Spectrally resolved light absorption properties of cooled soot from a methane flame

The optical properties of combustion-generated soot, crucial information for quantitative soot emission diagnostics and for climate modeling, have been determined for the particular case of cooled soot from a methane flame. Optical extinction measurements were performed over a wavelength range of 450–750 nm using a novel diffuse-light, spectrally resolved line-of-sight attenuation experiment, and quantified using extractive methods coupled with scanning and transmission electron microscopy in conjunction with a detailed uncertainty analysis. The absorption component of the total measured extinction was isolated by calculating the expected scattering contribution, according to the Rayleigh–Debye–Gans approximation for polydisperse fractal aggregates. In contrast to the large degree of scatter seen in data previously reported in the literature, a consistent trend of negligible variation of the soot absorption refractive index function E(m) with wavelength over the visible was observed (E(m)=0.35±0.03 at wavelengths of 450–750 nm). These new data are also cast in the form of dimensionless extinction, which is independent of the scatter correction, as well as mass absorption cross section, which is independent of the mass density of soot and is commonly used by atmospheric modelers.

[1]  N. Selçuk,et al.  Determination of soot temperature, volume fraction and refractive index from flame emission spectrometry , 2007 .

[2]  Constantine M. Megaridis,et al.  Morphology of flame-generated soot as determined by thermophoretic sampling , 1987 .

[3]  Ümit Özgür Köylü,et al.  Optical Properties of Soot in Buoyant Laminar Diffusion Flames , 1994 .

[4]  D. E. Rosner,et al.  Fractal-like Aggregates: Relation between Morphology and Physical Properties. , 2000, Journal of colloid and interface science.

[5]  R. Burnett,et al.  Lung cancer, cardiopulmonary mortality, and long-term exposure to fine particulate air pollution. , 2002, JAMA.

[6]  Richard Raspet,et al.  Photoacoustic and filter-based ambient aerosol light absorption measurements : Instrument comparisons and the role of relative humidity , 2003 .

[7]  Bianca Maria Vaglieco,et al.  In situ evaluation of the soot refractive index in the UV-visible from the measurement of the scattering and extinction coefficients in rich flames , 1990 .

[8]  C. Sorensen Light Scattering by Fractal Aggregates: A Review , 2001 .

[9]  Stefan Will,et al.  Laser-induced incandescence: recent trends and current questions , 2006 .

[10]  A. Ferrero,et al.  Measurement uncertainty , 2006, IEEE Instrumentation & Measurement Magazine.

[11]  Gerard M. Faeth,et al.  Refractive Indices at Visible Wavelengths of Soot Emitted From Buoyant Turbulent Diffusion Flames , 1997 .

[12]  Ümit Özgür Köylü,et al.  Soot Morphology and Optical Properties in Nonpremixed Turbulent Flame Environments , 1995 .

[13]  Ömer L. Gülder,et al.  Determination of the soot absorption function and thermal accommodation coefficient using low-fluence LII in a laminar coflow ethylene diffusion flame , 2004 .

[14]  P. Chylek,et al.  Effect of absorbing aerosols on global radiation budget , 1995 .

[15]  Ümit Özgür Köylü,et al.  Structure of Overfire Soot in Buoyant Turbulent Diffusion Flames at Long Residence Times , 1992 .

[16]  S. D. Stasio,et al.  Influence of the soot property uncertainties in temperature and volume-fraction measurements by two-colour pyrometry , 1994 .

[17]  G. Faeth,et al.  Optical Properties in the Visible of Overfire Soot in Large Buoyant Turbulent Diffusion Flames , 2000 .

[18]  Nelson P. Bryner,et al.  Comparison of a fractal smoke optics model with light extinction measurements , 1994 .

[19]  A. M. Brasil,et al.  a Recipe for Image Characterization of Fractal-Like Aggregates , 1998 .

[20]  G. M. Faeth,et al.  Spectral extinction coefficients of soot aggregates from turbulent diffusion flames , 1996 .

[21]  J. Seinfeld,et al.  Atmospheric Chemistry and Physics: From Air Pollution to Climate Change , 1997 .

[22]  Matthew R. Johnson,et al.  Diffuse-light two-dimensional line-of-sight attenuation for soot concentration measurements. , 2008, Applied optics.

[23]  T. T. Charalampopoulos,et al.  Refractive indices of pyrolytic graphite, amorphous carbon, and flame soot in the temperature range 25° to 600°C☆ , 1993 .

[24]  Takashi Kashiwagi,et al.  Simultaneous optical measurement of soot volume fraction and temperature in premixed flames , 1994 .

[25]  E. Therssen,et al.  Determination of the ratio of soot refractive index function E(m) at the two wavelengths 532 and 1064 nm by laser induced incandescence , 2007 .

[26]  Ümit Özgür Köylü,et al.  Optical Properties of Overfire Soot in Buoyant Turbulent Diffusion Flames At Long Residence Times , 1994 .

