The method and apparatus of laser-induced incandescence (LII) to analyze characteristics of submicron-sized particles are described. LII is recognized as a good tool for determining the characteristics of small particles in a gas, e.g., volume fraction, particle size, and specific surface area. It uses the fact that the incandescence signal is proportional to the volume of the particles. It also uses the fact that transient cooling is dependent on the specific surface area of the particle, which is related to diameter of the particle. In LII, particles are heated by a pulsed laser light beam to a temperature where incandescence from the particles can be distinguished from ambient light. The temperature of particles and their volume fraction governs the incandescence. The temperature decay rate is proportional to the primary particle size. The invention uses an optical arrangement that ensures a near-uniform laser energy distribution spatial profile. The invention also uses a low fluence laser beam pulse to avoid evaporation of particles. Without significant evaporation and with a uniform energy profile, accurate and precise measurements can be conducted more easily and reliably.

The influence of pressure on laser-induced incandescence (LII) is investigated systematically in premixed, laminar, sooting ethylene /air flames at 1-15 bar with wavelength-, laser fluence-, and time-resolved detection. In the investigated pressure range the LII signal decay rate is proportional to pressure. This observation is consistent with the prediction of heat-transfer models in the free-molecular regime. Pressure does not systematically affect the relationship between LII signal and laser fluence. With appropriate detection timing the pressure influence on LII signal "s proportionality to soot volume fraction obtained by extinction measurements is only minor compared with the variation observed in different flames at fixed pressures. The implications for particle sizing and soot volume fraction measurements using LII techniques at elevated pressures are discussed.

The influence of pressure on laser-induced incandescence (LII) is investigated systematically in premixed, laminar, sooting ethylene/air flames at 1-15 bar with wavelength-, laser fluence-, and time-resolved detection. In the investigated pressure range the LII signal decay rate is proportional to pressure. This observation is consistent with the prediction of heat-transfer models in the free-mol. regime. Pressure does not systematically affect the relation between LII signal and laser fluence. With appropriate detection timing the pressure influence on LII signal’s proportionality to soot vol. fraction obtained by extinction measurements is only minor compared with the variation obsd. in different flames at fixed pressures. The implications for particle sizing and soot vol. fraction measurements using LII techniques at elevated pressures are discussed.

We present a data set for testing models of time-resolved laser-induced incandescence of soot. Measurements were made in a laminar ethene diffusion flame over a wide range of laser fluences at 532 nm. The laser was seeded to provide a smooth temporal profile, and the beam was spatially filtered and imaged into the flame to provide a homogeneous spatial profile. The particle incandescence was imaged onto a fast photodiode. The measurements are compared with the standard Melton model and with a new model that incorporates physical mechanisms not included in the Melton model.

This paper describes a model for analyzing and predicting the temporal behavior of laser-induced incandescence (LII) from combustion-generated soot, carbon black, and other carbonaceous particles on a nanosecond time scale. The model accounts for particle heating by absorption of light from a pulsed laser and cooling by sublimation, conduction, and radiation. The model also includes mechanisms for oxidation, melting, and annealing of the particles and nonthermal photodesorption of carbon clusters from the particle surface. At fluences above 0.1 J/cm2, particle temperatures during the laser pulse are determined by the balance between absorption and sublimation, whereas at lower fluences particle temperatures do not reach the sublimation temperature, and temperatures are predominantly controlled by absorption and conduction. After the laser pulse, temperatures are predominantly controlled by conductive cooling rates. Oxidative heating may compete with conductive cooling on these time scales. Annealing of the particles to a more ordered phase of carbon is predicted to occur at fluences as low as 0.02 J/cm2. Annealing may strongly influence sublimation rates, and changes in emissivity during annealing are predicted to increase signal decay rates. Supersonic expansion of the carbon clusters sublimed from the surface is calculated to occur at fluences above 0.12 J/cm2. When compared with LII measurements recorded in a flame at atmospheric pressure, the model reproduces the shapes and relative magnitudes of LII temporal profiles over a wide range of laser fluences. Comparisons between model predictions and experimental observations suggest that the particles do not melt at laser fluences that lead to melting of bulk graphite. These comparisons also indicate that the energy released during particle annealing is much smaller than that released during annealing of neutron- or electron-irradiated graphite. Despite good agreement between model and experimental results, large uncertainties exist for input parameters used to calculate annealing rates and rates of oxidation, conduction, absorption, emission, and photolytic desorption of carbon clusters for both the initial and annealed particles.

