A DNS study of aerosol and small-scale cloud turbulence interaction

The purpose of this study is to investigate the interaction between small-scale turbulence and aerosol and cloud microphysical properties using direct numerical simulations (DNS). We consider the domain located at the height of about 2000 m from the sea level, experiencing transient high supersaturation due to atmospheric fluctuations of temperature and humidity. To study the effect of total number of particles (Ntot) on air temperature, activation and supersaturation, we vary Ntot. To investigate the effect of aerosol dynamics on small-scale turbulence and vertical air motion, we vary the intensity of turbulent fluctuations and the buoyant force. We find that even a small number of aerosol particles (55.5 cm−3), and therefore a small droplet number concentration, strongly affects the air temperature due to release of latent heat. The system comes to an equilibrium faster and the relative number of activated particles appears to be smaller for larger Ntot. We conclude that aerosol particles strongly affect the air motion. In a case of updraught coursed by buoyant force, the presence of aerosol particles results in acceleration of air motion in vertical direction and increase of turbulent fluctuations

Numerical framework for the computation of urban flux footprints employing large-eddy simulation and Lagrangian stochastic modeling

Conventional footprint models cannot account for the heterogeneity of the urban landscape imposing a pronounced uncertainty on the spatial interpretation of eddycovariance (EC) flux measurements in urban studies. This work introduces a computational methodology that enables the generation of detailed footprints in arbitrarily complex urban flux measurements sites. The methodology is based on conducting high-resolution large-eddy simulation (LES) and Lagrangian stochastic (LS) particle analysis on a model that features a detailed topographic description of a real urban environment. The approach utilizes an arbitrarily sized target volume set around the sensor in the LES domain, to collect a dataset of LS particles which are seeded from the potential source area of the measurement and captured at the sensor site. The urban footprint is generated from this dataset through a piecewise postprocessing procedure, which divides the footprint evaluation into multiple independent processes that each yield an intermediate result. These results are ultimately selectively combined to produce the final footprint. The strategy reduces the computational cost of the LES-LS simulation and incorporates techniques to account for the complications that arise when the EC sensor is mounted on a building instead of a conventional flux tower. The presented computational framework also introduces a result assessment strategy which utilizes the obtained urban footprint together with a detailed land cover type dataset to estimate the potential error that may arise if analytically derived footprint models were employed instead. The methodology is demonstrated with a case study that concentrates on generating the footprint for a building-mounted EC measurement station in downtown Helsinki, Finland, under the neutrally stratified atmospheric boundary layer.Peer reviewe

Experimental validation of footprint models for eddy covariance CO2 flux measurements above grassland by means of natural and artificial tracers

Footprint models, which simulate source area for scalar fluxes, are fundamental tools for a correct interpretation of micromoeteorological flux measurements and ecosystem exchange inferred from such data. Over the last two decades models of varying complexity have been developed, but all of them suffer from a significant lack of experimental validation. In this study two different experimental tests have been conducted with the aim of offering validation: a manipulation of the vegetation cover and an artificial tracer emission. In the first case the extension of the flux source has been changed progressively by successive cuts of vegetation, while in the second case by varying the distance of a tracer emission line respect to the measurement point. Results have been used to validate two analytical and a numerical footprint models. The experimental data show a good agreement with footprint models and indicate a limited extension of the flux source area, with approximately 75% of the sources confined within a range of 10-20 times the effective measurement height, i.e. the measurement height above the zero plane displacement. Another interesting result was the strong dependence on the surface roughness of both experimental estimates and numerical simulations of footprint. The effect of surface roughness on experimental results and models outputs was comparable to the effect of atmospheric stability. This indicates that surface roughness and turbulence conditions may play a significant role in source area location, in particular above inhomogeneous surfaces with change in roughness, as in the case of the manipulation experiment. Consequently a careful site specific quantification of these parameters seems to be fundamental to obtain realistic footprint estimates and significantly improve eddy covariance flux interpretation at complex sites.Peer reviewe

