ALBERT

Description: There is considerable uncertainty as to whether interannual variability in climate and terrestrial ecosystem production is sufficient to explain observed variation in atmospheric carbon content over the past 20-30 years. In this paper, we investigated the response of net CO2 exchange in terrestrial ecosystems to interannual climate variability (1983 to 1988) using global satellite observations as drivers for the NASA-CASA (Carnegie-Ames-Stanford Approach) simulation model. This computer model of net ecosystem production (NEP) is calibrated for interannual simulations driven by monthly satellite vegetation index data (NDVI) from the NOAA Advanced Very High Resolution Radiometer (AVHRR) at 1 degree spatial resolution. Major results from NASA-CASA simulations suggest that from 1985 to 1988, the northern middle-latitude zone (between 30 and 60 degrees N) was the principal region driving progressive annual increases in global net primary production (NPP; i.e., the terrestrial biosphere sink for carbon). The average annual increase in NPP over this predominantly northern forest zone was on the order of +0.4 Pg (10 (exp 15) g) C per year. This increase resulted mainly from notable expansion of the growing season for plant carbon fixation toward the zonal latitude extremes, a pattern uniquely demonstrated in our regional visualization results. A net biosphere source flux of CO2 in 1983-1984, coinciding with an El Nino event, was followed by a major recovery of global NEP in 1985 which lasted through 1987 as a net carbon sink of between 0.4 and 2.6 Avg C per year. Analysis of model controls on NPP and soil heterotrophic CO2 fluxes (Rh) suggests that regional warming in northern forests can enhance ecosystem production significantly. In seasonally dry tropical zones, periodic drought and temperature drying effects may carry over with at least a two-year lag time to adversely impact ecosystem production. These yearly patterns in our model-predicted NEP are consistent in magnitude with the estimated exchange of CO2 by the terrestrial biosphere with the atmosphere, as determined by previous isotopic (delta (sup 13 C) convolution analysis. Ecosystem simulation results can help further target locations where net carbon sink fluxes have occurred in the past or may be verified in subsequent field studies.

Description: Large uncertainties in the effects that aerosols have on climate require improved in-situ measurements of extinction coefficient and single-scattering albedo. This abstract describes the use of continuous wave cavity ring-down (CW-CRD) technology to address this problem. The innovations in this instrument are the use of CW-CRD to measure aerosol extinction coefficient, the simultaneous measurement of scattering coefficient, and small size suitable for a wide range of aircraft applications. Our prototype instrument measures extinction and scattering coefficient at 690 nm and extinction coefficient at 1550 nm. The instrument itself is small (60 x 48 x 15 cm) and relatively insensitive to vibrations. The prototype instrument has been tested in our lab and used in the field. While improvements in performance are needed, the prototype has been shown to make accurate and sensitive measurements of extinction and scattering coefficients. Combining these two parameters, one can obtain the single-scattering albedo and absorption coefficient, both important aerosol properties. The use of two wavelengths also allows us to obtain a quantitative idea of the size of the aerosol through the Angstrom exponent. Minimum sensitivity of the prototype instrument is 1.5 x 10(exp -6)/m (1.5/Mm). Validation of the measurement of extinction coefficient has been accomplished by comparing the measurement of calibration spheres with Mie calculations. This instrument and its successors have potential to help reduce uncertainty currently associated with aerosol optical properties and their spatial and temporal variation. Possible applications include studies of visibility, climate forcing by aerosol, and the validation of aerosol retrieval schemes from satellite data.

Description: A better knowledge of PSC composition and formation mechanisms is important to better understand and predict stratospheric ozone depletion. Several past studies have attempted to compare modeling results with satellite observations. These comparisons have concentrated on case studies. In this paper we adopt a statistical approach. POAM PSC observations from several Arctic winters are categorized into Type Ia and Ib PSCs using a technique based on Strawa et al. The discrimination technique has been modified to employ the wavelengths dependence of the extinction signal at all wavelengths rather than only at 603 and 10 18 nm. Winter-long simulations for the 1999-2000 Arctic winter have been made using the IMPACT model. These simulations have been constrained by aircraft observations made during the SOLVE/THESEO 2000 campaign. A complete set of winter-long simulations was run for several different microphysical and PSC formation scenarios. The simulations give us perfect knowledge of PSC type (Ia, Ib, or II), composition, especially condensed phase HNO3 which is important for denitrification, and condensed phase H2O. Comparisons are made between the simulation and observation of PSC extinction at 1018 rim versus wavelength dependence, winter-long percentages of Ia and Ib occurrence, and temporal and altitude trends of the PSCs. These comparisons allow us to comment on how realistic some modeling scenarios are.

