Direct eddy-covariance measurements of aerosol number fluxes obtained during the 2007 CHATS field experiment in Dixon, California, USA are compared with relaxed eddy accumulation simulations using temperature and water vapour concentration as proxy scalars. After a brief discussion of the limited time response of the aerosol measurement, the applicability of temperature and water vapour concentration as proxy scalars for aerosol number concentration is investigated by evaluating scalar and spectral correlation coefficients as simple measures of scalar similarity. In addition, the proportionality factor b, which compensates for the use of a constant sampling flow in relaxed eddy accumulation, is derived from the time series of aerosol number, temperature and water vapour, and its variability is analyzed. The reduction of the b factor due to application of a deadband, i.e. the rejection of data when the vertical wind speed is close to zero, is evaluated for all three studied scalars, and compared with published functional relationships. In this study, using temperature or water vapour as proxy scalars for aerosol number shows no advantage over the use of a constant b factor. Thus, it is suggested to apply a deadband HREA = w′/σw = 0.6 to 0.8 (where w′ is the vertical velocity fluctuation and σw is its standard deviation), to use a theoretical b factor based on a parameterization that includes a stability dependence, and to calculate the deadband effect according to a derived relation for aerosol relaxed eddy accumulation. © Springer Science+Business Media B.V. 2008.

Dry deposition of ozone is an important sink of ozone in near surface air. When dry deposition occurs through plant stomata, ozone can injure the plant, altering water and carbon cycling and reducing crop yields. Quantifying both stomatal and nonstomatal uptake accurately is relevant for understanding ozone's impact on human health as an air pollutant and on climate as a potent short-lived greenhouse gas and primary control on the removal of several reactive greenhouse gases and air pollutants. Robust ozone dry deposition estimates require knowledge of the relative importance of individual deposition pathways, but spatiotemporal variability in nonstomatal deposition is poorly understood. Here we integrate understanding of ozone deposition processes by synthesizing research from fields such as atmospheric chemistry, ecology, and meteorology. We critically review methods for measurements and modeling, highlighting the empiricism that underpins modeling and thus the interpretation of observations. Our unprecedented synthesis of knowledge on deposition pathways, particularly soil and leaf cuticles, reveals process understanding not yet included in widely-used models. If coordinated with short-term field intensives, laboratory studies, and mechanistic modeling, measurements from a few long-term sites would bridge the molecular to ecosystem scales necessary to establish the relative importance of individual deposition pathways and the extent to which they vary in space and time. Our recommended approaches seek to close knowledge gaps that currently limit quantifying the impact of ozone dry deposition on air quality, ecosystems, and climate.

The emission, dispersion, and photochemistry of isoprene (C5H8) and related chemical species in the convective boundary layer (CBL) during sunlit daytime were studied over a mixed forest in the southeastern United States by combining ground-based and aircraft observations. Fluxes of isoprene and monoterpenes were quantified at the top of the forest canopy using a high-resolution proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS). Snapshot (2 min sampling duration) vertical profiles of isoprene, methyl vinyl ketone (MVK)Cmethacrolein (MACR), and monoterpenes were collected from aircraft every hour in the CBL (100-1000 m). Both ground-based and airborne collected volatile organic compound (VOC) data are used to constrain the initial conditions of a mixed-layer chemistry model (MXLCH), which is applied to examine the chemical evolution of the O3-NOx-HOx-VOC system and how it is affected by boundary layer dynamics in the CBL. The chemical loss rate of isoprene (1 h) is similar to the turbulent mixing timescale (0.1-0.5 h), which indicates that isoprene concentrations are equally dependent on both photooxidation and boundary layer dynamics. Analysis of a modelderived concentration budget suggests that diurnal evolution of isoprene inside the CBL is mainly controlled by surface emissions and chemical loss; the diurnal evolution of O3 is dominated by entrainment. The NO to HO2 ratio (NO :HO2) is used as an indicator of anthropogenic impact on the CBL chemical composition and spans a wide range (1-163). The fate of hydroxyl-substituted isoprene peroxyl radical (HOC5H8OO q; ISOPOO) is strongly affected by NO:HO2, shifting from NO-dominant to NO-HO2-balanced conditions from early morning to noontime. This chemical regime change is reflected in the diurnal evolution of isoprene hydroxynitrates (ISOPN) and isoprene hydroxy hydroperoxides (ISOPOOH).

The Canopy Horizontal Array Turbulence Study (CHATS) experimental study was conducted at a Cilker Orchards's walnut blocks in Dixon, California, before and after leaves emerged, to help improve understanding, simulation capabilities, and modeling of coupled vegetation-atmosphere-land surface interactions. The campaign took place over 12 weeks in the spring of 2007 and was broken into three 4-week phases. Canopy-induced mechanical and thermodynamical vertical variation of turbulence transport characteristics and the linkages between canopy-scale motions and the larger scale planetary boundary layer (PBL) turbulence were measured. The observations focused on measurements characterizing stratification influences on the spatial structure of canopy-induced turbulence, the trace gas source/sink distribution associated with vegetation, and the overall impact of canopy-induced processes on trace gas transport.