First remote sensing observations of trifluoromethane (HFC-23) in the upper troposphere and lower stratosphere

摘要

This work reports the first remote sensing measurements of atmospheric HFC-23 (CHF_3) using solar occultation measurements made by the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) and the Jet Propulsion Laboratory Mark IV (MkIV) balloon interferometer. A total of 8809 ACE occultations measured between 2004 and 2010 have been processed, along with 24 MkIV occultations measured between 1989 and 2007. ACE data (yearly averages over the 10-25 km altitude range) in the tropics/subtropics (40°S-40°N) reveal a trend of 4.0 ± 1.6% per year in the growth of HFC-23 for 2004-2009 (or 3.9 ± 1.2% per year for 2004-2010), slightly smaller than surface measurements from Cape Grim air archive samples over the same time period (4.7 ± 0.3% per year). The northern midlatitude and high-latitude MkIV data (averaged over the 10-25 km altitude range) indicate a growth rate of 5.8 ± 0.3% per year over the period 1989-2007 (5.3 ± 0.4% per year for just the midlatitude data), similar to the Cape Grim surface trend of 5.7 ± 0.1% per year over the same period. The absolute HFC-23 volume mixing ratios measured by ACE and MkIV in the upper troposphere/lower stratosphere are in good agreement (<5% bias) with each other but are ～30% larger than ground-based measurements. The source of this bias has not been definitively ascertained; however, spectroscopic errors are the most likely cause.