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Black carbon (BC) concentrations observed in 22 snowpits sampled in the northwest sector of the Greenland ice sheet in April 2014 have allowed us to identify a strong and widespread BC aerosol deposition event, which was dated to have accumulated in the pits from two snow storms between 27 July and 2 August 2013. This event comprises a significant portion (57 on average across all pits) of total BC deposition over 10 months (July 2013 to April 2014). Here we link this deposition event to forest fires burning in Canada during summer 2013 using modeling and remote sensing tools. Aerosols were detected by both the Cloud-Aerosol Lidar with Orthogonal Polarization (on board CALIPSO) and Moderate Resolution Imaging Spectroradiometer (Aqua) instruments during transport between Canada and Greenland. We use high-resolution regional chemical transport modeling (WRF-Chem) combined with high-resolution fire emissions (FINNv1.5) to study aerosol emissions, transport, and deposition during this event. The model captures the timing of the BC deposition event and shows that fires in Canada were the main source of deposited BC. However, the model underpredicts BC deposition compared to measurements at all sites by a factor of 2100. Underprediction of modeled BC deposition originates from uncertainties in fire emissions and model treatment of wet removal of aerosols. Improvements in model descriptions of precipitation scavenging and emissions from wildfires are needed to correctly predict deposition, which is critical for determining the climate impacts of aerosols that originate from fires.

Biomass burning is an annual occurrence in the tropical southern hemisphere (SH) and represents a major source of regional pollution. Vegetation fires emit carbon monoxide (CO), which due to its medium lifetime is an excellent tracer of tropospheric transport. CO is also one of the few tropospheric trace gases currently observed from satellite and this provides long-term global measurements. In this paper, we use the 5 year CO data record from the Measurement Of Pollution In The Troposphere (MOPITT) instrument to examine the inter-annual variability of the SH CO loading and show how this relates to climate conditions which determine the intensity of fire sources. The MOPITT observations show an annual austral springtime peak in the SH zonal CO loading each year with dry-season biomass burning emissions in S. America, southern Africa, the Maritime Continent, and northwestern Australia. Although fires in southern Africa and S. America typically produce the greatest amount of CO, the most significant inter-annual variation is due to varying fire activity and emissions from the Maritime Continent and northern Australia. We find that this variation in turn correlates well with the El Nino Southern Oscillation precipitation index. Between 2000 and 2005, emissions were greatest in late 2002 and an inverse modeling of the MOPITT data using the MOZART chemical transport model estimates the southeast Asia regional fire source for the year August 2002 to September 2003 to be 52 Tg CO. Comparison of the MOPITT retrievals and NOAA surface network measurements indicate that the latter do not fully capture the inter-annual variability or the seasonal range of the CO zonal average concentration due to biases associated with atmospheric and geographic sampling.

We analyze the transport of pollution across the Pacific during the NASA INTEX-B (Intercontinental Chemical Transport Experiment Part 8) campaign in spring 2006 and examine how this year compares to the time period for 2000 through 2006. In addition to aircraft measurements of carbon monoxide (CO) collected during INTEX-B, we include in this study multi-year satellite retrievals of CO from the Measurements of Pollution in the Troposphere (MOPITT) instrument and simulations from the chemistry transport model MOZART-4. Model tracers are used to examine the contributions of different source regions and source types to pollution levels over the Pacific. Additional modeling studies are performed to separate the impacts of inter-annual variability in meteorology and .dynamics from changes in source strength. interannual variability in the tropospheric CO burden over the Pacific and the US as estimated from the MOPITT data range up to 7% and a somewhat smaller estimate (5%) is derived from the model. When keeping the emissions in the model constant between years, the year-to-year changes are reduced (2%), but show that in addition to changes in emissions, variable meteorological conditions also impact transpacific pollution transport. We estimate that about 113 of the variability in the tropospheric CO loading over the contiguous US is explained by changes in emissions and about 213 by changes in meteorology and transport. Biomass burning sources are found to be a larger driver for inter-annual variability in the CO loading compared to fossil and biofuel sources or photochemical CO production even though their absolute contributions are smaller. Source contribution analysis shows that the aircraft sampling during INTEX-B was fairly representative of the larger scale region, but with a slight bias towards higher influence from Asian contributions.

