Abstract

A relaxed eddy accumulation (REA) system was designed to continuously measure total gaseous mercury (TGM) fluxes over a forest canopy. TGM concentration measurements were measured at 5-min intervals with a Tekran model 2537A mercury analyzer located above the forest canopy on a walk-up meteorological tower. Ten-minute averages for up- and downdraft mercury concentrations were used to calculate the flux. The multiresolution decomposition technique was used to determine day- and nighttime averaging periods for the turbulent statistics used in the REA technique. This paper documents the REA system for mercury flux measurements and its use over a forest canopy.

The REA system response to the averaging times for the turbulent statistics and corrections to up- and downdraft concentrations are major considerations when using the technique with the Tekran mercury analyzer over a forest canopy. TGM flux data collected from 18 August to 12 September 2005 are used here to demonstrate the capabilities of the REA system to measure both short- (1-h time periods) and long-term flux dynamics. During the demonstration period the TGM median flux was 21.9 ± 32.6 ng m⁻² h⁻¹ and the median atmospheric TGM concentrations were 1.34 ± 0.13 ng m⁻² h⁻¹. Maximum short-term TGM evasive fluxes occurred during the daylight hours with minimums during the nighttime. A consistent bimodal emission pattern was observed during the daytime emissions over the canopy. The first peak occurred immediately following the evaporation of the nighttime dew on the canopy and the second peak occurred in the late afternoon.

Abstract

This paper presents a review of recent natural surface mercury exchange research in the context of a new modeling framework. The literature indicates that the mercury biogeochemical flux is more dynamic than the current models predict, with interacting multimedia storage and processes. Although several natural mercury emissions models have been created and incorporated into air quality models (AQMs), none are coupled with air quality models on a mass balance basis, and all lack the capacity to explain processes that involve the transport of mercury across atmosphere–surface media concentration gradients. Existing natural mercury emission models treat the surface as both an infinite source and infinite sink for emissions and deposition, respectively, and estimate emissions through the following three pathways: soil, vegetation, and surface waters. The use of these three transport pathways, but with compartmentalized surface storage in a surface–vegetation–atmosphere transport (SVAT) resistance model, is suggested. Surface water fluxes will be modeled using a two-film diffusion model coupled to a surface water photochemical model. This updated framework will allow both the parameterization of the transport of mercury across atmosphere–surface media concentration gradients and the accumulation/depletion of mercury in the surface media. However, several key parameters need further experimental verification before the proposed modeling framework can be implemented in an AQM. These include soil organic mercury interactions, bioavailability, cuticular transport of mercury, atmospheric surface compensation points for different vegetation species, and enhanced soil diffusion resulting from pressure perturbations.

Abstract

Families of solitary waves (“solitons”) associated with two atmospheric bores on the same day were observed by an unprecedented number of ground-based and airborne profiling systems during the International H₂O Project (IHOP). In addition, a very high-resolution numerical weather prediction model initialized with real data was used with success to simulate one of the bores and the evolving soliton. The predicted wave amplitude, phase speed, wavelength, and structure compared well to these extraordinarily detailed observations. The observations suggest that during the active phase (when turbulent mixing was active, which was prior to bore collapse), the bores and waves vigorously mixed dry air from above a nocturnal boundary layer down to the surface. Refractivity computed from near-surface radar observations showed pronounced decreases due to sudden drying during the passage of the bores in this phase, but refractivity increases appeared during the period of bore collapse. During both phases, the bores wafted aerosol-laden moist air up to the middle troposphere and weakened the capping inversion, thus reducing inhibition to deep convection development. The model results indicate that the refractivity decreases near the surface were due to drying caused by downward turbulent mixing of air by the wave circulations. Turbulent kinetic energy was generated immediately behind the bore head, then advected rearward and downward by the solitary waves. During the dissipation stage, the lifting by the bore head produced adiabatic cooling aloft and distributed the very moist air near the surface upward through the bore depth, but without any drying due to the absence of vigorous mixing. Thus, this study shows that the moist thermodynamic effects caused by atmospheric bores and solitons strongly depend upon the life cycle of these phenomena.