Boreal forest BVOC exchange : emissions versus in-canopy sinks

A multilayer gas dry deposition model has been developed and implemented into a one-dimensional chemical transport model SOSAA (model to Simulate the concentrations of Organic vapours, Sulphuric Acid and Aerosols) to calculate the dry deposition velocities for all the gas species included in the chemistry scheme. The new model was used to analyse in-canopy sources and sinks, including gas emissions, chemical production and loss, dry deposition, and turbulent transport of 12 featured biogenic volatile organic compounds (BVOCs) or groups of BVOCs (e.g. monoterpenes, isoprene+2-methyl-3-buten-2-ol (MBO), sesquiterpenes, and oxidation products of mono-and sesquiterpenes) in July 2010 at the boreal forest site SMEAR II (Station for Measuring Ecosystem-Atmosphere Relations). According to the significance of modelled monthly-averaged individual source and sink terms inside the canopy, the selected BVOCs were classified into five categories: 1. Most of emitted gases are transported out of the canopy (monoterpenes, isoprene + MBO). 2. Chemical reactions remove a significant portion of emitted gases (sesquiterpenes). 3. Bidirectional fluxes occur since both emission and dry deposition are crucial for the in-canopy concentration tendency (acetaldehyde, methanol, acetone, formaldehyde). 4. Gases removed by deposition inside the canopy are compensated for by the gases transported from above the canopy (acetol, pinic acid, beta-caryophyllene's oxidation product BCSOZOH). 5. The chemical production is comparable to the sink by deposition (isoprene's oxidation products ISOP34OOH and ISOP34NO3). Most of the simulated sources and sinks were located above about 0.2 h(c) (canopy height) for oxidation products and above about 0.4 h(c) for emitted species except formaldehyde. In addition, soil deposition (including deposition onto understorey vegetation) contributed 11-61% to the overall in-canopy deposition. The emission sources peaked at about 0.8-0.9 h(c), which was higher than 0.6 h(c) where the maximum of dry deposition onto overstorey vegetation was located. This study provided a method to enable the quantification of the exchange between atmosphere and biosphere for numerous BVOCs, which could be applied in large-scale models in future. With this more explicit canopy exchange modelling system, this study analysed both the temporal and spatial variations in individual in-canopy sources and sinks, as well as their combined effects on driving BVOC exchange. In this study 12 featured BVOCs or BVOC groups were analysed. Other compounds could also be investigated similarly by being classified into these five categories.Peer reviewe

Comparison between static chamber and tunable diode laser-based eddy covariance techniques for measuring nitrous oxide fluxes from a cotton field

Nitrous oxide (N2O) fluxes from a cotton field in northern China were measured for a year using the static chamber method based on a gas chromatograph (GC) and the eddy covariance (EC) technique based on a tunable diode laser (TDL). The aims were to compare the N2O fluxes obtained from both techniques, assess the uncertainties in the fluxes and evaluate the annual direct emission factors (EFds, i.e. the loss rate of fertilizer nitrogen via N2O emission) using the year-round datasets. During the experimental period, the hourly and daily mean chamber fluxes ranged from 0.6 to 781.8 and from 1.2 to 468.8 g N m−2 h−1, respectively. The simultaneously measured daily mean EC fluxes varied between −10.8 and 912.0 g N m−2 h−1. The EC measurements only provided trustworthy 30-min fluxes during high-emission period (a 20-day period immediately after the irrigation that followed the nitrogen fertilization event). A reliable comparison was confined to the high-emission period and showed that the chamber fluxes were 17–20% lower than the EC fluxes. This difference may implicate the magnitude of systematic underestimation in the fluxes from chamber measurements. The annual emission from the fertilized cotton field was estimated at 1.43 kg N ha−1 yr−1 by the chamber observations and 3.15 kg N ha−1 yr−1 by the EC measurements. The EFds calculated from the chamber and EC data were 1.04% and 1.65%, respectively. The chamber-based estimate was very close to the default value (1.0%) recommended by the Intergovernmental Panel on Climate Change. However, the difference in the EFds based on the two measurement techniques may vary greatly with changing environmental conditions and management practices. Further comparison studies are still needed to elucidate this issue.Peer reviewe

Aerosol dynamics within and above forest in relation to turbulent transport and dry deposition

A 1-D atmospheric boundary layer (ABL) model coupled with a detailed atmospheric chemistry and aerosol dynamical model, the model SOSAA, was used to predict the ABL and detailed aerosol population (characterized by the number size distribution) time evolution. The model was applied over a period of 10 days in May 2013 to a pine forest site in southern Finland. The period was characterized by frequent new particle formation events and simultaneous intensive aerosol transformation. The aim of the study was to analyze and quantify the role of aerosol and ABL dynamics in the vertical transport of aerosols. It was of particular interest to what extent the fluxes above the canopy deviate from the particle dry deposition on the canopy foliage due to the above-mentioned processes. The model simulations revealed that the particle concentration change due to aerosol dynamics frequently exceeded the effect of particle deposition by even an order of magnitude or more. The impact was, however, strongly dependent on particle size and time. In spite of the fact that the timescale of turbulent transfer inside the canopy is much smaller than the timescales of aerosol dynamics and dry deposition, leading us to assume well-mixed properties of air, the fluxes at the canopy top frequently deviated from deposition inside the forest. This was due to transformation of aerosol concentration throughout the ABL and resulting complicated pattern of vertical transport. Therefore we argue that the comparison of timescales of aerosol dynamics and deposition defined for the processes below the flux measurement level do not unambiguously describe the importance of aerosol dynamics for vertical transport above the canopy. We conclude that under dynamical conditions reported in the current study the micrometeorological particle flux measurements can significantly deviate from the dry deposition into the canopy. The deviation can be systematic for certain size ranges so that the time-averaged particle fluxes can be also biased with respect to deposition sink.Peer reviewe

