altitude of detrainment in large quantities. We expect that Br2 will make a larger relative contribution to the total vertical transport of bromine atoms in scenarios with higher CHBr3 mixing ratios in the boundary layer, which have been observed in other regions. Finally, given the highly detailed description of the chemistry, transport and washout of bromine compounds within our simulations, we make a series of recommendations about the physical and chemical processes that should be represented in 3-D chemical transport models (CTMs) and chemistry climate models (CCMs), which are the primary theoretical means of estimating the contribution made by CHBr3 and other very short-lived substances (VSLS) to the stratospheric bromine budget.
Investigation of the diurnal pattern of the vertical distribution of pollen in the lower troposphere using LIDAR

The diurnal pattern of the vertical distribution of biogenic pollen in the lower troposphere was investigated by LIDAR. Meteorological data were taken at the ground. Pollen concentrations were measured at the surface using a Burkard 7-day-recording volumetric spore sampler. Aerosol extinction coefficients and depolarization ratios at 532 nm were obtained from LIDAR measurements in spring (4 May–2 June) 2009 in Gwangju, South Korea. Linear volume depolarization ratios varied between 0.08 and 0.14 and were observed only during daytime (09:00–17:00 local time (LT)) during days of high pollen concentration (4 to 9 May). Daily average pollen concentrations ranged 1000–2500 cm−3 in the same period. The temporal evolution of the vertical distribution of the linear volume depolarization ratio showed a specific diurnal pattern. Linear volume depolarization ratios of more than 0.06, were measured near the surface in the morning. High depolarization ratios were detected up to 2 km aboveground between 12:00 and 14:00 LT, whereas high depolarization ratios were observed only close to the surface after 17:00 LT. Low values of depolarization ratios (≤0.05) were detected after 18:00 LT until the next morning. During the measurement period, the daily variations of the high depolarization ratios close to the surface showed correlation to number concentration measurements of pollen. This finding suggests that high depolarization ratios could be attributed to enhanced pollen concentrations. The diurnal characteristics of the high values of depolarization ratios are thought to be closely associated with turbulent transport. Diurnal and vertical characteristics of pollen, if measured continuously, could be used to improve the accuracy of pollen-forecasting models via data assimilation studies.
Improved simulation of regional CO2 surface concentrations using GEOS-Chem and fluxes from VEGAS

CO2 measurements have been combined with simulated CO2 distributions from a transport model in order to produce the optimal estimates of CO2 surface fluxes in inverse modeling. However, one persistent problem in using model–observation comparisons for this goal relates to the issue of compatibility. Observations at a single station reflect all underlying processes of various scales. These processes usually cannot be fully resolved by model simulations at the grid points nearest the station due to lack of spatial or temporal resolution or missing processes in the model. In this study the stations in one region were grouped based on the amplitude and phase of the seasonal cycle at each station. The regionally averaged CO2 at all stations in one region represents the regional CO2 concentration of this region. The regional CO2 concentrations from model simulations and observations were used to evaluate the regional model results. The difference of the regional CO2 concentration between observation and modeled results reflects the uncertainty of the large-scale flux in the region where the grouped stations are. We compared the regional CO2 concentrations between model results with biospheric fluxes from the Carnegie-Ames-Stanford Approach (CASA) and VEgetation-Global-Atmosphere-Soil (VEGAS) models, and used observations from GLOBALVIEW-CO2 to evaluate the regional model results. The results show the largest difference of the regionally averaged values between simulations with fluxes from VEGAS and observations is less than 5 ppm for North American boreal, North American temperate, Eurasian boreal, Eurasian temperate and Europe, which is smaller than the largest difference between CASA simulations and observations (more than 5 ppm). There is still a large difference between two model results and observations for the regional CO2 concentration in the North Atlantic, Indian Ocean, and South Pacific tropics. The regionally averaged CO2 concentrations will be helpful for comparing CO2 concentrations from modeled results and observations and evaluating regional surface fluxes from different methods.
Dependence of particle nucleation and growth on high-molecular-weight gas-phase products during ozonolysis of α-pinene

We report the first time-dependent measurements of high-molecular-weight (up to 700 amu) gas-phase oxidation products from α-pinene ozonolysis in an aerosol chamber under dry and low-NOx conditions. Measurements of products having mole fractions ranging from 10−14 to 10−11 were carried out with a chemical ionization mass spectrometer (the Cluster CIMS). Most products that were correlated with number concentrations of the smallest particles measured (10–20 nm) had molecular weights in the 430–560 amu range. Those products are proposed to be likely responsible for the initial nuclei formation and the early growth of the freshly nucleated particles based on their high molecular weights and chemical identities, both of which suggest low-volatility compounds. Another group of oxidation products in the lower mass range of 140–380 amu was well correlated with particles larger than 20 nm. We postulate that those products contributed to the later growth of particles (i.e., larger than 20 nm in diameter). Although particle nucleation in this study was primarily due to condensation of oxidation products from α-pinene ozonolysis, the involvement of residual sulfuric acid vapor in particle nucleation cannot be totally excluded.
Absorptivity of brown carbon in fresh and photo-chemically aged biomass-burning emissions

Experiments were conducted to investigate light absorption of organic aerosol (OA) in fresh and photo-chemically aged biomass-burning emissions. The experiments considered residential hardwood fuel (oak) and fuels commonly consumed in wild-land and prescribed fires in the United States (pocosin pine and gallberry). Photo-chemical aging was performed in an environmental chamber. We constrained the effective light-absorption properties of the OA using conservative limiting assumptions, and found that both primary organic aerosol (POA) in the fresh emissions and secondary organic aerosol (SOA) produced by photo-chemical aging contain brown carbon, and absorb light to a significant extent. This work presents the first direct evidence that SOA produced in aged biomass-burning emissions is absorptive. For the investigated fuels, SOA is less absorptive than POA in the long visible, but exhibits stronger wavelength-dependence and is more absorptive in the short visible and near-UV. Light absorption by SOA in biomass-burning emissions might be an important contributor to the global radiative forcing budget.