Radon (222Rn) is a powerful natural tracer of mixing and exchange processes in the atmospheric boundary layer. The authors present and discuss the main features of a unique dataset of 50 high-resolution vertical radon profiles up to 3500 m above ground level, obtained in clear and cloudy daytime terrestrial boundary layers over an inland rural site in Australia using an instrumented motorized research glider. It is demonstrated that boundary layer radon profiles frequently exhibit a complex layered structure as a result of mixing and exchange processes of varying strengths and extents working in clear and cloudy conditions within the context of the diurnal cycle and the synoptic meteorology. Normalized aircraft radon measurements are presented, revealing the characteristic structure and variability of three major classes of daytime boundary layer: 1) dry convective boundary layers, 2) mixed layers topped with residual layers, and 3) convective boundary layers topped with coupled nonprecipitating clouds. Robust and unambiguous signatures of important atmospheric processes in the boundary layer are identifiable in the radon profiles, including “top-down” mixing associated with entrainment in clear-sky cases and strongly enhanced venting and subcloud-layer mixing when substantial active cumulus are present. In poorly mixed conditions, radon gradients in the daytime atmospheric surface layer significantly exceed those predicted by Monin–Obukhov similarity theory. In two case studies, it is demonstrated for the first time that a sequence of vertical radon profiles measured over the course of a single day can consistently reproduce major structural features of the evolving boundary layer.

Radon is increasingly being used as a tool for quantifying stability influences on urban pollutant concentrations. Bulk radon gradients are ideal for this purpose, since the vertical differencing substantially removes contributions from processes on timescales greater than diurnal and (assuming a constant radon source) gradients are directly related to the intensity of nocturnal mixing. More commonly, however, radon measurements are available only at a single height. In this study we argue that single-height radon observations should not be used quantitatively as an indicator of atmospheric stability without prior conditioning of the time series to remove contributions from larger-scale "non-local" processes. We outline a simple technique to obtain an approximation of the diurnal radon gradient signal from a single-height measurement time series, and use it to derive a four category classification scheme for atmospheric stability on a "whole night" basis. A selection of climatological and pollution observations in the Sydney region are then subdivided according to the radon-based scheme on an annual and seasonal basis. We compare the radon-based scheme against a commonly used Pasquill–Gifford (P–G) type stability classification and reveal that the most stable category in the P–G scheme is less selective of the strongly stable nights than the radon-based scheme; this lead to significant underestimation of pollutant concentrations on the most stable nights by the P–G scheme. Lastly, we applied the radon-based classification scheme to mixing height estimates calculated from the diurnal radon accumulation time series, which provided insight to the range of nocturnal mixing depths expected at the site for each of the stability classes.

Two-point radon gradients provide a direct, unambiguous measure of near-surface atmospheric mixing. A 31-month data set of hourly radon measurements at 2 and 50 m is used to characterize the season...

A time-dependent map of radon-222 flux density at the Australian land surface has been constructed with a spatial resolution of 0.05° and temporal resolution of one month. Radon flux density was calculated from a simple model utilising data from national gamma-ray aerial surveys; modelled soil moisture, available from 1900 in near real-time; and maps of soil properties. The model was calibrated against a data set of accumulation chamber measurements, thereby constraining it with experimental data. A notable application of the map is in atmospheric mixing and transport studies which use radon as a tracer, where it is a clear improvement on the common assumption of uniform radon flux density.

