Biomass combustion produces black carbon (BC) and brown carbon (BrC) aerosols that contribute substantially to warming the Earth’s atmosphere. Accurate knowledge of their emissions and absorption per unit mass (mass absorption cross-section; MAC) can be used to quantify the radiative impact of these combustion products. We isolated particles generated from laboratory biomass burning fires by morphology and found that some particles from biomass burning do not correspond to either BC or BrC according to common operational definitions. Unlike BrC, these particles strongly absorb red light, with a MAC and spectral dependence of absorption between that of BrC and BC. They also have intermediate volatility: they survive thermodenuding at 250 °C but do not heat to incandescence in a single particle soot photometer (SP2) instrument. We also found evidence for intermediate properties in ambient wildfire smoke from the 2013 Rim Fire in California. More work is needed to understand how much this intermediate material contributes to atmospheric light absorption from typical combustion, whether or not it corresponds to “tar balls”, and how it may affect previous MAC measurements that were attributed to enhanced absorption by transparent coatings.
The development of interband cascade lasers (ICLs) has made the strong C-H transitions in the 3 μm spectral region increasingly accessible. We present the demonstration of a single mode distributed feedback ICL coupled to a V-shaped optical cavity in an optical feedback cavity-enhanced absorption spectroscopy (OF-CEAS) experiment. We achieved a minimum detectable absorption coefficient, αmin, of cm−1 for a spectrum of CH4 at 3.24 μm with a two second acquisition time (100 scans averaged). This corresponds to a detection limit of 3 ppb CH4 at atmospheric pressure, which is comparable to previously reported OF-CEAS instruments with diode lasers or quantum cascade lasers. The ability to frequency lock an ICL source in the important 3 μm region to an optical cavity holds great promise for future spectroscopic applications.
Particle morphology is an important parameter affecting aerosol optical properties that are relevant to climate and air quality, yet it is poorly constrained due to sparse in situ measurements. Biomass burning is a large source of aerosol that generates particles with different morphologies. Quantifying the optical contributions of non-spherical aerosol populations is critical for accurate radiative transfer models, and for correctly interpreting remote sensing data. We deployed a laser imaging nephelometer at the Missoula Fire Sciences Laboratory to sample biomass burning aerosol from controlled fires during the FIREX intensive laboratory study. The laser imaging nephelometer measures the unpolarized scattering phase function of an aerosol ensemble using diode lasers at 375 and 405 nm. Scattered light from the bulk aerosol in the instrument is imaged onto a charge-coupled device (CCD) using a wide-angle field-of-view lens, which allows for measurements at 4–175∘ scattering angle with ∼ 0.5∘ angular resolution. Along with a suite of other instruments, the laser imaging nephelometer sampled fresh smoke emissions both directly and after removal of volatile components with a thermodenuder at 250 ∘C. The total integrated aerosol scattering signal agreed with both a cavity ring-down photoacoustic spectrometer system and a traditional integrating nephelometer within instrumental uncertainties. We compare the measured scattering phase functions at 405 nm to theoretical models for spherical (Mie) and fractal (Rayleigh–Debye–Gans) particle morphologies based on the size distribution reported by an optical particle counter. Results from representative fires demonstrate that particle morphology can vary dramatically for different fuel types. In some cases, the measured phase function cannot be described using Mie theory. This study demonstrates the capabilities of the laser imaging nephelometer instrument to provide realtime, in situ information about dominant particle morphology, which is vital for understanding remote sensing data and accurately describing the aerosol population in radiative transfer calculations.