Comparisons of aircraft measurements of carbon monoxide (CO) to the retrievals of CO using observations from the Measurements of Pollution in The Troposphere (MOPITT) instrument onboard the Terra satellite are presented. Observations made as part of the NASA INTEX-B and NSF MIRAGE field campaigns during March May 2006 are used to validate the MOPITT CO retrievals, along with routine samples from 2001 through 2006 from NOAA and the MOZAIC measurements from commercial aircraft. A significant positive bias, around 20% for total column CO, in MOPITT CO was found in the comparison to in situ measurements during 2006. Comparisons to the long-term records of measurements from NOAA and MOZAIC revealed an increasing bias in the V3 MOPITT CO retrievals over time. The impact of an instrumental drift is illustrated through retrieval simulations.

A comprehensive group of reactive nitrogen species (NO, NOz, HN03, HOzN02, PANs, alkyl nitrates, and aerosol-NO3) were measured over North America during July/August 2004 from the NASA DC-8 platform (0.1 - 12 km). Nitrogen containing tracers of biomass combustion (HCN and CH3CN) were also measured along with a host of other gaseous (CO, VOC, OVOC, halocarbon) and aerosol tracers. Clean background air as well as air with influences from biogenic emissions, anthropogenic pollution, biomass combustion, convection, lightning, and the stratosphere was sampled over the continental United States, the Atlantic, and the Pacific. The North American upper troposphere (UT) was found to be greatly influenced by both lightning NO, and surface pollution lofted via convection and contained elevated concentrations of PAN, ozone, hydrocarbons, and NO,. Observational data suggest that lightning was a far greater contributor to NO, in the UT than previously believed. PAN provided a dominant reservoir of reactive nitrogen in the UT while nitric acid dominated in the lower troposphere (LT). Peroxynitric acid (H02N02) was present in sizable concentrations peaking at around 8 km. Aerosol nitrate appeared to be mostly contained in large soil based particles in the LT. Plumes from Alaskan fires contained large amounts of PAN and aerosol nitrate but little enhancement in ozone. A comparison of observed data with simulations from four 3-D models shows significant differences between observations and models as well as among models. We investigate the partitioning and interplay of the reactive nitrogen species within characteristic air masses and further examine their role in ozone formation.

Measurements of carbon monoxide (CO) made as part of three aircraft experiments during the summer of 2004 over North America have been used for the continued validation of the CO retrievals from the Measurements of Pollution in the Troposphere (MOPITT) instrument on board the Terra satellite. Vertical profiles measured during the NASA INTEX-A campaign, designed to be coincident with MOPITT overpasses, as well as measurements made during the COBRA-2004 and MOZAIC experiments, provided valuable validation comparisons. On average, the MOPITT CO retrievals are biased slightly high for these North America locations. While the mean bias differs between the different aircraft experiments (e.g., 7.0 ppbv for MOZAIC to 18.4 ppbv for COBRA at 700 hPa), the standard deviations are quite large, so the results for the three data sets can be considered consistent. On average, it is estimated that MOPITT is 7- 14% high at 700 hPa and 03% high at 350 hPa. These results are consistent with the validation results for the Carr, Colorado, Harvard Forest, Massachusetts, and Poker Flats, Alaska, aircraft profiles for "phase 2" presented by Emmons et al. (2004) and are generally within the design criteria of 10% accuracy.

