Intercomparison between Aura MLS and ground-based millimeter-wave observations of stratospheric O3 and HNO3 from Thule (76.5° N, 68.7° W)

Abstract

The Ground-Based Millimeter-wave Spectrometer (GBMS) measures rotational emission spectra of middle atmospheric trace gases, with a spectral window of 600 MHz tunable between approximately 230 and 280 GHz and a resolution of up to 65 kHz. It was designed and built at the State University of New York at Stony Brook in the early 90’s and since then has been regularly upgraded and operated at a variety of sites in both hemispheres, at polar and mid-latitudes. In view of a growing need for long-term data sets of stratospheric constituents, in January 2009 we resolved to establish a long-term GBMS observation site at the Arctic station of Thule Air Base (76.5°N, 68.8°W), Greenland, in order to track the long- and short-term interactions between the changing climate and the seasonal processes tied to the ozone depletion phenomenon. Since then three winter campaigns were carried out from Thule during the period January-March 2009, 2010 and 2011. Observations of O3, HNO3, CO and N2O were performed, mostly on a daily basis, except during periods characterized by poor weather conditions. In this study we compare GBMS stratospheric O3 and HNO3 measurements obtained during these three winter periods at Thule with colocated satellite observations from the Aura Microwave Limb Sounder (MLS) experiment. The Version 3.3 Aura MLS O3 and HNO3 data sets have a resolution of about 2.5 km and 3-4 km, respectively, in the stratosphere. The MLS precisions range from 0.1 to 0.6 ppmv for O3 and about 0.6-0.7 ppbv for HNO3 throughout the stratosphere. Based on preliminary comparisons with correlative data sets and on results obtained for v2.2, systematic uncertainties are estimated to lead to HNO3 measurements biases that vary between ±0.5 and ±2 ppbv and multiplicative errors of ±5 –15% throughout most of the stratosphere. Similarly, a systematic uncertainty of the order of 5-10% has been assessed for O3 data. As for the GBMS, the O3 pure rotational transition line at 276.923 GHz is observed with a ~1.5-hour integration, while the weaker HNO3 spectrum, represented by a cluster of superimposed emission lines centered at 269.1 GHz, needs about 4 hours of integration. Taking advantage of the dependence of the line broadening on atmospheric pressure, inversion techniques allow the retrieval of vertical profiles from approximately 15 to 50 km. In the past, GBMS O3 and HNO3 spectra were deconvolved using a Chahine-Twomey (C-T) and an iterative constrained Matrix Inversion (MI) technique, respectively. More recently, the GBMS retrieval algorithm has been updated to an Optimal Estimation Method (OEM) in order to conform to the standard of the NDACC microwave group, and to easily provide retrievals with a set of averaging kernels that grants more straightforward comparisons with other data sets. The nominal vertical resolution of the retrieved profiles (defined as the FWHM of averaging kernels) is ~8 km for O3 and ~ 12 km for HNO3, although the inversion technique locates the maximum of the mixing ratio profile of both species with a much better accuracy (i.e., ~ ±1 km). The 1σ uncertainty of O3 and HNO3 mixing ratio vertical profiles depends on altitude and is estimated at ~15% or 0.3 ppbv, whichever is larger. Each GBMS profile is compared to the closest MLS profile, with coincidence criteria of ±10° longitude, ±2.5° latitude and ±12 h. In order to avoid of severely compromising the comparison between GBMS and Aura MLS observations due to the much higher resolution of the satellite-derived data sets, we ‘convolved’ the MLS profiles using the GBMS averaging kernels before directly comparing the two data sets. For both species a fairly good agreement between MLS and GBMS profiles is observed, with the GBMS showing, however, a ~10-15% low bias at the mixing ratio peak