The Interaction of High-Speed Turbulence with Flames: Global Properties and Internal Flame Structure

We study the dynamics and properties of a turbulent flame, formed in the presence of subsonic, high-speed, homogeneous, isotropic Kolmogorov-type turbulence in an unconfined system. Direct numerical simulations are performed with Athena-RFX, a massively parallel, fully compressible, high-order, dimensionally unsplit, reactive-flow code. A simplified reaction-diffusion model represents a stoichiometric H2-air mixture. The system being modeled represents turbulent combustion with the Damkohler number Da = 0.05 and with the turbulent velocity at the energy injection scale 30 times larger than the laminar flame speed. The simulations show that flame interaction with high-speed turbulence forms a steadily propagating turbulent flame with a flame brush width approximately twice the energy injection scale and a speed four times the laminar flame speed. A method for reconstructing the internal flame structure is described and used to show that the turbulent flame consists of tightly folded flamelets. The reaction zone structure of these is virtually identical to that of the planar laminar flame, while the preheat zone is broadened by approximately a factor of two. Consequently, the system evolution represents turbulent combustion in the thin-reaction zone regime. The turbulent cascade fails to penetrate the internal flame structure, and thus the action of small-scale turbulence is suppressed throughout most of the flame. Finally, our results suggest that for stoichiometric H2-air mixtures, any substantial flame broadening by the action of turbulence cannot be expected in all subsonic regimes.Comment: 30 pages, 9 figures; published in Combustion and Flam

The Interaction of High-Speed Turbulence with Flames: Turbulent Flame Speed

(Abridged) Direct numerical simulations of the interaction of a premixed flame with driven, subsonic, homogeneous, isotropic, Kolmogorov-type turbulence in an unconfined system are used to study the mechanisms determining the turbulent flame speed, S_T, in the thin reaction zone regime. High intensity turbulence is considered with the r.m.s. velocity 35 times the laminar flame speed, S_L, resulting in the Damkohler number Da = 0.05. Here we show that: (1) The flame brush has a complex internal structure, in which the isosurfaces of higher fuel mass fractions are folded on progressively smaller scales. (2) Global properties of the turbulent flame are best represented by the structure of the region of peak reaction rate, which defines the flame surface. (3) In the thin reaction zone regime, S_T is predominantly determined by the increase of the flame surface area, A_T, caused by turbulence. (4) The observed increase of S_T relative to S_L exceeds the corresponding increase of A_T relative to the surface area of the planar laminar flame, on average, by ~14%, varying from only a few percent to ~30%. (5) This exaggerated response is the result of tight flame packing by turbulence, which causes frequent flame collisions and formation of regions of high flame curvature, or "cusps." (6) The local flame speed in the cusps substantially exceeds its laminar value, which results in a disproportionately large contribution of cusps to S_T compared with the flame surface area in them. (7) A criterion is established for transition to the regime significantly influenced by cusp formation. In particular, at Karlovitz numbers Ka > 20, flame collisions provide an important mechanism controlling S_T, in addition to the increase of A_T by large-scale motions and the potential enhancement of diffusive transport by small-scale turbulence.Comment: 44 pages, 20 figures; published in Combustion and Flam

Reactive Halogens in the Marine Boundary Layer (RHaMBLe): The tropical North Atlantic experiments

The NERC UK SOLAS-funded Reactive Halogens in the Marine Boundary Layer (RHaMBLe) programme comprised three field experiments. This manuscript presents an overview of the measurements made within the two simultaneous remote experiments conducted in the tropical North Atlantic in May and June 2007. Measurements were made from two mobile and one ground-based platforms. The heavily instrumented cruise D319 on the RRS Discovery from Lisbon, Portugal to São Vicente, Cape Verde and back to Falmouth, UK was used to characterise the spatial distribution of boundary layer components likely to play a role in reactive halogen chemistry. Measurements onboard the ARSF Dornier aircraft were used to allow the observations to be interpreted in the context of their vertical distribution and to confirm the interpretation of atmospheric structure in the vicinity of the Cape Verde islands. Long-term ground-based measurements at the Cape Verde Atmospheric Observatory (CVAO) on São Vicente were supplemented by long-term measurements of reactive halogen species and characterisation of additional trace gas and aerosol species during the intensive experimental period. This paper presents a summary of the measurements made within the RHaMBLe remote experiments and discusses them in their meteorological and chemical context as determined from these three platforms and from additional meteorological analyses. Air always arrived at the CVAO from the North East with a range of air mass origins (European, Atlantic and North American continental). Trace gases were present at stable and fairly low concentrations with the exception of a slight increase in some anthropogenic components in air of North American origin, though NOx mixing ratios during this period remained below 20 pptv (note the non-IUPAC adoption in this manuscript of pptv and ppbv, equivalent to pmol mol−1 and nmol mol−1 to reflect common practice). Consistency with these air mass classifications is observed in the time series of soluble gas and aerosol composition measurements, with additional identification of periods of slightly elevated dust concentrations consistent with the trajectories passing over the African continent. The CVAO is shown to be broadly representative of the wider North Atlantic marine boundary layer; measurements of NO, O3 and black carbon from the ship are consistent with a clean Northern Hemisphere marine background. Aerosol composition measurements do not indicate elevated organic material associated with clean marine air. Closer to the African coast, black carbon and NO levels start to increase, indicating greater anthropogenic influence. Lower ozone in this region is possibly associated with the increased levels of measured halocarbons, associated with the nutrient rich waters of the Mauritanian upwelling. Bromide and chloride deficits in coarse mode aerosol at both the CVAO and on D319 and the continuous abundance of inorganic gaseous halogen species at CVAO indicate significant reactive cycling of halogens. Aircraft measurements of O3 and CO show that surface measurements are representative of the entire boundary layer in the vicinity both in diurnal variability and absolute levels. Above the inversion layer similar diurnal behaviour in O3 and CO is observed at lower mixing ratios in the air that had originated from south of Cape Verde, possibly from within the ITCZ. ECMWF calculations on two days indicate very different boundary layer depths and aircraft flights over the ship replicate this, giving confidence in the calculated boundary layer depth