Description: Winter-long simulations of the 1999-2000 winter using a coupled microphysical/chemical model have been carried out to explore how PSC microphysics affects ozone loss. Although many models assures that water ice formation leads to denitrification, these simulations show that observed characteristics of the 1999-2000 winter can not be reproduced by such a denitrification mechanism. Instead, denitrification observations are best reproduced by a small number of particles freezing at temperatures near the nitric acid trihydration condensation point. Implications of such a mechanism for assessments of future ozone loss will be discussed. The simulations have also revealed that ozone loss during the 1999-2000 winter was sensitive to chlorine reactivation that occurred during February. Uncertainties in PSC microphysics and heterogeneous reaction rates both influence the modelled chlorine reactivation. For the 1999-2000 winter, these uncertainties have a larger effect on model ozone loss than denitrification. The role of denitrification would have increased if the Arctic vortex had persisted for a longer period.

Description: Interest in the distribution of black carbon (soot) aerosol (BCA) in the atmosphere is based on the following: (1) Because BCA has the highest absorption cross section of any compound know, it can absorb solar radiation to cause atmospheric warming; (2) Because BCA is a strong adsorber of gases, it can catalyze heterogeneous chemical reactions to modify the chemical composition of the atmosphere; (3) If aircraft emission is the major source of BCA, it can serve as an atmospheric tracer of aircraft exhaust. We collect BCA particles as small as 0.02 micrometers by wires mounted on both the DC-8 and ER-2 aircraft. After return to the laboratory, the wires are examined with a field emission scanning electron microscope to identify BCA particles by their characteristics morphology, Typically, BCA exists in the atmosphere as small particles of complex morphology. The particle sizes at the source are measured in tens of Angstrom units; after a short residence time in the atmosphere, individual particles coalesce to loosely packed agglomerates of typical dimensions 0.01 to 0.1 micrometer. We approximate the size of each BCA aggregate by that of a sphere of equivalent volume. This is done by computing the volume of a sphere whose diameter is the mean between averaged minimum and maximum dimensions of the BCA particle. While this procedure probably underestimates the actual surface area, it permits us to compare BCA size distributions among themselves and with other types of aerosols.

Description: The Alpha Jet Atmospheric eXperiment (AJAX) has been flying a scientific payload since January 2011 measuring ozone, carbon dioxide, methane, formaldehyde and meteorological parameters up to 9 kilometers. AJAX is located and operated from the San Francisco Bay Area and has flown a total of 229 flights, on a regular basis (approximately 3 per month) over all seasons cataloguing a long-term record of trace gas concentrations over California and Nevada. The AJAX project focuses on science questions which benefit from routine, frequent observations with flexible scheduling. This presentation will provide an overview of AJAX activities including a discussion of airborne measurements for: Long-Range Transport (LRT) and Stratosphere-to-Troposphere Transport (STT). Regular sampling by AJAX has aided identification of LRT and evidence of STT, which during spring and summer months are visible as elevated O3 laminae within airborne profiles. Some laminae have the ability to impact surface level air quality; Satellite validation - Regular AJAX missions include flights to Railroad Valley, NV in coordination with GOSAT (Greenhouse Gases Observing Satellite) and OCO-2 (Carbon Observatory-2) observations, and more recently to provide coincident measurements under TROPOMI (TROPOspheric Monitoring Instrument); The AJAX project is uniquely flexible to incorporate specialized flights with limited planning notice, such as sampling emissions from California wildfires. Nine wildfires have been sampled, with some more than once allowing to observe emission changes as the fire progresses; Pandora validation - Future work will include development of flight strategies for validation of ground based Pandora spectrometers.

Description: The process of supercooled liquid water crystallization into ice is still not well understood. Current experimental data on homogeneous freezing rates of ice nucleation in supercooled water droplets show considerable scatter. For example, at -33 C, the reported freezing nucleation rates vary by as much as 5 orders of magnitude, which is well outside the range of measurement uncertainties. Until now, experimental data on the freezing of supercooled water has been analyzed under the assumption that nucleation of ice took place in the interior volume of a water droplet. Here, the same data is reanalyzed assuming that the nucleation occurred "pseudoheterogeneously" at the air (or oil)-liquid water interface of the droplet. Our analysis suggest that the scatter in the nucleation data can be explained by two main factors. First, the current assumption that nucleation occurs solely inside the volume of a water droplet is incorrect. Second, because the nucleation process most likely occurs on the surface, the rates of nuclei formation could differ vastly when oil or air interfaces are involved. Our results suggest that ice freezing in clouds may initiate on droplet surfaces and such a process can allow for low amounts of liquid water (approx. 0.002 g per cubic meters) to remain supercooled down to -40 C as observed in the atmosphere.

