G. G. Pfister

The Impact of Boreal Forest Fire on Climate Warming

We report measurements and analysis of a boreal forest fire, integrating the effects of greenhouse gases, aerosols, black carbon deposition on snow and sea ice, and postfire changes in surface albedo. The net effect of all agents was to increase radiative forcing during the first year (34 ± 31 Watts per square meter of burned area), but to decrease radiative forcing when averaged over an 80-year fire cycle (–2.3 ± 2.2 Watts per square meter) because multidecadal increases in surface albedo had a larger impact than fire-emitted greenhouse gases. This result implies that future increases in boreal fire may not accelerate climate warming.

Cloud Coverage Based on All-Sky Imaging and Its Impact on Surface Solar Irradiance

In Lauder, Central Otago, New Zealand, two all-sky imaging systems have been in operation for more than 1 yr, measuring the total, opaque, and thin cloud fraction, as well as indicating whether the sun is obscured by clouds. The data provide a basis for investigating the impact of clouds on the surface radiation field. The allsky cloud parameters were combined with measurements of global, direct, and diffuse surface solar irradiance over the spectral interval from 0.3 to 3 mm. Here, the results of ongoing analysis of this dataset are described. As a reference for the magnitude of the cloud influence, clear-sky irradiance values are estimated as a simple function of solar zenith angle and the earth‐sun distance. The function is derived from a least squares fit to measurements taken when available cloud images show clear-sky situations. Averaged over a longer time period, such as 1 month, cloud fraction and surface irradiance are clearly negatively correlated. Monthly means in the ratio of the measured surface irradiance to the clear-sky value had a correlation coefficient of about 20.9 with means of cloud fraction for the months from July 2000 to June 2001. In the present work reductions in the surface irradiance and situations in which clouds cause radiation values to exceed the expected clear-sky amount are analyzed. Over 1 yr of observations, 1-min-averaged radiation measurements exceeding the expected clearsky value by more than 10% were observed with a frequency of 5%. In contrast, a reduction of more than 10% below estimated clear-sky values occurred in 66% of the cases, while clear-sky irradiances (measured irradiance within 610% of estimated clear-sky value) were observed 29% of the time. Low cloud fractions frequently lead to moderate enhancement, because the sun is often unobscured and the clouds are brighter than the sky that they hide. As cloud fraction increases the sun is likely to be obscured, causing irradiance values to fall well below clear-sky values. However, in the case of unobscured sun, there is a tendency for strongest enhancements when cloud fractions are highest. Enhancements, especially at high solar zenith angle, are also often observed in association with thin clouds.

Significant enhancements of nitrogen oxides, black carbon, and ozone in the North Atlantic lower free troposphere resulting from North American boreal wildfires

enhancements of CO, BC, NOy and NOx, with levels up to 250 ppbv, 665 ng m 3 , 1100 pptv and 135 pptv, respectively. Enhancement ratios relative to CO were variable in the plumes sampled, most likely because of variations in wildfire emissions and removalprocessesduringtransport.AnalysesofDBC/DCO,DNOy/DCOandDNOx/DCO ratios indicate that NOy and BC were on average efficiently exported in these plumes and suggest that decomposition of PAN to NOx was a significant source of NOx. High levels of NOx suggest continuing formation of O3 in these well-aged plumes. O3 levels were also significantly enhanced in the plumes, reaching up to 75 ppbv. Analysis of DO3/DCO ratios showed distinct behaviors of O3 in the plumes, which varied from significant to lower O3 production. We identify several potential reasons for the complex effects of boreal wildfire emissions on O3 and conclude that this behavior needs to be explored further in the future. These observations demonstrate that boreal wildfire emissions significantly contributed to the NOx and O3 budgets in the central North Atlantic lower free troposphere during summer 2004 and imply large-scale impacts on direct radiative forcing of the atmosphere and on tropospheric NOx and O3.

International Photolysis Frequency Measurement and Model Intercomparison (IPMMI): Spectral actinic solar flux measurements and modeling

