Forest emissions of biogenic volatile organic compounds (BVOCs), such as isoprene and other terpenes, play a role in the production of tropospheric ozone and aerosols. In a northern Michigan forest, the direct measurement of total OH reactivity, which is the inverse of the OH lifetime, was significantly greater than expected. The difference between measured and expected OH reactivity, called the missing OH reactivity, increased with temperature, as did emission rates for terpenes and other BVOCs. These measurements are consistent with the hypothesis that unknown reactive BVOCs, perhaps terpenes, provide the missing OH reactivity.

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We present an overview of the background, scientific goals, and execution of the Aerosol, Radiation, and Cloud Processes affecting Arctic Climate (ARCPAC) project of April 2008. We then summarize airborne measurements, made in the troposphere of the Alaskan Arctic, of aerosol particle size distributions, composition, and optical properties and discuss the sources and transport of the aerosols. The aerosol data were grouped into four categories based on gas-phase composition. First, the background troposphere contained a relatively diffuse, sulfate-rich aerosol extending from the top of the sea-ice inversion layer to 7.4 km altitude. Second, a region of depleted (relative to the background) aerosol was present within the surface inversion layer over sea-ice. Third, layers of dense, organic-rich smoke from open biomass fires in southern Russia and southeastern Siberia were frequently encountered at all altitudes from the top of the inversion layer to 7.1 km. Finally, some aerosol layers were dominated by components originating from fossil fuel combustion. <br></br> Of these four categories measured during ARCPAC, the diffuse background aerosol was most similar to the average springtime aerosol properties observed at a long-term monitoring site at Barrow, Alaska. The biomass burning (BB) and fossil fuel layers were present above the sea-ice inversion layer and did not reach the sea-ice surface during the course of the ARCPAC measurements. The BB aerosol layers were highly scattering and were moderately hygroscopic. On average, the layers produced a noontime net heating of ~0.1 K day^&minus;1 between 3 and 7 km and a slight cooling at the surface. The ratios of particle mass to carbon monoxide (CO) in the BB plumes, which had been transported over distances >5000 km, were comparable to the high end of literature values derived from previous measurements in wildfire smoke. These ratios suggest minimal precipitation scavenging and removal of the BB particles between the time they were emitted and the time they were observed in dense layers above the sea-ice inversion layer

In 2017, western Canadian wildfires injected smoke into the stratosphere that was detectable by satellites for more than 8 months. The smoke plume rose from 12 to 23 kilometers within 2 months owing to solar heating of black carbon, extending the lifetime and latitudinal spread. Comparisons of model simulations to the rate of observed lofting indicate that 2% of the smoke mass was black carbon. The observed smoke lifetime in the stratosphere was 40% shorter than calculated with a standard model that does not consider photochemical loss of organic carbon. Photochemistry is represented by using an empirical ozone-organics reaction probability that matches the observed smoke decay. The observed rapid plume rise, latitudinal spread, and photochemical reactions provide new insights into potential global climate impacts from nuclear war.

Abstract. Results from a tightly constrained photochemical point model for OH and HO2 are compared to OH and HO2 data collected during the Program for •e•earch on Oxidants: Photochemistry, Emissions, and Transport (PROPHET) summer 1998 intensive campaign held in northern Michigan. The PROPHET campaign was located in a deciduous forest marked by relatively low NOz levels and high isoprene emissions. Detailed HOz budgets are presented. The model is generally unable to match the measured OH, with the observations 2.7 times greater than the model on average. The model HO2, however, is in good agreement with the measured HO2. Even with an additional postulated OH source from the ozonolysis of unmeasured terpenes, the measured OH is 1.5 times greater than the model; the model HO2 with this added source is 15% to 30% higher than the measured HO2. Moreover, the HO2/OH ratios as modeled are 2.5 to 4 times higher than the measured ratios, indicating that the cycling between OH and HO2 is poorly described by the model. We discuss possible reasons for the discrepancies.

