Gaseous elemental mercury depletion events observed at Cape Point during 2007–2008

Gaseous mercury in the marine boundary layer has been measured with a 15 min temporal resolution at the Global Atmosphere Watch station Cape Point since March 2007. The most prominent features of the data until July 2008 are the frequent occurrences of pollution (PEs) and depletion events (DEs). Both types of events originate mostly within a short transport distance (up to about 100 km), which are embedded in air masses ranging from marine background to continental. The Hg/CO emission ratios observed during the PEs are within the range reported for biomass burning and industrial/urban emissions. The depletion of gaseous mercury during the DEs is in many cases almost complete and suggests an atmospheric residence time of elemental mercury as short as a few dozens of hours, which is in contrast to the commonly used estimate of approximately 1 year. The DEs observed at Cape Point are not accompanied by simultaneous depletion of ozone which distinguishes them from the halogen driven atmospheric mercury depletion events (AMDEs) observed in Polar Regions. Nonetheless, DEs similar to those observed at Cape Point have also been observed at other places in the marine boundary layer. Additional measurements of mercury speciation and of possible mercury oxidants are hence called for to reveal the chemical mechanism of the newly observed DEs and to assess its importance on larger scales

ATMOSPHERIC MERCURY MEASUREMENTS AT CAPE POINT, SOUTH AFRICA

Over the 1995-2009 period the gaseous elemental mercury (GEM) concentrations have decreased by about 0.04 ng m-3 yr-1 -at Cape Point (CPT). A reduction of the same magnitude is indicated by measurements during intermittent ship cruises, implying a homogeneous distribution of GEM concentrations in the Southern Hemisphere (SH) and a 30% reduction of its atmospheric burden. Almost all GEM measurements in the Northern Hemisphere (NH) point to a substantial decrease but the trends are inhomogeneous, most likely due to a variable source distribution. However, measurements in the NH during ship cruises suggest a trend of similar magnitude. A decrease in the total atmospheric GEM burden by about 30% is inconsistent with the current mercury budgets. The most probable explanation for this is subsiding re-emissions from the legacy of large past emissions. High-resolution data since 2007 revealed depletion (DES) as well as pollution events (PEs). Both types are embedded in air masses ranging from marine background to continental. The DES observed at Cape Point are a local phenomenon (<100 km) and are the first mercury depletion events reported outside the Polar Regions. In contrast to polar DES, the DES at CPT are not accompanied by concurrent O3 depletion. They mostly appear at wind speeds < 10 m s-1 and their predominating occurrence between 11 and 18 hours suggests a photochemical destruction mechanism which could not be explained yet. GEM correlates with CO, C02, and CH4 during most PES at CPT (GEM levels > 1.3 ng m-3) and with 222Rn during about half the events. Most of the observed GEM/CO emission ratios are within the range bracketed by values reported for biomass burning and industrial/urban emissions, thus suggesting a mixture of both. No significant differences of GEM/CO and GEM/C02 could be found between different source regions defined by backward trajectories. This implies that exceptionally high emissions ascribed to the Gauteng region in global mercury inventories are overestimated

Comparison of SST diurnal variation models over the Tropical Warm Pool region

Four sea surface temperature (SST) diurnal variation (DV) models have been compared against Multi-functional Transport Satellite - 1R (MTSAT-1R) SST measurements over the Tropical Warm Pool region (TWP, 90°E-170°E, 25°S-15°N) for four months from January to April 2010. The four models include one empirical model formulated by Chelle Gentemann (hereafter CG03), one physical model proposed by Zeng and Beljaars in 2005 (ZB05) and its updated version (ZB+T), and one air-sea coupled model (the Met Office Unified Model Global Coupled configuration 2, GC2) with ZB05 warm layer scheme added on top of the standard configuration. The sensitivity of the v3 MTSAT-1R data to the “true” changes in SST is first investigated using drifting buoys and is estimated to be 0.60 ± 0.05. This being significantly different from 1, the models are validated against MTSAT-1R data and the same data scaled by the inverse of the sensitivity (representing an estimate of the true variability). Results indicate that all models are able to capture the general DV patterns but with differing accuracies and features. Specifically, CG03 and ZB+T underestimate strong (> 2 K) DV events’ amplitudes especially if we assume that sensitivity-scaled MTSAT-1R variability is most realistic. ZB05 can effectively capture the DV cycles under most DV and wind conditions, as well as the DV spatial distribution. GC2 tends to overestimate small-moderate (< 2 K) DV events but can reasonably predict large DV events. 1-3 hr lags in warming start and peak times are found in GC2

Relationships Between Giant Sea Salt Particles and Clouds Inferred from Aircraft Physicochemical Data

This study uses airborne data from multiple field campaigns off the California coast to determine the extent to which a size distribution parameter and a cloud water chemical measurement can capture the effect of giant cloud condensation nuclei (GCCN), specifically sea salt, on marine stratocumulus cloud properties. The two GCCN proxy variables, near-surface particle number concentration for diameters > 5 µm and cloud water chloride concentration, are significantly correlated (95% confidence) with each other, and both exhibit expected relationships with other parameters (e.g., surface wind) that typically coincide with sea salt emissions. Factors influencing the relationship between these two GCCN proxy measurements include precipitation rate (R) and the standard deviation of the sub-cloud vertical velocity owing likely to scavenging effects and improved mixing/transport of sea salt to cloud base, respectively. When comparing twelve pairs of high and low chloride cloud cases (at fixed liquid water path and cloud drop number concentration), the average drop spectra for high chloride cases exhibit enhanced drop number at diameters exceeding 20 µm, especially above 30 µm. In addition, high chloride cases coincide with enhanced mean columnar R and negative values of precipitation susceptibility. The difference in drop effective radius between high and low chloride conditions decreases with height in cloud, suggesting that some GCCN-produced rain drops precipitate before reaching cloud tops. The sign of cloud responses (i.e., R) to perturbations in giant sea salt particle concentration, as evaluated from MERRA-2 reanalysis data, is consistent with the aircraft data

Stratocumulus Cloud Clearings and Notable Thermodynamic and Aerosol Contrasts across the Clear–Cloudy Interface

Data from three research flights, conducted over water near the California coast, are used to investigate the boundary between stratocumulus cloud decks and clearings of different sizes. Large clearings exhibit a diurnal cycle with growth during the day and contraction overnight and a multiday life cycle that can include oscillations between growth and decay, whereas a small coastal clearing was observed to be locally confined with a subdiurnal lifetime. Subcloud aerosol characteristics are similar on both sides of the clear–cloudy boundary in the three cases, while meteorological properties exhibit subtle, yet important, gradients, implying that dynamics, and not microphysics, is the primary driver for the clearing characteristics. Transects, made at multiple levels across the cloud boundary during one flight, highlight the importance of microscale (~1 km) structure in thermodynamic properties near the cloud edge, suggesting that dynamic forcing at length scales comparable to the convective eddy scale may be influential to the larger-scale characteristics of the clearing. These results have implications for modeling and observational studies of marine boundary layer clouds, especially in relation to aerosol–cloud interactions and scales of variability responsible for the evolution of stratocumulus clearings