Concentrations and isotope ratios of helium and other noble gases in the   Earth's atmosphere during 1978-2011
  The evolution of the atmospheric noble gas composition during the past few decades has hardly been studied because, in contrast to many other atmospheric gases, systematic time-series measurements have not been available. Based on theoretical considerations, the atmospheric noble gas isotope composition is assumed to be stable on time scales of up to about 10^6 years, with the potential exception of anthropogenic changes predicted for the He concentration and the 3He/4He ratio. However, experimental assessments of the predicted changes in the atmospheric He isotope composition are controversial. To empirically test these assumptions and predictions, we analysed the noble gas isotope composition in samples of the Cape Grim Air Archive, a well-defined archive of marine boundary layer air in the southern hemisphere. The resulting time series of the 20Ne, 40Ar, 86Kr and 136Xe concentrations and 20Ne/22Ne and 40Ar/36Ar ratios during 1978-2011 demonstrate the stability of the atmospheric Ne, Ar, Kr and Xe composition during this time interval. The He isotope data provide strong evidence for a decrease in the 3He/4He during the same time interval at a mean rate of 0.23-0.30 permil per year. This result is consistent with most model predictions of the rate of decrease in the atmospheric 3He/4He ratio associated with mining and burning of fossil fuels. 
Matthias S. Brennwald, Nadia Vogel, Simon Figura, Martin K. Vollmer,   Ray Langenfelds, L. Paul Steele, Rolf Kipfer
physics.ao-ph physics.geo-ph