Je. Mulquiney et al., A NEW INVERSE METHOD FOR TRACE GAS FLUX ESTIMATION - 2 - APPLICATION TO TROPOSPHERIC CFCL3 FLUXES, J GEO RES-A, 103(D1), 1998, pp. 1429-1442
An initial application of a new inverse method for the estimation of f
lux strengths of long-lived atmospheric trace gases is presented. CFCl
3 is studied using the Australian National University's Chemical Trans
port Model. Unit-pulse responses are derived from the model, and used
to identify a time-varying state-space model of tropospheric CFCl3. Th
is in turn is used in a Kalman filter to perform two input-estimation
studies. The first uses model generated measurements to estimate known
flux strengths. This demonstrates the robustness of the method, altho
ugh it is found that instantaneous stratospheric loss rates are not we
ll-estimated using only surface concentration measurements. Emissions
however, are robustly estimated. A time-averaged tropospheric lifetime
can be estimated however, with an accuracy of +/-5 years. Thirteen ye
ars of Atmospheric Lifetime Experiment/Global Atmospheric Gases Experi
ment CFCl3 measurements are used in the second flux estimation experim
ent. The estimated fluxes though are outside known physical limits for
CFCl3, and it is concluded that either a more accurate/appropriate tr
ansport model, or more measurement locations, are needed to obtain use
ful information regarding regional tropospheric CFCl3 fluxes.