A DNS study of aerosol and small-scale cloud turbulence interaction

The purpose of this study is to investigate the interaction between small-scale turbulence and aerosol and cloud microphysical properties using direct numerical simulations (DNS). We consider the domain located at the height of about 2000aEuro-m from the sea level, experiencing transient high supersaturation due to atmospheric fluctuations of temperature and humidity. To study the effect of total number of particles (N-tot) on air temperature, activation and supersaturation, we vary N-tot. To investigate the effect of aerosol dynamics on small-scale turbulence and vertical air motion, we vary the intensity of turbulent fluctuations and the buoyant force. We find that even a small number of aerosol particles (55.5aEuro-cm(-3)), and therefore a small droplet number concentration, strongly affects the air temperature due to release of latent heat. The system comes to an equilibrium faster and the relative number of activated particles appears to be smaller for larger N-tot. We conclude that aerosol particles strongly affect the air motion. In a case of updraught coursed by buoyant force, the presence of aerosol particles results in acceleration of air motion in vertical direction and increase of turbulent fluctuations.Peer reviewe

Large-eddy simulation and stochastic modeling of Lagrangian particles for footprint determination in the stable boundary layer

Large-eddy simulation (LES) and Lagrangian stochastic modeling of passive particle dispersion were applied to the scalar flux footprint determination in the stable atmospheric boundary layer. The sensitivity of the LES results to the spatial resolution and to the parameterizations of small-scale turbulence was investigated. It was shown that the resolved and partially resolved ("subfilter-scale") eddies are mainly responsible for particle dispersion in LES, implying that substantial improvement may be achieved by using recovering of small-scale velocity fluctuations. In LES with the explicit filtering, this recovering consists of the application of the known inverse filter operator. The footprint functions obtained in LES were compared with the functions calculated with the use of first-order single-particle Lagrangian stochastic models (LSMs) and zeroth-order Lagrangian stochastic models - the random displacement models (RDMs). According to the presented LES, the source area and footprints in the stable boundary layer can be substantially more extended than those predicted by the modern LSMs.Peer reviewe

Seasonal and diurnal variation in CO fluxes from an agricultural bioenergy crop

Carbon monoxide (CO) is an important reactive trace gas in the atmosphere, while its sources and sinks in the biosphere are poorly understood. Soils are generally considered as a sink of CO due to microbial oxidation processes, while emissions of CO have been reported from a wide range of soil-plant systems. We measured CO fluxes using the micrometeorological eddy covariance method from a bioenergy crop (reed canary grass) in eastern Finland from April to November 2011. Continuous flux measurements allowed us to assess the seasonal and diurnal variability and to compare the CO fluxes to simultaneously measured net ecosystem exchange of CO2, N2O and heat fluxes as well as to relevant meteorological, soil and plant variables in order to investigate factors driving the CO exchange. The reed canary grass (RCG) crop was a net source of CO from mid-April to mid-June and a net sink throughout the rest of the measurement period from mid-June to November 2011, excluding a measurement break in July. CO fluxes had a distinct diurnal pattern with a net CO uptake in the night and a net CO emission during the daytime with a maximum emission at noon. This pattern was most pronounced in spring and early summer. During this period the most significant relationships were found between CO fluxes and global radiation, net radiation, sensible heat flux, soil heat flux, relative humidity, N2O flux and net ecosystem exchange. The strong positive correlation between CO fluxes and radiation suggests abiotic CO production processes, whereas the relationship between CO fluxes and net ecosystem exchange of CO2, and night-time CO fluxes and N2O emissions indicate biotic CO formation and microbial CO uptake respectively. The study shows a clear need for detailed process studies accompanied by continuous flux measurements of CO exchange to improve the understanding of the processes associated with CO exchange.Peer reviewe