[27]  K. Thomson,et al.  Sensitivity and relative error analyses of soot temperature and volume fraction determined by two-color LII , 2009 .

[28]  Rajan K. Chakrabarty,et al.  Aerosol light absorption and its measurement: A review , 2009 .

[29]  S. Friedlander,et al.  The self-preserving particle size distribution for coagulation by brownian motion☆ , 1966 .

[30]  Dieter Braun,et al.  Why molecules move along a temperature gradient , 2006, Proceedings of the National Academy of Sciences.

[31]  T. Charalampopoulos An automated light scattering system and a method for the in situ measurement of the index of refraction of soot particles , 1987 .

[32]  H. Horvath,et al.  UV-VIS-NIR spectral optical properties of soot and soot-containing aerosols , 2003 .

[33]  Ümit Özgür Köylü Quantitative analysis of in situ optical diagnostics for inferring particle/aggregate parameters in flames : Implications for soot surface growth and total emissivity , 1997 .

[34]  T. Bond,et al.  Light Absorption by Carbonaceous Particles: An Investigative Review , 2006 .

[35]  Christopher R. Shaddix,et al.  Measurement of the dimensionless extinction coefficient of soot within laminar diffusion flames , 2007 .

[36]  Fengshan Liu,et al.  Comparison of LII derived soot temperature measurements with LII model predictions for soot in a laminar diffusion flame , 2009 .

[37]  Constantine M. Megaridis,et al.  Morphological Description of Flame-Generated Materials , 1990 .

[38]  L. Lamar,et al.  World Energy Statistics , 1994 .

[39]  J. Mullins,et al.  The optical properties of soot: a comparison between experimental and theoretical values , 1987 .

[40]  Ümit Özgür Köylü,et al.  Range of validity of the Rayleigh-Debye-Gans theory for optics of fractal aggregates. , 1996, Applied optics.

[41]  A. F. Sarofim,et al.  Optical Constants of Soot and Their Application to Heat-Flux Calculations , 1969 .

[42]  C. Megaridis,et al.  Absorption and scattering of light by polydisperse aggregates. , 1991, Applied optics.

[43]  Kirk A. Fuller,et al.  Light Scattering by Agglomerates: Coupled Electric and Magnetic Dipole Method , 1994 .

[44]  C. Koshland,et al.  Inverted co-flow diffusion flame for producing soot , 2005 .

[45]  H. Philipp,et al.  Optical Properties of Graphite , 1965 .

[46]  Takashi Kashiwagi,et al.  Comparisons of the soot volume fraction using gravimetric and light extinction techniques , 1995 .

[47]  Chuen-Jinn Tsai,et al.  The effect of environmental conditions and electrical charge on the weighing accuracy of different filter materials. , 2002, The Science of the total environment.

[48]  Ö. Gülder,et al.  Two-dimensional imaging of soot volume fraction in laminar diffusion flames. , 1999, Applied optics.

[49]  Hsueh-Chia Chang,et al.  Determination of the wavelength dependence of refractive indices of flame soot , 1990, Proceedings of the Royal Society of London. Series A: Mathematical and Physical Sciences.

[50]  S. De Iuliis,et al.  Two-color laser-induced incandescence (2C-LII) technique for absolute soot volume fraction measurements in flames. , 2005, Applied optics.

[51]  C. Sorensen,et al.  Light-scattering measurements of monomer size, monomers per aggregate, and fractal dimension for soot aggregates in flames. , 1992, Applied optics.

[52]  C. Sorensen,et al.  Test of static structure factors for describing light scattering from fractal soot aggregates , 1992 .

[53]  Ernst,et al.  Dynamic scaling in the kinetics of clustering. , 1985, Physical review letters.

[54]  D. E. Rosner,et al.  Fractal Morphology Analysis of Combustion-Generated Aggregates Using Angular Light Scattering and Electron Microscope Images , 1995 .

[55]  M. Schnaiter,et al.  Coating of soot and (NH4)2SO4 particles by ozonolysis products of α-pinene , 2003 .

[56]  V. Ramanathan,et al.  Global and regional climate changes due to black carbon , 2008 .

[57]  P. Greenberg,et al.  Soot volume fraction imaging. , 1997, Applied optics.

[58]  K. Gurton,et al.  Trans-spectral absorption and scattering of electromagnetic radiation by diesel soot. , 1991, Applied optics.

[59]  C. Dasch,et al.  One-dimensional tomography: a comparison of Abel, onion-peeling, and filtered backprojection methods. , 1992, Applied optics.

[60]  Tiago L. Farias,et al.  Fractal and projected structure properties of soot aggregates , 1995 .

[61]  Matthew R. Johnson,et al.  Analysis of uncertainties in instantaneous soot volume fraction measurements using two-dimensional, auto-compensating, laser-induced incandescence (2D-AC-LII) , 2011 .