We present a global chemical data assimilation system using a global atmosphere model, the Community Atmosphere Model (CAM3) with simplified chemistry and the Data Assimilation Research Testbed (DART) assimilation package. DART is a community software facility for assimilation studies using the ensemble Kalman filter approach. Here, we apply the assimilation system to constrain global tropospheric carbon monoxide (CO) by assimilating meteorological observations of temperature and horizontal wind velocity and satellite CO retrievals from the Measurement of Pollution in the Troposphere (MOPITT) satellite instrument. We verify the system performance using independent CO observations taken on board the NSFINCAR C-130 and NASA DC-8 aircrafts during the April 2006 part of the Intercontinental Chemical Transport Experiment (INTEX-B). Our evaluations show that MOPITT data assimilation provides significant improvements in terms of capturing the observed CO variability relative to no MOPITT assimilation (i.e. the correlation improves from 0.62 to 0.71, significant at 99% confidence). The assimilation provides evidence of median CO loading of about 150 ppbv at 700 hPa over the NE Pacific during April 2006. This is marginally higher than the modeled CO with no MOPITT assimilation (-140 ppbv). Our ensemble-based estimates of model uncertainty also show model overprediction over the source region (i.e. China) and underprediction over the NE Pacific, suggesting model errors that cannot be readily explained by emissions alone. These results have important implications for improving regional chemical forecasts and for inverse modeling of CO sources and further demonstrate the utility of the assimilation system in comparing non-coincident measurements, e.g. comparing satellite retrievals of CO with in-situ aircraft measurements. The work described above also brought to light several short-comings of the data assimilation approach for CO profiles. Because of the limited vertical resolution of the measurement, the retrievals at different altitudes are correlated which can lead to problems with numerical error and overall efficiency. This has resulted in a manuscript that is about to be submitted to JGR

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 deltaO3/deltaCO (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%.

Interaction with the ongoing satellite measurements programs was an important goal of INTEX- A. The Terra/MOPITT instrument had been making global measurements of the tropospheric carbon monoxide (CO) distribution for 4 years, and was in a unique position to provide valuable support during the field campaign. Remote sensing of CO directly addressed the scientific questions motivating the IXTEX-A strategy and deployment, and measurement of this gas was rated as being mission critical. CO is an important trace gas in tropospheric chemistry due to its role in determining the atmospheric oxidizing capacity, as an ozone precursor, and as an indicator and tracer of both natural and anthropogenic pollution arising from incomplete combustion. The satellite perspective provided the more general temporal and spatial context to the aircraft and ground-based measurements during the subsequent scientific analysis. We proposed to build on the experience of supplying MOPITT data to previous field campaigns, such as TRACE-P. We provided expedited MOPITT data processing in near real-time, along with basic analysis of the measurements to indicate, where possible, the origin of the CO plumes that impacted the regions of flight operations and other in situ measurement activities. To ensure maximum exploitation of the satellite information, we will also had a scientist in the field to present and interpret the MOPITT data for the INTEX team, and to help ensure its utility in flight planning.

We describe ground-based measurements of ClO made at McMurdo Station, Antarctica, during September and October 1992. Vertical profiles were retrieved from molecular rotational emission spectra at 278 GHz. Peak mixing ratios of 1.6 +/- 0.3 ppbv were seen in mid-September at approximately 18 km altitude, suggestive of somewhat larger quantities than were measured at the same site and season in 1987. As the core of the polar vortex moved away from McMurdo by early October, the ClO mixing ratio at this altitude dropped to less than 0.2 ppbv, coincident with increasing temperature, ozone, and NO2. The diurnal variation of ClO was also observed. The lower stratospheric layer from 15 to 27 km was found to reach approximately midday abundance by 2 - 3 hours after sunrise. The column abundance in this layer began to decrease by the period 4 - 2 hours before sunset and had declined to approximately one quarter of its midday value by 2 - 0 hours before sunset. In contrast, the ClO column in the upper stratosphere, from 28 to 50 km, built up slowly until midday and remained large while sunlight persisted.

We have determined the vertical distribution of chlorine monoxide (ClO), from measurements of pressure-broadened molecular-emission spectra made over Thule, Greenland, during the 1993 Arctic spring. The measurements show a weak lower stratospheric layer of chlorine monoxide inside the vortex in late February, which was, however, significantly greater in mixing ratio than that seen in observations we made in the spring of 1992. ClO was also observed in much smaller quantities in early to mid-March 1993 when Thule was outside the vortex. The amount of ClO within the vortex was severely reduced by the time it returned over Thule in late March. This reduction occurred several weeks earlier relative to the winter solstice than the decline of ClO inside the Antarctic vortex in 1993. The enhanced Arctic lower stratospheric layer seen in late February 1993 at a nearly equivalent photochemical period, and beyond. We have calculated daily ozone loss rates, due primarily to the dimer chlorine catalytic cycle, from both sets of measurements. The vertical integral of the Arctic daily percentage ozone loss when the largest ClO levels were present, at the end of February, is found to be approximately one quarter of that in the Antarctic at a photochemical period only 1 week later. The relative weakness of daily ozone depletion, combined with the early disappearance of ClO in the Arctic, suggests that hemispheric dilution by ozone-poor air from within the Arctic vortex is unlikely to be sufficient to explain the historically extreme loss of midlatitude northern hemisphere ozone which began in 1992 and persisted throughout 1993.