Abstract. This study presents airborne in situ and satellite remote sensing climatologies of cirrus clouds and humidity. The climatologies serve as a guide to the properties of cirrus clouds, with the new in situ database providing detailed insights into boreal midlatitudes and the tropics, while the satellite-borne data set offers a global overview. To this end, an extensive, quality-checked data archive, the Cirrus Guide II in situ database, is created from airborne in situ measurements during 150 flights in 24 campaigns. The archive contains meteorological parameters, ice water content (IWC), ice crystal number concentration (Nice), ice crystal mean mass radius (Rice), relative humidity with respect to ice (RHice), and water vapor mixing ratio (H2O) for each of the flights. Depending on the parameter, the database has been extended by about a factor of 5–10 compared to earlier studies. As one result of our investigation, we show that the medians of Nice, Rice, and RHice have distinct patterns in the IWC–T parameter space. Lookup tables of these variables as functions of IWC and T can be used to improve global model cirrus representation and remote sensing retrieval methods. Another outcome of our investigation is that across all latitudes, the thicker liquid-origin cirrus predominate at lower altitudes, while at higher altitudes the thinner in situ-origin cirrus prevail. Further, examination of the radiative characteristics of in situ-origin and liquid-origin cirrus shows that the in situ-origin cirrus only slightly warm the atmosphere, while liquid-origin cirrus have a strong cooling effect. An important step in completing the Cirrus Guide II is the provision of the global cirrus Nice climatology, derived by means of the retrieval algorithm DARDAR-Nice from 10 years of cirrus remote sensing observations from satellite. The in situ measurement database has been used to evaluate and improve the satellite observations. We found that the global median Nice from satellite observations is almost 2 times higher than the in situ median and increases slightly with decreasing temperature. Nice medians of the most frequently occurring cirrus sorted by geographical regions are highest in the tropics, followed by austral and boreal midlatitudes, Antarctica, and the Arctic. Since the satellite climatologies enclose the entire spatial and temporal Nice occurrence, we could deduce that half of the cirrus are located in the lowest, warmest (224–242 K) cirrus layer and contain a significant amount of liquid-origin cirrus. A specific highlight of the study is the in situ observations of cirrus and humidity in the Asian monsoon anticyclone and the comparison to the surrounding tropics. In the convectively very active Asian monsoon, peak values of Nice and IWC of 30 cm−3 and 1000 ppmv are detected around the cold point tropopause (CPT). Above the CPT, ice particles that are convectively injected can locally add a significant amount of water available for exchange with the stratosphere. We found IWCs of up to 8 ppmv in the Asian monsoon in comparison to only 2 ppmv in the surrounding tropics. Also, the highest RHice values (120 %–150 %) inside of clouds and in clear sky are observed around and above the CPT. We attribute this to the high H2O mixing ratios (typically 3–5 ppmv) observed in the Asian monsoon compared to 1.5 to 3 ppmv found in the tropics. Above the CPT, supersaturations of 10 %–20 % are observed in regions of weak convective activity and up to about 50 % in the Asian monsoon. This implies that the water available for transport into the stratosphere might be higher than the expected saturation value.

[1] Significant production of HONO was observed on glass sample manifold wall surface when exposed to sunlight during the PROPHET 2000 summer measurement intensive. It is hypothesized that the artifact HONO was produced by photolysis of adsorbed nitric acid/nitrate on the manifold wall surfaces followed by the subsequent reaction of produced NO 2 and adsorbed H 2 O on surface. This observation suggests against the use of an unshielded glass manifold as a sampling inlet for the measurement of atmospheric HONO. It may also have some implications in interpreting field NO x data measured using similar glass inlet manifolds, especially from the clean remote environments where NO x is low and HNO 3 is a major fraction of NO y .

An enhanced aerosol layer near the tropopause over Asia during the June-September period of the Asian summer monsoon (ASM) was recently identified using satellite observations. Its sources and climate impact are presently not well-characterized. To improve understanding of this phenomenon, we made in situ aerosol measurements during summer 2015 from Kunming, China, then followed with a modeling study to assess the global significance. The in situ measurements revealed a robust enhancement in aerosol concentration that extended up to 2 km above the tropopause. A climate model simulation demonstrates that the abundant anthropogenic aerosol precursor emissions from Asia coupled with rapid vertical transport associated with monsoon convection leads to significant particle formation in the upper troposphere within the ASM anticyclone. These particles subsequently spread throughout the entire Northern Hemispheric (NH) lower stratosphere and contribute significantly (∼15%) to the NH stratospheric column aerosol surface area on an annual basis. This contribution is comparable to that from the sum of small volcanic eruptions in the period between 2000 and 2015. Although the ASM contribution is smaller than that from tropical upwelling (∼35%), we find that this region is about three times as efficient per unit area and time in populating the NH stratosphere with aerosol. With a substantial amount of organic and sulfur emissions in Asia, the ASM anticyclone serves as an efficient smokestack venting aerosols to the upper troposphere and lower stratosphere. As economic growth continues in Asia, the relative importance of Asian emissions to stratospheric aerosol is likely to increase.