The use of disjunct eddy sampling methods for the determination of ecosystem level fluxes of trace gases

The concept of disjunct eddy sampling (DES) for use in measuring ecosystem-level micrometeorological fluxes is re-examined. The governing equations are discussed as well as other practical considerations and guidelines concerning this sampling method as it is applied to either the disjunct eddy covariance (DEC) or disjunct eddy accumulation (DEA) techniques. A disjunct eddy sampling system was constructed that could either be combined with relatively slow sensors (response time of 2 to 40 s) to measure fluxes using DEC, or could also be used to accumulate samples in stable reservoirs for later laboratory analysis (DEA technique). Both the DEC and DEA modes of this sampler were tested against conventional eddy covariance (EC) for fluxes of either CO2 (DEC) or isoprene (DEA). Good agreement in both modes was observed relative to the EC systems. However, the uncertainty in a single DEA flux measurement was considerable (40%) due to both the reduced statistical sampling and the analytical precision of the concentration difference measurements. We have also re-investigated the effects of nonzero mean vertical wind velocity on accumulation techniques as it relates to our DEA measurements. Despite the higher uncertainty, disjunct eddy sampling can provide an alternative technique to eddy covariance for determining ecosystem-level fluxes for species where fast sensors do not currently exist

Urban Dispersion Program Overview and MID05 Field Study Summary

The Urban Dispersion Program (UDP) was a 4-year project (2004–2007) funded by the U.S. Department of Homeland Security with additional support from the Defense Threat Reduction Agency. The U.S. Environmental Protection Agency (EPA) also contributed to UDP through funding a human-exposure component of the New York City (NYC) field studies in addition to supporting an EPA scientist in conducting modeling studies of NYC. The primary goal of UDP was to improve the scientific understanding of the flow and diffusion of airborne contaminants through and around the deep street canyons of NYC. The overall UDP project manager and lead scientist was Dr. Jerry Allwine of Pacific Northwest National Laboratory. UDP had several accomplishments that included conducting two tracer and meteorological field studies in Midtown Manhattan

Asian Tracer Experiment and Atmospheric Modeling (TEAM) Project: Draft Field Work Plan for the Asian Long-Range Tracer Experiment

This report provides an experimental plan for a proposed Asian long-range tracer study as part of the international Tracer Experiment and Atmospheric Modeling (TEAM) Project. The TEAM partners are China, Japan, South Korea and the United States. Optimal times of year to conduct the study, meteorological measurements needed, proposed tracer release locations, proposed tracer sampling locations and the proposed durations of tracer releases and subsequent sampling are given. Also given are the activities necessary to prepare for the study and the schedule for completing the preparation activities leading to conducting the actual field operations. This report is intended to provide the TEAM members with the information necessary for planning and conducting the Asian long-range tracer study. The experimental plan is proposed, at this time, to describe the efforts necessary to conduct the Asian long-range tracer study, and the plan will undoubtedly be revised and refined as the planning goes forward over the next year

A Tracer Investigation of Pheromone Dispersion in Lodgepole and Ponderosa Pine Forest Canopies

Tracer experiments were conducted in 2000 and 2001 to study spread of insect pheromone plumes in forest canopies. The field sites consisted of lodgepole pine (Pinus contorta) and ponderosa pine (P. ponderosa) canopies in 2000 and 2001, respectively. Ranges of temperature, wind speed, and turbulence conditions were similar in the two campaigns, and field data showed comparable variability on near-instantaneous time scales of wind speed, wind direction, and plume behavior. We developed simple empirical equations to estimate average horizontal and vertical plume spread as functions of standard turbulence statistics, downwind distance from the source, and wind speed. For horizontal plume spread, predicted dispersion coefficients were within a factor of 3, or better, for 97 percent of the observed values in the combined dataset from 2000 and 2001. Likewise, 99 percent of the predicted vertical dispersion coefficients were within a factor of 3 of the observed data

Modeling and Measuring the Nocturnal Drainage Flow in a High-Elevation, Subalpine Forest with Complex Terrain

