Abstract

We introduce a tool to determine surface fluxes from atmospheric concentration data in the midst of distributed sources or sinks over land, the Stochastic Time‐Inverted Lagrangian Transport (STILT) model, and illustrate the use of the tool with CO 2 data over North America. Anthropogenic and biogenic emissions of trace gases at the surface cause large variations of atmospheric concentrations in the planetary boundary layer (PBL) from the “near field,” where upstream sources and sinks have strong influence on observations. Transport in the near field often takes place on scales not resolved by typical grid sizes in transport models. STILT provides the capability to represent near‐field influences, transforming this noise to signal useful in diagnosing surface emissions. The model simulates transport by following the time evolution of a particle ensemble, interpolating meteorological fields to the subgrid scale location of each particle. Turbulent motions are represented by a Markov chain process. Significant computational savings are realized because the influence of upstream emissions at different times is modeled using a single particle simulation backward in time, starting at the receptor and sampling only the portion of the domain that influences the observations. We assess in detail the physical and numerical requirements of STILT and other particle models necessary to avoid inconsistencies and to preserve time symmetry (reversibility). We show that source regions derived from backward and forward time simulations in STILT are similar, and we show that deviations may be attributed to violation of mass conservation in currently available analyzed meterological fields. Using concepts from information theory, we show that the particle approach can provide significant gains in information compared to conventional gridcell models, principally during the first hours of transport backward in time, when PBL observations are strongly affected by surface sources and sinks.