Inferring Aerosol Properties from Space-Based Measurements: An Alternative to Direct Retrieval
No abstract available
Engineering topics
Publications and source records attributed to Deshler, Terry.
No abstract available
We present 20 years (1996-2015) of austral springtime measurements of chlorine monoxide (ClO) over Antarctica from the Chlorine Oxide Experiment (ChlOEl) ground-based millimeter wave spectrometer at Scott Base, Antarctica, as well 12 years (2004-2015) of ClO measurements from the Aura Microwave Limb Sounder (MLS). From August onwards we observe a strong increase in lower stratospheric ClO, with a peak column amount usually occurring in early September. From mid-September onwards we observe a strong decrease in ClO. In order to study interannual differences, we focus on a 3-week period from 28 August to 17 September for each year and compare the average column ClO anomalies. These column ClO anomalies are shown to be highly correlated with the average ozone mass deficit for September and October of each year. We also show that anomalies in column ClO are strongly anti-correlated with 30 hPa temperature anomalies, both on a daily and an interannual timescale. Making use of this anti-correlation we calculate the linear dependence of the interannual variations in column C1O on interannual variations in temperature. By making use of this relationship, we can better estimate the underlying trend in the total chlorine (Cl(sub y) = HCl + ClONO2 + HOCl + 2 x Cl2 + 2 x Cl2+ ClO + Cl). The resultant trends in Cl(sub y), which determine the long-term trend in ClO, are estimated to be -0.5 +/-0.2, -1.40.9, and -0.60.4% per year, for zonal MLS, Scott Base MLS (both 2004-2015), and ChlOE (1996-2015) respectively. These trends are within 1sigma of trends in stratospheric Cl(sub y) previously found at other latitudes. The decrease in ClO is consistent with the trend expected from regulations enacted under the Montreal Protocol.
Interest in stratospheric aerosol and its role in climate have increased over the last decade due to the observed increase in stratospheric aerosol since 2000 and the potential for changes in the sulfur cycle induced by climate change. This review provides an overview about the advances in stratospheric aerosol research since the last comprehensive assessment of stratospheric aerosol was published in 2006. A crucial development since 2006 is the substantial improvement in the agreement between in situ and space-based inferences of stratospheric aerosol properties during volcanically quiescent periods. Furthermore, new measurement systems and techniques, both in situ and space based, have been developed for measuring physical aerosol properties with greater accuracy and for characterizing aerosol composition. However, these changes induce challenges to constructing a long-term stratospheric aerosol climatology. Currently, changes in stratospheric aerosol levels less than 20% cannot be confidently quantified. The volcanic signals tend to mask any nonvolcanically driven change, making them difficult to understand. While the role of carbonyl sulfide as a substantial and relatively constant source of stratospheric sulfur has been confirmed by new observations and model simulations, large uncertainties remain with respect to the contribution from anthropogenic sulfur dioxide emissions. New evidence has been provided that stratospheric aerosol can also contain small amounts of nonsulfatematter such as black carbon and organics. Chemistry-climate models have substantially increased in quantity and sophistication. In many models the implementation of stratospheric aerosol processes is coupled to radiation and/or stratospheric chemistry modules to account for relevant feedback processes.
Satellite observations and numerical modeling studies have demonstrated that the Asian Summer Monsoon (ASM) can provide a conduit for gas-phase pollutants in south Asia to reach the lower stratosphere. Now, observations from the CALIPSO satellite have revealed the Asian Tropopause Aerosol Layer (ATAL), a summertime accumulation of aerosols associated with ASM anticyclone, in the upper troposphere and lower stratosphere (UTLS). The ATAL has potential implications for regional cloud properties, climate, and chemical processes in the UTLS. Here, we show in situ measurements from balloon-borne instrumentation, aircraft and satellite observations, combined with trajectory and chemical transport model (CTM) simulations to explore the origin, composition, physical and optical properties of aerosols in the ATAL. In particular, we show balloon-based observations from our BATAL-2015 field campaign to India and Saudi Arabia in summer 2015, including in situ backscatter measurements from COBALD instruments, and some of the first observations of size and volatility of aerosols in the ATAL layer using optical particle counters (OPCs). Back trajectory calculations initialized from CALIPSO observations point to deep convection over North India as a principal source of ATAL aerosols. Available aircraft observations suggest significant sulfur and carbonaceous contributions to the ATAL, which is supported by simulations using the GEOS-Chem CTM. Source elimination studies conducted with the GEOS-Chem indicate that 80-90% of ATAL aerosols originate from south Asian sources, in contrast with some earlier studies.
Stratospheric aerosol measurements from the University of Wyoming balloonborne optical particle counters (OPCs), the Stratospheric Aerosol and Gas Experiment (SAGE) II, and the Halogen Occultation Experiment (HALOE) were compared in the period 1982-2000, when measurements were available. The OPCs measure aerosol size distributions, and HALOE multiwavelength (2.45-5.26 micrometers) extinction measurements can be used to retrieve aerosol size distributions. Aerosol extinctions at the SAGE II wavelengths (0.386-1.02 micrometers) were computed from these size distributions and compared to SAGE II measurements. In addition, surface areas derived from all three experiments were compared. While the overall impression from these results is encouraging, the agreement can change with latitude, altitude, time, and parameter. In the broadest sense, these comparisons fall into two categories: high aerosol loading (volcanic periods) and low aerosol loading (background periods and altitudes above 25 km). When the aerosol amount was low, SAGE II and HALOE extinctions were higher than the OPC estimates, while the SAGE II surface areas were lower than HALOE and the OPCS. Under high loading conditions all three instruments mutually agree to within 50%.