The nocturnal drainage flow of air causes significant uncertainty in ecosystem CO2, H2O, and energy budgets determined with the eddy covariance measurement approach. In this study, we examined the magnitude, nature, and dynamics of the nocturnal drainage flow in a subalpine forest ecosystem with complex terrain. We used an experimental approach involving four towers, each with vertical profiling of wind speed to measure the magnitude of drainage flows and dynamics in their occurrence. We developed an analytical drainage flow model, constrained with measurements of canopy structure and SF6 diffusion, to help us interpret the tower profile results. Model predictions were in good agreement with observed profiles of wind speed, leaf area density, and wind drag coefficient. Using theory, we showed that this one‐dimensional model is reduced to the widely used exponential wind profile model under conditions where vertical leaf area density and drag coefficient are uniformly distributed. We used the model for stability analysis, which predicted the presence of a very stable layer near the height of maximum leaf area density. This stable layer acts as a flow impediment, minimizing vertical dispersion between the subcanopy air space and the atmosphere above the canopy. The prediction is consistent with the results of SF6 diffusion observations that showed minimal vertical dispersion of nighttime, subcanopy drainage flows. The stable within‐canopy air layer coincided with the height of maximum wake‐to‐shear production ratio. We concluded that nighttime drainage flows are restricted to a relatively shallow layer of air beneath the canopy, with little vertical mixing across a relatively long horizontal fetch. Insight into the horizontal and vertical structure of the drainage flow is crucial for understanding the magnitude and dynamics of the mean advective CO2 flux that becomes significant during stable nighttime conditions and are typically missed during measurement of the turbulent CO2 flux. The model and interpretation provided in this study should lead to research strategies for the measurement of these advective fluxes and their inclusion in the overall mass balance for CO2 at this site with complex terrain

Comparison of aromatic hydrocarbon measurements made by PTR-MS, DOAS and GC-FID during the MCMA 2003 Field Experiment

A comparison of aromatic hydrocarbon measurements is reported for the CENICA supersite in the district of Iztapalapa during the Mexico City Metropolitan Area field experiment in April 2003 (MCMA 2003). Data from three different measurement methods were compared: a Proton Transfer Reaction Mass Spectrometer (PTR-MS), long path measurements using a UV Differential Optical Absorption Spectrometer (DOAS), and Gas Chromatography-Flame Ionization analysis (GC-FID) of canister samples. The principle focus was on the comparison between PTR-MS and DOAS data. Lab tests established that the PTR-MS and DOAS calibrations were consistent for a suite of aromatic compounds including benzene, toluene, p-xylene, ethylbenzene, 1,2,4-trimethylbenzene, phenol and styrene. The point sampling measurements by the PTR-MS and GC-FID showed good correlations (r=0.6), and were in reasonable agreement for toluene, C2-alkylbenzenes and C3-alkylbenzenes. The PTR-MS benzene data were consistently high, indicating interference from ethylbenzene fragmentation for the 145 Td drift field intensity used in the experiment. Correlations between the open-path data measured at 16-m height over a 860-m path length (retroreflector in 430 m distance), and the point measurements collected at 37-m sampling height were best for benzene (r=0.61), and reasonably good for toluene, C2-alkylbenzenes, naphthalene, styrene, cresols and phenol (r>0.5). There was good agreement between DOAS and PTR-MS measurements of benzene after correction for the PTR-MS ethylbenzene interference. Mixing ratios measured by DOAS were on average a factor of 1.7 times greater than the PTR-MS data for toluene, C2-alkylbenzenes, naphthalene and styrene. The level of agreement for the toluene data displayed a modest dependence on wind direction, establishing that spatial gradients – horizontal, vertical, or both – in toluene mixing ratios were significant, and up to a factor of 2 despite the fact that all measurements were conducted above roof level. Our analysis highlights a potential problem in defining a VOC sampling strategy that is meaningful for the comparison with photochemical transport models: meaningful measurements require a spatial fetch that is comparable to the grid cell size of models, which is typically a few 10 km2. Long-path DOAS measurements inherently average over a larger spatial scale than point measurements. The spatial representativeness can be further increased if observations are conducted outside the surface roughness sublayer, which might require measurements at altitudes as high as 10 s of metres above roof level.Alexander von Humboldt-Stiftung (Feodor Lynen fellowship)Henry & Camille Dreyfus Foundation (Postdoctral Fellowship in Environmental Chemistry

Eddy covariance flux measurements of pollutant gases in urban Mexico City

Eddy covariance (EC) flux measurements of the atmosphere/surface exchange of gases over an urban area are a direct way to improve and evaluate emissions inventories, and, in turn, to better understand urban atmospheric chemistry and the role that cities play in regional and global chemical cycles. As part of the MCMA-2003 study, we demonstrated the feasibility of using eddy covariance techniques to measure fluxes of selected volatile organic compounds (VOCs) and CO2 [CO subscript 2] from a residential district of Mexico City (Velasco et al., 2005a, b). During the MILAGRO/MCMA-2006 field campaign, a second flux measurement study was conducted in a different district of Mexico City to corroborate the 2003 flux measurements, to expand the number of species measured, and to obtain additional data for evaluation of the local emissions inventory. Fluxes of CO2 [CO subscript 2] and olefins were measured by the conventional EC technique using an open path CO2 [CO subscript 2] sensor and a Fast Isoprene Sensor calibrated with a propylene standard. In addition, fluxes of toluene, benzene, methanol and C2-benzenes [C subscript 2 - benzenes] were measured using a virtual disjunct EC method with a Proton Transfer Reaction Mass Spectrometer. The flux measurements were analyzed in terms of diurnal patterns and vehicular activity and were compared with the most recent gridded emissions inventory. In both studies, the results showed that the urban surface of Mexico City is a net source of CO2 [CO subscript 2] and VOCs with significant contributions from vehicular traffic. Evaporative emissions from commercial and other anthropogenic activities were significant sources of toluene and methanol. The data show that the emissions inventory is in reasonable agreement with measured olefin and CO2 [CO subscript 2] fluxes, while C2-benzenes [C subscript 2 - benzenes] and toluene emissions from evaporative sources are overestimated in the inventory. It appears that methanol emissions from mobile sources occur, but are not present in the mobile emissions inventory.National Science Foundation (U.S.) (Grant ATM-0528227)United States. Dept. of Energy (Award DE-FG02-05ER63980)Mexico. Comisión Ambiental MetropolitanaMolina Center for Energy and the Environmen