We have recovered vertical profiles of stratospheric N2O from spectra observed using a ground-based mm-wave spectrometer during the Arctic spring. The measurements were made from Thule, Greenland (76.3 deg N, 68.4 deg W) on nine occasions from late February to late March, 1992 as part of the Upper Atmosphere Research Satellite (UARS) Correlative Measurements Program and the European Arctic Stratospheric Ozone Experiment (EASOE). During late February Thule was under inside edge of the Arctic vortex and mixing ratio profiles measured in that period are substantially reduced from typical high-latitude summer values. By late March the polar vortex had moved well away from Thule and N2O mixing ratios were greatly increased, coinciding with a basic change in circulation that brought in air from the Aleutian high. The motion of the vortex is also illustrated in the change in potential vorticity above Thule. A correlation with ozone balloonsonde data from Thule is made and compared to similar analyses of the Airborne Arctic Stratospheric Expedition (AASE) measurements. Within the sensitivity of our analysis, the correlation of N2O and O3 shows no evidence of ozone depletion within the vortex during this period; however, there is a distinct difference in the correlation inside and outside the vortex.

Measurements of chlorine monoxide in the stratosphere over Thule, Greenland (73.6 N, 68.4 W) were made quasi-continuously during the period February 8 to March 24, 1992, using a high-sensitivity ground based mm-wave spectrometer. These observations give diurnal, short term, and long term changes in the mixing ratio and vertical distribution of ClO. At an equivalent time after the Antarctic winter solstice, very large concentrations (up to approximately 1.5 ppbv) occur in lower stratospheric ClO, resulting in massive ozone destruction. We saw no evidence for large (approximately 1 top 1.5 ppbv) amounts of ClO in the 16-25 km range over Thule in February or March, in agreement with UARS (satellite) observations by the MLS mm-wave spectrometer for this period, and in marked contrast to UARS/MLS and ER-2 aircraft measurements over northern Europe and eastern Canada, respectively, during January, 1992. We have evidence for smaller enhancements (approximately 0.2 to 0.5 ppbv) in the 18-30 km range during late February-early March, which could result from transport of residual low NO2 air following earlier polar stratospheric cloud (PSC) processing (the last of which occurred at least one month earlier, however) or the result of chemical processing by Pinatubo aerosols. Direct influence of Pinatubo aerosols on Arctic ozone during the spring of 1992 has been difficult to assess, and this enhancement of low-altitude ClO might be a significant indicator of aerosol effects.

We describe a recently constructed ground-based mm-wave spectrometer incorporating a superconducting tunnel junction as a heterodyne mixer-receiver. Under conditions of low tropospheric water vapor, the superior sensitivity of this receiver allows spectral line measurements of stratospheric molecules with mixing ratios as small as a few tenths of a part per billion (e.g., ClO, HCN) to be made in 4 to 6 hours, with a signal to noise ratio of at least 30:1. We expect to be able to halve this time by further improvement of the mixer's intrinsic noise level.

The cooling capacity of a recently purchased RMC-Cryosystems Model LTS 4.5-025 closed-cycle He refrigerator was measured over the range 4-35 K. It is found that the nominal cooling capacity of 250 mW is only met or exceeded over a narrow temperature range around 4.3 + or - 0.5 K, and that, above this range, there exists a considerable region of much lower cooling capacity, not exceeding about 100 mW. It is believed that this behavior results from use of a fixed-aperture Joule-Thompson expansion valve, and might be alleviated if the J-T valve could be adjusted to compensate for changing flow within the 5-20 K temperature range. Present performance may severely limit or prevent effective use in applications where an irreducible heat inflow exists which is greater than about 100 mW, yet substantially less than the quoted capacity at about 4 K.