Abstract

Forecasts of zonal wind fields produced by the medium-range forecast (MRF) model of the National Meteorological Center are used to create predictions of the atmosphere's angular momentum at lead times of 1–10 days. Forecasts of this globally integrated quantity are of interest to geodesists and others concerned with monitoring changes in the earth's orientation for navigational purposes. Based on momentum forecasts archived for the period December 1985–November 1986, we find that, on average, the MRF exhibits positive skill relative to persistence-based forecasts at all lead times. Over our entire one-year study period, the improvement over persistence exceeds 20% for 2–6-day forecasts and remains as large as 10% even for 10-day forecasts. On the other hand, skill scores for the MRF momentum predictions vary considerably from month to month, and for a sizeable fraction of our study period the MRF is less skillful than persistence. Thus, although our initial impression of the overall quality of the MRF momentum forecasts is favorable, further improvement is certainly desirable.

Abstract

The chemical species emitted by forests create complex atmospheric oxidation chemistry and influence global atmospheric oxidation capacity and climate. The Southern Oxidant and Aerosol Study (SOAS) provided an opportunity to test the oxidation chemistry in a forest where isoprene is the dominant biogenic volatile organic compound. Hydroxyl (OH) and hydroperoxyl (HO₂) radicals were two of the hundreds of atmospheric chemical species measured, as was OH reactivity (the inverse of the OH lifetime). OH was measured by laser-induced fluorescence (LIF) and by taking the difference in signals without and with an OH scavenger that was added just outside the instrument’s pinhole inlet. To test whether the chemistry at SOAS can be simulated by current model mechanisms, OH and HO₂ were evaluated with a box model using two chemical mechanisms: Master Chemical Mechanism, version 3.2 (MCMv3.2), augmented with explicit isoprene chemistry and MCMv3.3.1. Measured and modeled OH peak at about 10⁶ cm⁻³ and agree well within combined uncertainties. Measured and modeled HO₂ peak at about 27 pptv and also agree well within combined uncertainties. Median OH reactivity cycled between about 11 s⁻¹ at dawn and about 26 s⁻¹ during midafternoon. A good test of the oxidation chemistry is the balance between OH production and loss rates using measurements; this balance was observed to within uncertainties. These SOAS results provide strong evidence that the current isoprene mechanisms are consistent with measured OH and HO₂ and, thus, capture significant aspects of the atmospheric oxidation chemistry in this isoprene-rich forest.

Abstract

The Clouds, Aerosol, and Precipitation in the Marine Boundary Layer (CAP-MBL) deployment at Graciosa Island in the Azores generated a 21-month (April 2009–December 2010) comprehensive dataset documenting clouds, aerosols, and precipitation using the Atmospheric Radiation Measurement Program (ARM) Mobile Facility (AMF). The scientific aim of the deployment is to gain improved understanding of the interactions of clouds, aerosols, and precipitation in the marine boundary layer.

Graciosa Island straddles the boundary between the subtropics and midlatitudes in the northeast Atlantic Ocean and consequently experiences a great diversity of meteorological and cloudiness conditions. Low clouds are the dominant cloud type, with stratocumulus and cumulus occurring regularly. Approximately half of all clouds contained precipitation detectable as radar echoes below the cloud base. Radar and satellite observations show that clouds with tops from 1 to 11 km contribute more or less equally to surface-measured precipitation at Graciosa. A wide range of aerosol conditions was sampled during the deployment consistent with the diversity of sources as indicated by back-trajectory analysis. Preliminary findings suggest important two-way interactions between aerosols and clouds at Graciosa, with aerosols affecting light precipitation and cloud radiative properties while being controlled in part by precipitation scavenging.

The data from Graciosa are being compared with short-range forecasts made with a variety of models. A pilot analysis with two climate and two weather forecast models shows that they reproduce the observed time-varying vertical structure of lower-tropospheric cloud fairly well but the cloud-nucleating aerosol concentrations less well. The Graciosa site has been chosen to be a permanent fixed ARM site that became operational in October 2013.