Dust Plume Modeling at Fort Bliss: Full Training Scenario

The potential for air quality impacts from heavy mechanized vehicles operating in the training ranges and on the unpaved main supply routes at Fort Bliss is being investigated. The investigation uses the atmospheric modeling system DUSTRAN to simulate fugitive dust emission and dispersion from typical activities occurring on the installation. This report conveys the results of DUSTRAN simulations conducted using a “Full Training” scenario developed by Fort Bliss personnel. he Full Training scenario includes simultaneous off-road activities of two full Heavy Brigade Combat Teams (HCBTs) and one HCBT battalion on three training ranges. Simulations were conducted for the six-day period, April 25-30, 2005, using previously archived meteorological records. Simulation results are presented in the form of 24-hour average PM10 plots and peak 1-hour PM10 concentration plots, where the concentrations represent contributions resulting from the specified military vehicular activities, not total ambient PM10 concentrations. Results indicate that the highest PM10 contribution concentrations occurred on April 30 when winds were light and variable. Under such conditions, lofted particulates generated by vehicular movement stay in the area of generation and are not readily dispersed. The effect of training duration was investigated by comparing simulations with vehicular activity extending over a ten hour period (0700 to 1700 MST) with simulations where vehicular activity was compressed into a one hour period (0700 to 0800 MST). Compressing all vehicular activity into one hour led to higher peak one-hour and 24-hour average concentration contributions, often substantially higher

Dust Plume Modeling at Fort Bliss: Move-Out Operations, Combat Training and Wind Erosion

The potential for air-quality impacts from heavy mechanized vehicles operating in the training ranges and on the unpaved main supply routes at Fort Bliss was investigated. This report details efforts by the staff of Pacific Northwest National Laboratory for the Fort Bliss Directorate of Environment in this investigation. Dust emission and dispersion from typical activities, including move outs and combat training, occurring on the installation were simulated using the atmospheric modeling system DUSTRAN. Major assumptions associated with designing specific modeling scenarios are summarized, and results from the simulations are presented

Distribution, magnitudes, reactivities, ratios and diurnal patterns of volatile organic compounds in the Valley of Mexico during the MCMA 2002 and 2003 field campaigns

International audienceA wide array of volatile organic compound (VOC) measurements was conducted in the Valley of Mexico during the MCMA-2002 and 2003 field campaigns. Study sites included locations in the urban core, in a heavily industrial area and at boundary sites in rural landscapes. In addition, a novel mobile-laboratory-based conditional sampling method was used to collect samples dominated by fresh on-road vehicle exhaust to identify those VOCs whose ambient concentrations were primarily due to vehicle emissions. Five distinct analytical techniques were used: whole air canister samples with Gas Chromatography/Flame Ionization Detection (GC-FID), on-line chemical ionization using a Proton Transfer Reaction Mass Spectrometer (PTR-MS), continuous real-time detection of olefins using a Fast Olefin Sensor (FOS), and long path measurements using UV Differential Optical Absorption Spectrometers (DOAS). The simultaneous use of these techniques provided a wide range of individual VOC measurements with different spatial and temporal scales. The VOC data were analyzed to understand concentration and spatial distributions, diurnal patterns, origin and reactivity in the atmosphere of Mexico City. The VOC burden (in ppbC) was dominated by alkanes (60%), followed by aromatics (15%) and olefins (5%). The remaining 20% was a mix of alkynes, halogenated hydrocarbons, oxygenated species (esters, ethers, etc.) and other unidentified VOCs. However, in terms of ozone production, olefins were the most relevant hydrocarbons. Elevated levels of toxic hydrocarbons, such as 1,3-butadiene, benzene, toluene and xylenes were also observed. Results from these various analytical techniques showed that vehicle exhaust is the main source of VOCs in Mexico City and that diurnal patterns depend on vehicular traffic. Finally, examination of the VOC data in terms of lumped modeling VOC classes and its comparison to the VOC lumped emissions reported in other photochemical air quality modeling studies suggests that some, but not all, VOC classes are underestimated in the emissions inventory by factors of 1.1 to 3