[1] The International Photolysis Frequency Measurement and Model Intercomparison (IPMMI) took place in Boulder, Colorado, from 15 to 19 June 1998, aiming to investigate the level of accuracy of photolysis frequency and spectral downwelling actinic flux measurements and to explore the ability of radiative transfer models to reproduce the measurements. During this period, 2 days were selected to compare model calculations with measurements, one cloud-free and one cloudy. A series of ancillary measurements were also performed and provided parameters required as input to the models. Both measurements and modeling were blind, in the sense that no exchanges of data or calculations were allowed among the participants, and the results were objectively analyzed and compared by two independent referees. The objective of this paper is, first, to present the results of comparisons made between measured and modeled downwelling actinic flux and irradiance spectra and, second, to investigate the reasons for which some of the models or measurements deviate from the others. For clear skies the relative agreement between the 16 models depends strongly on solar zenith angle (SZA) and wavelength as well as on the input parameters used, like the extraterrestrial (ET) solar flux and the absorption cross sections. The majority of the models (11) agreed to within about +/-6% for solar zenith angles smaller than similar to60degrees. The agreement among the measured spectra depends on the optical characteristics of the instruments (e.g., slit function, stray light rejection, and sensitivity). After transforming the measurements to a common spectral resolution, two of the three participating spectroradiometers agree to within similar to10% for wavelengths longer than 310 nm and at all solar zenith angles, while their differences increase when moving to shorter wavelengths. Most models agree well with the measurements (both downwelling actinic flux and global irradiance), especially at local noon, where the agreement is within a few percent. A few models exhibit significant deviations with respect either to wavelength or to solar zenith angle. Models that use the Atmospheric Laboratory for Applications and Science 3 (ATLAS-3) solar flux agree better with the measured spectra, suggesting that ATLAS-3 is probably more appropriate for radiative transfer modeling in the ultraviolet.

Contribution of isoprene to chemical budgets: A model tracer study with the NCAR CTM MOZART‐4

[1] We present a study of the sensitivity of isoprene emission calculations in a global chemistry transport model (CTM) to input land cover characteristics and analyze the impacts of changes in isoprene on the tropospheric budgets of atmospheric key species. The CTM Model for Ozone and Related Chemical Species, version 4 (MOZART-4) includes the online calculation of isoprene emissions based on the Model of Emissions of Gases and Aerosols from Nature (MEGAN), which is driven by three different land parameter inputs. We also included a tagging scheme in the CTM, which keeps track of the production of carbon containing species from isoprene oxidation. It is found that the amount of tropospheric carbon monoxide (CO), formaldehyde (HCHO) and peroxyacetylnitrate (PAN) explained by isoprene oxidation ranges from 9–16%, 15–27%, and 22–32%, depending on the isoprene emissions scenario. Changes in the global tropospheric burden with different land cover inputs can reach up to 10% for CO, 15% for HCHO, and 20% for PAN. Changes for ozone are small on a global scale, but regionally differences are as large as 3DU in the tropospheric column and as large as 5 ppbv in the surface concentrations. Our results demonstrate that a careful integration of isoprene emissions and chemistry in CTMs is very important for simulating the budgets of a number of atmospheric trace gases. We further demonstrate that the model tagging scheme has the capability of improving conventional methods of constraining isoprene emissions from space-borne HCHO column observations, especially in regions where a considerable part of the variability in the HCHO column is not related to isoprene.

Ozone production from the 2004 North American boreal fires

We examine the ozone production from boreal forest fires based on a case study of wildfires in Alaska and Canada in summer 2004. The model simulations were performed with the chemistry transport model, MOZART-4, and were evaluated by comparison with a comprehensive set of aircraft measurements. In the analysis we use measurements and model simulations of carbon monoxide (CO) and ozone (O3) at the PICO-NARE station located in the Azores within the pathway of North American outflow. The modeled mixing ratios were used to test the robustness of the enhancement ratio ΔO3/ΔCO (defined as the excess O3 mixing ratio normalized by the increase in CO) and the feasibility for using this ratio in estimating the O3 production from the wildfires. Modeled and observed enhancement ratios are about 0.25 ppbv/ppbv which is in the range of values found in the literature and results in a global net O3 production of 12.9 ± 2 Tg O3 during summer 2004. This matches the net O3 production calculated in the model for a region extending from Alaska to the east Atlantic (9–11 Tg O3) indicating that observations at PICO-NARE representing photochemically well aged plumes provide a good measure of the O3 production of North American boreal fires. However, net chemical loss of fire-related O3 dominates in regions far downwind from the fires (e.g., Europe and Asia) resulting in a global net O3 production of 6 Tg O3 during the same time period. On average, the fires increased the O3 burden (surface −300 mbar) over Alaska and Canada during summer 2004 by about 7–9% and over Europe by about 2–3%.

From model intercomparison toward benchmark UV spectra for six real atmospheric cases

The validity of a radiative transfer model can be checked either by comparing its results with measurements or with solutions for artificial cases. Unfortunately, neither type of comparison can guarantee that the spectral UV surface irradiance is accurately calculated for real atmospheric cases. There is a need therefore for benchmarks, i.e., standard results that can be used as a validation tool for UV radiation models. In this paper we give such benchmarks for six cloud-free situations. The chosen cases are characterized by different values of solar zenith angle, ozone column, aerosol loading, and surface albedo. Observations are also available for these cases to allow a further comparison between model results and measurements. An intercomparison of 12 numerical models is used to construct the benchmarks. Each model is supplied with identical input data, and a distinction is made between models that assume a planeparallel geometry and those that use a pseudospherical approximation. Differences remain between the model results, because of different treatments of the input data set. Calculations of direct and global transmission and direct and global irradiance are within 3% for wavelengths longer than 320 nm. For the low-Sun cases the calculations are within 10% for wavelengths longer than 300 nm. On the basis of these calculations, six benchmark UV spectra (295–400 nm) are established with a standard deviation of 2%. Relative standard deviations are higher for the lowest absolute intensities at low Sun (5% at 300 nm). The variation between models is typically less than the variation seen between model and measurement. Differences between the benchmarks and the observed spectra are mainly due to the uncertainty in the input parameters. In four of the six cases the benchmarks agree with the observed spectra within 13% over the whole UV spectral region.