A 340 year record of biogenic sulphur from the Weddell Sea area, Antarctic

The high MSA (methanesulphonic acid) concentration reflects the proximity of the Weddell Sea, believed to be a region of high marine phytoplankton production. The overall mean nss-SO2-4 (non sea salt sulphate) concentration is about 66% of the total sulphate deposited in snowfall. Low-frequency variations of MSA and ozygen-isotope signals correlate closely, indicating that they may be modulated by similar atmospheric processes. Positive correlations are observed between the oxygen-isotope signature and both MSA and nss SO2-4. A small negative correlation can be seen between both species and the annual duration of sea ice at Scotia Bay, Laurie Island in the South Orkneys, since 1902. -from Author

A 3000-year Siberian ice core record of vanillic acid and p-hydroxybenzoic acid

Biomass burning plays an important role in atmospheric chemistry, the global carbon cycle, and climate. The relationship between burning and climate, and the factors that influence burning emissions over long timescales are not well understood. Therefore, well-dated records are needed to establish a history of biomass burning. In this study we examine the distribution of vanillic (VA) and p-hydroxybenzoic (p-HBA) acids in a Siberian Arctic ice core (Akademii Nauk) covering the past 2800 years. These molecules are produced by the incomplete combustion of lignin, incorporated into atmospheric aerosols, and transported/deposited on ice sheets. VA and p-HBA are generated from the combustion of conifers and grasses, respectively, but are not uniquely derived from these sources. These records should be considered qualitative because a wide range of aerosols is generated from various plant materials under different combustion conditions. The records may also reflect changes in source region locations, transport efficiency, and atmospheric removal prior to deposition. Ice core samples were analyzed using ion chromatography with electrospray MS/MS detection. VA and p-HBA levels were markedly elevated during three time periods. The most recent of these periods occurred from AD 1450-1720 (140-220 m). The timing of two earlier peaks is less well constrained. They are estimated to be from 300-700 AD (400-500 m) and from 800-400 BC (610-670 m). The similarity between VA and p-HBA suggests that the two compounds are derived from a common source. These three periods of elevated VA and p-HBA are not evident in nitrate, ammonium, or black carbon measurements from the same ice core or with high latitude sedimentary charcoal records from North America, Europe, or eastern Siberia

Arctic ice core records of vanillic acid from Siberia, Greenland, and Svalbard

Biomass burning is a major source atmospheric gases and aerosols, and an important part of the global carbon cycle and radiation budget. The factors controlling centennial and millennial variability in region/global biomass burning are not well understood because there are few well-dated proxy records. We are exploring ice core records of organic compounds resulting from incomplete combustion of lignin as tracers for biomass burning. In this study we investigate the distribution of vanillic acid (VA) in Arctic ice cores. VA is a major product of conifer combustion, but may also be produced from angiosperms. VA was measured in ice core samples using ion chromatography with electrospray MS/MS detection. Here we present measurements of vanillic acid in three Arctic ice cores from Siberia (Akademii Nauk; 0-3 kyr bp), northern Greenland (Tunu; 0-1.75 kyr bp), and Svalbard (Lomonosovfonna; 0-0.75 kyr bp). The Siberian record exhibits 3 strong centennial scale maxima (1200-600 BC, AD 300-800, and AD 1450-1700). All three cores exhibit a smaller feature around 1250, with a subsequent decline in Greenland and Svalbard. VA levels in Greenland and Svalbard are generally smaller than those in Siberia. These results suggest strong input from Asian sources to the Siberian core, and lower Arctic-wide “background” levels at the other sites