The efforts envisioned within the original proposal (accepted February 1994) and the extension of this proposal (accepted February 1997) included measurement validations, the retrieval of aerosol size distributions and distribution moments, aerosol correction studies, and investigations of polar stratospheric clouds. A majority of the results from this grant have been published. The principal results from this grant are discussed.
A balloon-borne instrument was constructed for observations of vertical profiles of cloud condensation nucleus (CCN) concentrations, active at 1% supersaturation. Droplet concentration in the static thermal-gradient diffusion chamber is deduced from the amount of scattered laser light detected by a photodetector. The photodetector is calibrated using a video camera and computer system to count the number of droplets produced from NaCl aerosol. Preliminary data are available from nine early morning profiles obtained at Laramie, Wyoming, between June 1995 and January 1997. To complement the CCN measurements, instruments that measure condensation nuclei (CN) and aerosols with diameter greater than 0.30 micrometers (D(sub 0.3) were also included on the balloon package. CCN concentrations exhibited a general decrease from the surface to the top of the boundary layers, were generally uniform through well-mixed layers, and show variability above well-mixed layers. In general, the structure of the CCN profile appears to be closely related to the structure in the CN and D(sub 0.3) profiles. Summer profiles generally have CCN concentration greater than 200/cu cm up to 500 mbar, whereas winter profiles are less than 200/cu cm at all levels.
Throughout this study we focused on comparisons of CLAES and in situ measurements of ozone and aerosol extinction. Thus the comparison is between satellite data representative of large spatial regions and in situ data representative of nearly point samples. Both instruments provide vertical profiles, but the region of overlap is limited to between approximately 10 and 100 mb. CLAES Version 7 ozone measurements have been compared to electrochemical cell ozonesonde measurements over McMurdo Station, Antarctica (78 deg S, 167 deg E), Dumont d'Urville, Antarctica (66.7 deg S, 140 deg E), Laramie, Wyoming (41 deg N, 106 deg W), and Bear Island, Norway (74.3 deg N, 19 deg E). Comparisons were made between vertical ozone profiles, and between integrated column ozone over the region of overlap of the measurements. Comparisons using CLAES Version 8 data are underway. CLAES Version 8 aerosol extinction measurements at all wavelengths have also been compared to University of Wyoming aerosol extinctions over McMurdo Station, Antarctica, and over Laramie, Wyoming. Coincidences in all cases were determined by minimizing the distance between the CLAES observations and the surface station, and the time separation between the satellite and in situ measurements.
Vertical profiles of ozone and temperature have been measured at McMurdo Station, Antarctica, during the springs of 1986 to 1991, roughly every two days from 25 August to 31 October. Comparisons of temporal histories and average vertical structure for these years reveals some striking consistency in the ozone depletion process. Ozone depletion generally begins in early September, and with a half-life of 20-30 days, reaches its maximum in mid-October. The depletion occurs almost exclusively between 12 and 20 km. At the time of maximum depletion total ozone has been decreased roughly 40 percent while ozone between 12 and 20 km has been reduced 80 percent. Recovery generally begins in late October with the influx, above 20 km, of ozone rich air from the lower latitudes. From this record the worst years for ozone depletion were 1987, 1989, and 1990. A new region of ozone depletion, below 12 km, was observed in 1991, coinciding with the entrainment of a volcanic cloud into the polar vortex.
Atmospheric concentrations of contact-freezing nuclei were measured using a technique primarily sensitive to submicron aerosol particles. Diffusion and phoretic forces were relied on for the capture of nuclei by supercooled drops of distilled water exposed to the sample air. Nucleus concentrations were deduced from the rate at which the drops were observed to freeze, interpreting that rate on the basis of a theoretical prediction of aerosol capture rate for different assumed sizes of the nuclei. Measurements at Laramie, Wyoming, yielded average concentrations of contact-freezing nuclei of 1.7/L at -15 C and 3.1/L at -18 C for an assumed radius of 0.01 micron for the nucleating particles.
The results of six balloon flights at McMurdo Station, Antarctica, under varying temperature conditions, are used in a study of polar stratospheric clouds during Sept. 1989. A particle counter, with size resolution in the 0.5 micron radius region, indicates that cloud size distributions are always bimodal. Mode radii ranging from 0.05 to 0.10 microns were observed for the small particle mode, representing the sulfate layer or condensational growth enhancements of it. The data are not inconsistent with the expected increase in size with decreasing temperature of the small particle mode in the sulfate layer owing to deliquescence although this phenomenon is often masked by nitric acid trihydrate (NAT) condensation when temperatures are sufficiently low. Mode radii generally ranged from 1.5 to 3.5 micron for the large particle mode at concentrations 3 to 4 orders of magnitude lower than the small particle mode. The large particle mode, which normally comprises most of the mass, is presumably caused by NAT condensation on larger particles of the sulfate layer and indicates HNO3 mixing ratios of 1 to 5 ppbv for most of the cloud layers observed, suggesting substantial denitrification. On several occasions, distributions were observed with mode radii as high as 7 microns, and correspondingly large inferred mass, indicating water ice clouds in the 12 to 15 km region. On other occasions, absence of such clouds at very low temperatures indicated water vapor mixing ratios of less than 3 ppmv suggesting dehydration. Generally, the inferred HNO3 mixing ratios were higher in the lower stratosphere, suggesting redistribution through particle sedimentation.