Evidence of significant large‐scale impacts of boreal fires on ozone levels in the midlatitude Northern Hemisphere free troposphere

Summertime observations of O 3 and CO made at the PICO-NARE station during 2001, 2003, and 2004 are used to assess the impact of boreal forest fires on the distribution of O 3 mixing ratios in the midlatitude Northern Hemisphere (NH) lower free troposphere (FT). Backward trajectories were used to select measurements impacted by outflow from high-latitude regions. Measurements during these periods were segregated into two subsets: those obtained during periods with and without apparent significant upwind fire emissions. Periods affected by fire emissions were identified based on enhanced CO levels confirmed by global simulations of fire emissions transport. During fireimpacted periods, O 3 was shifted toward higher mixing ratios, with medians significantly higher than in periods without detectable upwind fire impacts. This implies a significant impact of boreal wildfires on midlatitude lower FT background O 3 during summer. Predicted future increases in boreal wildfires may therefore affect summertime O 3 levels over large regions.

Photolysis frequency of NO2: Measurement and modeling during the International Photolysis Frequency Measurement and Modeling Intercomparison (IPMMI)

[1] The photolysis frequency of NO2, j(NO2), was determined by various instrumental techniques and calculated using a number of radiative transfer models for 4 days in June 1998 at the International Photolysis Frequency Measurement and Modeling Intercomparison (IPMMI) in Boulder, Colorado. Experimental techniques included filter radiometry, spectroradiometry, and chemical actinometry. Eight research groups participated using 14 different instruments to determine j(NO2). The blind intercomparison experimental results were submitted to the independent experimental referee and have been compared. Also submitted to the modeling referee were the results of NO2 photolysis frequency calculations for the same time period made by 13 groups who used 15 different radiative transfer models. These model results have been compared with each other and also with the experimental results. The model calculation of clear-sky j(NO2) values can yield accurate results, but the accuracy depends heavily on the accuracy of the molecular parameters used in these calculations. The instrumental measurements of j(NO2) agree to within the uncertainty of the individual instruments and indicate the stated uncertainties in the instruments or the uncertainties of the molecular parameters may be overestimated. This agreement improves somewhat with the use of more recent NO2 cross-section data reported in the literature. INDEX TERMS: 0360 Atmospheric Composition and Structure: Transmission and scattering of radiation; 0365 Atmospheric Composition and Structure: Troposphere—composition and chemistry; 0394 Atmospheric Composition and Structure: Instruments and techniques; KEYWORDS: photolysis, NO2 (nitrogen dioxide), radiative transfer, intercomparison Citation: Shetter, R. E., et al., Photolysis frequency of NO2: Measurement and modeling during the International Photolysis Frequency Measurement and Modeling Intercomparison (IPMMI), J. Geophys. Res., 108(D16), 8544, doi:10.1029/2002JD002932, 2003.

Evaluation of the MOCAGE chemistry transport model during the ICARTT/ITOP experiment

Intercontinental Transport of Ozone and Precursors (ITOP), part of International Consortium for Atmospheric Research on Transport and Transformation (ICARTT), was a large experimental campaign designed to improve our understanding of the chemical transformations within plumes during long-range transport (LRT) of pollution from North America to Europe. This campaign took place in July and August 2004, when a strong fire season occurred in North America. Burning by-products were transported over large distances, sometimes reaching Europe. A chemical transport model, Modelisation de la Chimie Atmospherique Grande Echelle (MOCAGE), with a high grid resolution (0.5° × 0.5°) over the North Atlantic area and a daily inventory of biomass burning emissions over the United States, has been used to simulate the period. By comparing our results with available aircraft in situ measurements and satellite data (MOPITT CO and SCIAMACHY NO2), we show that MOCAGE is capable of representing the main characteristics of the tropospheric ozone-NOx-hydrocarbon chemistry during the ITOP experiment. In particular, high resolution allows the accurate representation of the pathway of exported pollution over the Atlantic, where plumes were transported preferentially at 6 km altitude. The model overestimates OH mixing ratios up to a factor of 2 in the lower troposphere, which results in a global overestimation of hydrocarbons oxidation by-products (PAN and ketones) and an excess of O3 (30–50 ppbv) in the planetary boundary layer (PBL) over the continental United States. Sensitivity study revealed that lightning NO emissions contributed significantly to the NOx budget in the upper troposphere of northeast America during the summer 2004.