Aromatic acids in a Eurasian Arctic ice core: a 3000-year proxy record of biomass burning

Wildfires and their emissions have significant impacts on ecosystems, climate, atmospheric chemistry and carbon cycling. Well-dated proxy records are needed to study the long-term climatic controls on biomass burning and the associated climate feedbacks. There is a particular lack of information about long-term biomass burning variations in Siberia, the largest forested area in the Northern Hemisphere. In this study we report analyses of aromatic acids (vanillic and para-hydroxybenzoic acids) over the past 3145 years in the Eurasian Arctic Akademii Nauk ice core. These compounds are aerosol-borne, semi-volatile organic compounds derived from lignin combustion. The analyses were made using ion chromatography with electrospray mass spectrometric detection. The levels of these aromatic acids ranged from below the detection limit (.01 to .05 ppb) to about 1 ppb, with roughly 30 % of the samples above the detection limit. In the preindustrial late Holocene, highly elevated aromatic acid levels are observed during four distinct periods (1180–660 BCE, 180–220 CE, 380–660 CE, and 1460–1660 CE). The timing of these periods coincides with the episodic pulsing of ice-rafted debris in the North Atlantic known as Bond events. Aromatic acid levels also are elevated during the onset of the industrial period from 1780 to 1860 CE, but with a different ratio of vanillic and para-hydroxybenzoic acid than is observed during the preindustrial period. This study provides the first millennial scale record of aromatic acids. It clearly demonstrates that coherent aromatic acid signals are recorded in polar ice cores that can be used as proxies for past trends in biomass burning

Frontal enhancement of dimethylsulfide concentrations across a Gulf Stream meander

Aqueous and atmospheric dimethyl sulfide (DMS) concentrations (0.4-4 nM, 5-350 ppt) were determined across a Gulf Stream meander in April 1989. Physical processes along and across the front were expected to result in biological changes also reflected in DMS levels. Highest concentrations of aqueous DMS (3-4 nM) were observed in surface waters coinciding with Slope waters at, or inshore of, the Gulf Stream north wall. This water also contained the highest chlorophyll levels (up to 2.6 pg chl/l) which co-varied with the sea surface DMS concentrations. Concentrations of atmospheric DMS were lower and more constant (21 * 9 ppt) outside the frontal area, either in Slope or Stream waters. At the northern wall of the Gulf Stream, a strikingly sharp increase in atmospheric DMS (up to 350 ppt) was observed. 1

The chemistry of OH and HO2 radicals in the boundary layer over the tropical Atlantic Ocean

Fluorescence Assay by Gas Expansion (FAGE) has been used to detect ambient levels of OH and HO2 radicals at the Cape Verde Atmospheric Observatory, located in the tropical Atlantic marine boundary layer, during May and June 2007. Midday radical concentrations were high, with maximum concentrations of 9 ×106 molecule cm−3 and 6×108 molecule cm−3 observed for OH and HO2, respectively. A box model incorporating the detailed Master Chemical Mechanism, extended to include halogen chemistry, heterogeneous loss processes and constrained by all available measurements including halogen and nitrogen oxides, has been used to assess the chemical and physical parameters controlling the radical chemistry. The model was able to reproduce the daytime radical concentrations to within the 1 σ measurement uncertainty of 20% during the latter half of the measurement period but significantly under-predicted [HO2] by 39% during the first half of the project. Sensitivity analyses demonstrate that elevated [HCHO] (~2 ppbv) on specific days during the early part of the project, which were much greater than the mean [HCHO] (328 pptv) used to constrain the model, could account for a large portion of the discrepancy between modelled and measured [HO2] at this time. IO and BrO, although present only at a few pptv, constituted ~19% of the instantaneous sinks for HO2, whilst aerosol uptake and surface deposition to the ocean accounted for a further 23% of the HO2 loss at noon. Photolysis of HOI and HOBr accounted for ~13% of the instantaneous OH formation. Taking into account that halogen oxides increase the oxidation of NOx (NO → NO2), and in turn reduce the rate of formation of OH from the reaction of HO2 with NO, OH concentrations were estimated to be 9% higher overall due to the presence of halogens. The increase in modelled OH from halogen chemistry gives an estimated 9% shorter lifetime for methane in this region, and the inclusion of halogen chemistry is necessary to model the observed daily cycle of O3 destruction that is observed at the surface. Due to surface losses, we hypothesise that HO2 concentrations increase with height and therefore contribute a larger fraction of the O3 destruction than at the surface