Description: During the 1999-2000 Arctic winter, the SAGE (Stratospheric Aerosol and Gas Experiment) III Ozone Loss and Validation Experiment (SOLVE) provided evidence of widespread solid-phase polar stratospheric clouds (PSCs) accompanied by severe nitrification. Previous simulations have shown that a freezing process occurring at temperatures above the ice frost point is necessary to explain these observations. In this work, the nitric acid freezing rates measured by Salcedo et al. and discussed by Tabazadeh et al. have been examined. These freezing rates have been tested in winter-long microphysical simulations of the 1999-2000 Arctic vortex evolution in order to determine whether they can explain the observations. A range of cases have been explored, including whether the PSC particles are composed of nitric acid dihydrate or trihydrate, whether the freezing process is a bulk process or occurs only on the particle surfaces, and uncertainties in the derived freezing rates. Finally, the possibility that meteoritic debris enhances the freezing rate has also been examined. The results of these simulations have been compared with key PSC and denitrification measurements made by the SOLVE campaign. The cases that best reproduce the measurements will he highlighted, with a discussion of the implications for our understanding of PSCs.

Description: A combination of CN counts, Ames wire impactor size analyses and optical particle counter data in aircraft exhaust results in a continuous particle size distribution between 0.01 micrometer and 1 micrometer particle radius sampled in the exhaust of a Boeing 757 research aircraft. The two orders of magnitude size range covered by the measurements correspond to 6-7 orders of magnitude particle concentration. CN counts and small particle wire impactor data determine a nucleation mode, composed of aircraft-emitted sulfuric acid aerosol, that contributes between 62% and 85% to the total aerosol surface area and between 31% and 34% to its volume. Soot aerosol comprises 0.5% of the surface area of the sulfuric acid aerosol. Emission indices are: EIH2SO4 = 0.05 g/kgFUEL and (0.2-0.5) g/kgFUEL (for 75 ppmm and 675 ppmm fuel-S, respectively), 2.5E4〈EISOOT〈1.3E-3 g/kgFUEL, and EICN 8E14 and 1.3E16 particles/kgFUEL (for 75 and 675 ppmm fuel-S). The sulfur (gas) to H2SO4 (particle) conversion efficiency is between 10% and 25%.

Description: Soot aerosol from aircraft has been implicated to cause long-term ozone depletion at mid-latitudes in the lower stratosphere at a rate of approx. equals 5%,per decade. During the 1996 SUCCESS field campaign, we sampling aerosols in the exhaust wake of a Boeing 757 aircraft and determined emission indices for sulfuric acid (EIH2SO4=4.8E-2 and 5.7E- 1. g/kgFUEL for 75 and 675 ppm fuel-sulfur, respectively) and soot (EIsoot=7.5E-4 g/kgFUEL). The corresponding fuel-sulfur to H2SO4 conversion efficiency was 25 % and 30%,respctively. Applying the H2SO4 emission index to the 1990 fuel by the world's commercial fleets of 1.3E11 kg, a conversion efficiency of 30% would have led to an annual contribution to the atmospheric sulfur budget by aircraft of 2.E7 kg H2SO4, if the fuels averaged 500 ppmm.The soot emission index given above yielded a 1990 injection of soot aerosol by aircraft of 1.E5 kg. Thus, soot amounts to only one half of one percent of the aerosol generated by aircraft. The fractal nature of soot may increase its actual surface area by about a factor of 10. The findings, however, of (1) stratospheric soot loadings commensurate with aircraft fuel consumption, based on the emission index given above and the assumption of stratospheric residence times of the order of one year; and (2) a trend in stratospheric soot loading of approx.6% per year since 1981, similar to the annual increase of aircraft operations since that time, implicate aircraft as stratospheric polluters. A trend similar to soot of H2SO4 aerosol loading could not be deciphered, neither from in situ measurements nor SAGE II extinction, against the "noise" due to volcanic eruptions, The current single scatter albedo of the stratospheric aerosol is omega = 0.993+/-0.004.