The UV-VIS-NIR spectral optical properties of soot and soot containing aerosols were investigated in detail during the AIDA Soot Aerosol Campaign 1999. One aim of the campaign was a comprehensive comparison of the microphysical properties of Diesel and spark generator soot. The mass specific extinction cross section at λ=450 nm of Diesel soot is 10.6±0.5 m2 g−1 which is almost a factor of two larger than the corresponding value of 5.7±0.3 m2 g−1 measured for spark generator soot. Coagulation-induced particle growth does not affect the soot extinction cross section and has a weak influence on the scattering properties of the soot aggregates. Atmospheric processing of freshly emitted soot was simulated in mixing experiments. The formation of mixed Diesel soot and dry ammonium sulfate particles by coagulation has only a minor effect on the soot absorption cross section. The coating of spark generated soot with organic material results in a strong increase of the single scattering albedo. A significant increase of the absorption coefficient at λ=473 nm during the coating process can be attributed to an enhancement of the specific soot absorption cross section by more than 30%.

A comparison of scanning mobility particle sizer (SMPS) and laser-induced incandescence (LII) measurements of diesel particulate matter (PM) was performed. The results reveal the significance of the aggregate nature of diesel PM on interpretation of size and volume fraction measurements obtained with an SMPS, and the accuracy of primary particle size measurements by LII. Volume fraction calculations based on the mobility diameter measured by the SMPS substantially over-predict the space-filling volume fraction of the PM. Correction algorithms for the SMPS measurements, to account for the fractal nature of the aggregate morphology, result in a substantial reduction in the reported volume. The behavior of the particulate volume fraction, mean and standard deviation of the mobility diameter, and primary particle size are studied as a function of the EGR for a range of steady-state engine speeds and loads for a turbocharged direct-injection diesel engine. Both the SMPS and LII techniques demonstrate good repeatability and consistency with each other. Increasing the EGR results in a sharp rise in the volume fraction of particulates for all engine speeds and loads. At all speed and load conditions the primary particle size decreases with increasing EGR.

A computational study of soot formation in an undilute axisymmetric laminar ethylene-air coflow jet diffusion flame at atmospheric pressure was conducted using a detailed gas-phase reaction mechanism and complex thermal and transport properties. A simple two-equation soot model was employed to predict soot formation, growth, and oxidation with interactions between the soot chemistry and the gas-phase chemistry taken into account. Both the optically thin model and the discrete-ordinates method coupled with a statistical narrow-band correlated-K based wide band model for radiative properties of CO, CO2, H2O, and soot were employed in the calculation of radiation heat transfer to evaluate the adequacy of using the optically thin model. Several calculations were performed with and without radiative transfer of radiating gases and/or soot to investigate their respective effects on the computed soot field and flame structure. Radiative heat transfer by both radiating gases and soot were found to be important in this relatively heavily sooting flame studied. Results of the optically thin radiation model are in good agreement with those obtained using the wide band model except for the flame temperature near the flame tip.

CONTEXT: Associations have been found between day-to-day particulate air pollution and increased risk of various adverse health outcomes, including cardiopulmonary mortality. However, studies of health effects of long-term particulate air pollution have been less conclusive. OBJECTIVE: To assess the relationship between long-term exposure to fine particulate air pollution and all-cause, lung cancer, and cardiopulmonary mortality. DESIGN, SETTING, AND PARTICIPANTS: Vital status and cause of death data were collected by the American Cancer Society as part of the Cancer Prevention II study, an ongoing prospective mortality study, which enrolled approximately 1.2 million adults in 1982. Participants completed a questionnaire detailing individual risk factor data (age, sex, race, weight, height, smoking history, education, marital status, diet, alcohol consumption, and occupational exposures). The risk factor data for approximately 500 000 adults were linked with air pollution data for metropolitan areas throughout the United States and combined with vital status and cause of death data through December 31, 1998. MAIN OUTCOME MEASURE: All-cause, lung cancer, and cardiopulmonary mortality. RESULTS: Fine particulate and sulfur oxide–related pollution were associated with all-cause, lung cancer, and cardiopulmonary mortality. Each 10-microg/m(3) elevation in fine particulate air pollution was associated with approximately a 4%, 6%, and 8% increased risk of all-cause, cardiopulmonary, and lung cancer mortality, respectively. Measures of coarse particle fraction and total suspended particles were not consistently associated with mortality. CONCLUSION: Long-term exposure to combustion-related fine particulate air pollution is an important environmental risk factor for cardiopulmonary and lung cancer mortality.