The dual carbon isotope signatures and optical properties of carbonaceous aerosols have been investigated simultaneously for the first time in the South Asian outflow during an intensive campaign at the Maldives Climate Observatory on Hanimaadhoo (MCOH) (February and March 2012). As one component of the Cloud Aerosol Radiative Forcing Dynamics Experiment, this paper reports on the sources and the atmospheric processing of elemental carbon (EC) and water‐soluble organic carbon (WSOC) as examined by a dual carbon isotope approach. The radiocarbon (Δ¹⁴C) data show that WSOC has a significantly higher biomass/biogenic contribution (86 ± 5%) compared to EC (59 ± 4%). The more ¹³C‐enriched signature of MCOH‐WSOC (−20.8 ± 0.7‰) compared to MCOH‐EC (−25.8 ± 0.3‰) and megacity Delhi WSOC (−24.1 ± 0.9‰) suggests that WSOC is significantly more affected by aging during long‐range transport than EC. The δ¹³C‐Δ¹⁴C signal suggests that the wintertime WSOC intercepted over the Indian Ocean largely represents aged primary biomass burning aerosols. Since light‐absorbing organic carbon aerosols (Brown Carbon (BrC)) have recently been identified as potential contributors to positive radiative forcing, optical properties of WSOC were also investigated. The mass absorption cross section of WSOC (MAC₃₆₅) was 0.5 ± 0.2 m² g⁻¹ which is lower than what has been observed at near‐source sites, indicating a net decrease of WSOC light‐absorption character during long‐range transport. Near‐surface WSOC at MCOH accounted for ~1% of the total direct solar absorbance relative to EC, which is lower than the BrC absorption inferred from solar spectral observations of ambient aerosols, suggesting that a significant portion of BrC might be included in the water‐insoluble portion of organic aerosols.

Wildfires contribute significantly to global soot emissions, yet their aerosol formation mechanisms and resulting particle properties are poorly understood and parameterized in climate models. The conventional view holds that soot is formed via the cluster-dilute aggregation mechanism in wildfires and emitted as aggregates with fractal dimension Df [ap] 1.8 mobility diameter Dm [le] 1[emsp14][mgr]m, and aerodynamic diameter Da [le] 300[emsp14]nm. Here we report the ubiquitous presence of soot superaggregates (SAs) in the outflow from a major wildfire in India. SAs are porous, low-density aggregates of cluster-dilute aggregates with characteristic Df [ap] 2.6, Dm > 1[emsp14][mgr]m, and Da [le] 300[emsp14]nm that form via the cluster-dense aggregation mechanism. We present additional observations of soot SAs in wildfire smoke-laden air masses over Northern California, New Mexico, and Mexico City. We estimate that SAs contribute, per unit optical depth, up to 35% less atmospheric warming than freshly-emitted (Df [ap] 1.8) aggregates, and [ap]90% more warming than the volume-equivalent spherical soot particles simulated in climate models.

Light-absorbing organic carbon aerosol – colloquially known as brown carbon (BrC) – is emitted from combustion processes and has a brownish or yellowish visual appearance, caused by enhanced light absorption at shorter visible and ultraviolet wavelengths (0.3 µm≲λ≲0.5 µm). Recently, optical properties of atmospheric BrC aerosols have become the topic of intense research, but little is known about how BrC deposition onto snow surfaces affects the spectral snow albedo, which can alter the resulting radiative forcing and in-snow photochemistry. Wildland fires in close proximity to the cryosphere, such as peatland fires that emit large quantities of BrC, are becoming more common at high latitudes, potentially affecting nearby snow and ice surfaces. In this study, we describe the artificial deposition of BrC aerosol with known optical, chemical, and physical properties onto the snow surface, and we monitor its spectral radiative impact and compare it directly to modeled values. First, using small-scale combustion of Alaskan peat, BrC aerosols were artificially deposited onto the snow surface. UV–Vis absorbance and total organic carbon (TOC) concentration of snow samples were measured for samples with and without artificial BrC deposition. These measurements were used to first derive a BrC (mass) specific absorption (m² g⁻¹) across the UV–Vis spectral range. We then estimate the imaginary part of the refractive index of deposited BrC aerosol using a volume mixing rule. Single-particle optical properties were calculated using Mie theory, and these values were used to show that the measured spectral snow albedo of snow with deposited BrC was in general agreement with modeled spectral snow albedo using calculated BrC optical properties. The instantaneous radiative forcing per unit mass of total organic carbon deposited to the ambient snowpack was found to be 1.23 ($+\mathrm{0.14}/-\mathrm{0.11}$ ) W m⁻² per part per million (ppm). We estimate the same deposition onto a pure snowpack without light-absorbing impurities would have resulted in an instantaneous radiative forcing per unit mass of 2.68 ($+\mathrm{0.27}/-\mathrm{0.22}$ ) W m⁻² per ppm of BrC deposited.

The broadband surface albedo of snow can greatly be reduced by the deposition of light-absorbing impurities, such as black carbon on or near its surface. Such a reduction increases the absorption of solar radiation and may initiate or accelerate snowmelt and snow albedo feedback. Coincident measurements of both black carbon concentration and broadband snow albedo may be difficult to obtain in field studies; however, using the relationship developed in this simple model sensitivity study, black carbon mass densities deposited can be estimated from changes in measured broadband snow albedo, and vice versa. Here, the relationship between the areal mass density of black carbon found near the snow surface to the amount of albedo reduction was investigated using the popular snow radiative transfer model Snow, Ice, and Aerosol Radiation (SNICAR). We found this relationship to be linear for realistic amounts of black carbon mass concentrations, such as those found in snow at remote locations. We applied this relationship to measurements of broadband albedo in the Chilean Andes to estimate how vehicular emissions contributed to black carbon (BC) deposition that was previously unquantified.

We report the experimental realization of continuous carbon aerogel production using a flame aerosol reactor by operating it in negative gravity (−g; up-side-down configuration). Buoyancy opposes the fuel and air flow forces in −g, which eliminates convectional outflow of nanoparticles from the flame and traps them in a distinctive non-tipping, flicker-free, cylindrical flame body, where they grow to millimeter-size aerogel particles and gravitationally fall out. Computational fluid dynamics simulations show that a closed-loop recirculation zone is set up in −g flames, which reduces the time to gel for nanoparticles by ≈10⁶ s, compared to positive gravity (upward rising) flames. Our results open up new possibilities of one-step gas-phase synthesis of a wide variety of aerogels on an industrial scale.

Deposition of light-absorbing aerosol on snow can drastically change the albedo of the snow surface and the energy balance of the snowpack. To study these important effects experimentally and to compare them with theory, it is desirable to have an apparatus for such deposition experiments. Here, we describe a simple apparatus to generate and evenly deposit light-absorbing aerosols onto a flat snow surface. Aerosols are produced (combustion aerosols) or entrained (mineral dust aerosols) and continuously transported into a deposition chamber placed on the snow surface where they deposit onto and into the snowpack, thereby modifying its surface reflectance and albedo. We demonstrate field operation of this apparatus by generating black and brown carbon combustion aerosols and entraining hematite mineral dust aerosol and depositing them on the snowpack. Changes in spectral snow reflectance are demonstrated qualitatively through pictures of snow surfaces after aerosol deposition and quantitatively by measuring hemispherical-conical reflectance spectra for the deposited areas and for adjacent snowpack in its natural state. Additional potential applications for this apparatus are mentioned and briefly discussed.