T. D. Fairlie

Increase in upper tropospheric and lower stratospheric aerosol levels and its potential connection with Asian pollution

Satellite observations have shown that the Asian Summer Monsoon strongly influences the upper troposphere and lower stratosphere (UTLS) aerosol morphology through its role in the formation of the Asian Tropopause Aerosol Layer (ATAL). Stratospheric Aerosol and Gas Experiment II solar occultation and Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) lidar observations show that summertime UTLS Aerosol Optical Depth (AOD) between 13 and 18 km over Asia has increased by three times since the late 1990s. Here we present the first in situ balloon measurements of aerosol backscatter in the UTLS from Western China, which confirm high aerosol levels observed by CALIPSO since 2006. Aircraft in situ measurements suggest that aerosols at lower altitudes of the ATAL are largely composed of carbonaceous and sulfate materials (carbon/sulfur elemental ratio ranging from 2 to 10). Back trajectory analysis from Cloud-Aerosol Lidar with Orthogonal Polarization observations indicates that deep convection over the Indian subcontinent supplies the ATAL through the transport of pollution into the UTLS. Time series of deep convection occurrence, carbon monoxide, aerosol, temperature, and relative humidity suggest that secondary aerosol formation and growth in a cold, moist convective environment could play an important role in the formation of ATAL. Finally, radiative calculations show that the ATAL layer has exerted a short-term regional forcing at the top of the atmosphere of −0.1 W/m2 in the past 18 years. Key Points Increase of summertime upper tropospheric aerosol levels over Asia since the 1990s Upper tropospheric enhancement also observed by in situ backscatter measurements Significant regional radiative forcing of −0.1 W/m2

Comment on "Large Volcanic Aerosol Load in the Stratosphere Linked to Asian Monsoon Transport"

Bourassa et al. (Reports, 6 July 2012, p. 78) have suggested that deep convection associated with the Asian monsoon played a critical role in transporting sulfur dioxide associated with the Nabro volcanic eruption (13 June 2011) from the upper troposphere (9 to 14 kilometers) into the lower stratosphere. An analysis of the CALIPSO lidar data indicates, however, that the main part of the Nabro volcanic plume was injected directly into the lower stratosphere during the initial eruption well before reaching the Asian monsoon deep convective region.

Large‐scale chemical evolution of the Arctic vortex during the 1999/2000 winter: HALOE/POAM III Lagrangian photochemical modeling for the SAGE III—Ozone Loss and Validation Experiment (SOLVE) campaign

Abstract : The LaRC Lagrangian Chemical Transport Model (LaRC LCTM) is used to simulate the kinematic and chemical evolution of an ensemble of trajectories initialized from Halogen Occultation Experiment (HALOE) and Polar Ozone and Aerosol Measurement (POAM) III atmospheric soundings over the SAGE III-Ozone Loss and Validation Experiment (SOLVE) campaign period. Initial mixing ratios of species which are not measured by HALOE or POAM III are specified using sunrise and sunset constituent CH(4) and constituent PV regressions obtained from the LaRC IMPACT model, a global three dimensional general circulation and photochemical model. Ensemble averaging of the trajectory chemical characteristics provides a vortex-average perspective of the photochemical state of the Arctic vortex. The vortex-averaged evolution of ozone, chlorine, nitrogen species, and ozone photochemical loss rates is presented. Enhanced chlorine catalyzed ozone loss begins in mid-January above 500 K, and the altitude of the peak loss gradually descends during the rest of the simulation. Peak vortex averaged loss rates of over 60 ppbv/day occur in early March at 450 K. Vortex averaged loss rates decline after mid- March. The accumulated photochemical ozone loss during the period from 1 December 1999 to 30 March 2000 peaks at 450 K with net losses of near 2.2 ppmv. The predicted distributions of CH4, O(3), denitrification, and chlorine activation are compared to the distributions obtained from in situ measurements to evaluate the accuracy of the simulations. The comparisons show best agreement when diffusive tendencies are included in the model calculations, highlighting the importance of this process in the Arctic vortex. Sensitivity tests examining the large-scale influence of orographically generated gravity wave temperature anomalies are also presented. Results from this sensitivity study show that mountain-wave temperature perturbations contribute an additional 2-8% O(3) loss during the 1999/2000 winter.