Vertical mixing of the nocturnal stable boundary layer (SBL) over a complex land surface is investigated for a range of stabilities, using a decoupling index (\(0 < D_{rb} < 1\)) based on the 2–50 m bulk gradient of the ubiquitous natural trace gas radon-222. The relationship between \(D_{rb}\) and the bulk Richardson number (\(R_{ib}\)) exhibits three broad regions: (1) a well-mixed region (\(D_{rb} \approx 0.05\)) in weakly stable conditions (\(R_{ib} < 0.03\)); (2) a steeply increasing region (\(0.05 < D_{rb} < 0.9\)) for “transitional” stabilities (\(0.03 < R_{ib} < 1\)); and (3) a decoupled region (\(D_{rb} \approx 0.9\)–1.0) in very stable conditions (\(R_{ib} > 1\)). \(D_{rb}\) exhibits a large variability within individual \(R_{ib}\) bins, however, due to a range of competing processes influencing bulk mixing under different conditions. To explore these processes in \(R_{ib}\)–\(D_{rb}\) space, we perform a bivariate analysis of the bulk thermodynamic gradients, various indicators of external influences, and key turbulence quantities at 10 and 50 m. Strong and consistent patterns are found, and five distinct regions in \(R_{ib}\)–\(D_{rb}\) space are identified and associated with archetypal stable boundary-layer regimes. Results demonstrate that the introduction of a scalar decoupling index yields valuable information about turbulent mixing in the SBL that cannot be gained directly from a single bulk thermodynamic stability parameter. A significant part of the high variability observed in turbulence statistics during very stable conditions is attributable to changes in the degree of decoupling of the SBL from the residual layer above. When examined in \(R_{ib}\)–\(D_{rb}\) space, it is seen that very different turbulence regimes can occur for the same value of \(R_{ib}\), depending on the particular combination of values for the bulk temperature gradient and wind shear, together with external factors. Extremely low turbulent variances and fluxes are found at 50 m height when \(R_{ib} > 1\) and \(D_{rb} \approx 1\) (fully decoupled). These “quiescent” cases tend to occur when geostrophic forcing is very weak and subsidence is present, but are not associated with the largest bulk temperature gradients. Humidity and net radiation data indicate the presence of low cloud, patchy fog or dew, any of which may aid decoupling in these cases by preventing temperature gradients from increasing sufficiently to favour gravity wave activity. The largest temperature gradients in our dataset are actually associated with smaller values of the decoupling index (\(D_{rb} < 0.7\)), indicating the presence of mixing. Strong evidence is seen from enhanced turbulence levels, fluxes and submeso activity at 50 m, as well as high temperature variances and heat flux intermittencies at 10 m, suggesting this region of the \(R_{ib}\)–\(D_{rb}\) distribution can be identified as a top-down mixing regime. This may indicate an important role for gravity waves and other wave-like phenomena in providing the energy required for sporadic mixing at this complex terrain site.

We demonstrate the ability of atmospheric radon concentrations to reliably and unambiguously identify local and remote terrestrial influences on an air mass, and thereby the potential for alteration of trace gas composition by anthropogenic and biogenic processes. Based on high accuracy (lower limit of detection 10–40 mBq m–3), high temporal resolution (hourly) measurements of atmospheric radon concentration we describe, apply and evaluate a simple two-step method for identifying and characterising constituent mole fractions in baseline air. The technique involves selecting a radon-based threshold concentration to identify the “cleanest” (least terrestrially influenced) air masses, and then performing an outlier removal step based on the distribution of constituent mole fractions in the identified clean air masses. The efficacy of this baseline selection technique is tested at three contrasting WMO GAW stations: Cape Grim (a coastal low-altitude site), Mauna Loa (a remote high-altitude island site), and Jungfraujoch (a continental high-altitude site). At Cape Grim and Mauna Loa the two-step method is at least as effective as more complicated methods employed to characterise baseline conditions, some involving up to nine steps. While it is demonstrated that Jungfraujoch air masses rarely meet the baseline criteria of the more remote sites, a selection method based on a variable monthly radon threshold is shown to produce credible “near baseline” characteristics. The seasonal peak-to-peak amplitude of recent monthly baseline CO2 mole fraction deviations from the long-term trend at Cape Grim, Mauna Loa and Jungfraujoch are estimated to be 1.1, 6.0 and 8.1 ppm, respectively