8 research outputs found
Exploring the Atmosphere of Neoproterozoic Earth: The Effect of O on Haze Formation and Composition
Previous studies of haze formation in the atmosphere of the Early Earth have
focused on N/CO/CH atmospheres. Here, we experimentally
investigate the effect of O on the formation and composition of aerosols
to improve our understanding of haze formation on the Neoproterozoic Earth. We
obtained in situ size, particle density, and composition measurements of
aerosol particles produced from N/CO/CH/O gas mixtures
subjected to FUV radiation (115-400 nm) for a range of initial
CO/CH/O mixing ratios (O ranging from 2 ppm to 0.2\%).
At the lowest O concentration (2 ppm), the addition increased particle
production for all but one gas mixture. At higher oxygen concentrations (20 ppm
and greater) particles are still produced, but the addition of O
decreases the production rate. Both the particle size and number density
decrease with increasing O, indicating that O affects particle
nucleation and growth. The particle density increases with increasing O.
The addition of CO and O not only increases the amount of oxygen in
the aerosol, but it also increases the degree of nitrogen incorporation. In
particular, the addition of O results in the formation of nitrate bearing
molecules. The fact that the presence of oxygen bearing molecules increases the
efficiency of nitrogen fixation has implications for the role of haze as a
source of molecules required for the origin and evolution of life. The
composition changes also likely affect the absorption and scattering behavior
of these particles but optical properties measurements are required to fully
understand the implications for the effect on the planetary radiative energy
balance and climate.Comment: 15 pages, 3 tables, 8 figures, accepted in Astrophysical Journa
Stable Isotope Fractionation in Titan Aerosol Formation
Stable isotope ratio measurements are a powerful tool used to understand both ancient and modern planetary processes. Instruments on the Cassini- Huygens spacecraft along with ground-based observations have measured several isotope pairs, including C-13/C-12 and N-15/N-14, in Titan's atmosphere. This includes isotopic measurements of the major atmospheric species, CH4 and N2, along with HCN, HC3N, C2H2. C2H6 and C4H2. However, the isotopic fractionation of Titan's organic aerosol has not conclusively been measured and therefore the effect of aerosol formation as an isotopic fractionation pathway in Titan's atmosphere has not been considered. Laboratory studies have measured the carbon and/or nitrogen isotopic fractionation of Titan aerosol analogs. [18] found that the carbon fractionation of photochemical organic aerosol analogs are more enriched in C-13. This enrichment in the aerosol analogs is opposite of what is predicted for photochemical products by the kinetic isotope effect. Additionally, both [16] and [18] found that the nitrogen fractionation in the organic aerosol analogs are opposite of what is observed in Titan's atmospheric N2 and HCN, with the aerosol analogs being a light nitrogen sink. Here we monitor the gas phase during photochemical aerosol analog production as a function of reaction time. In a recirculation experiment, the isotopic fractionation of carbon within the gas-phase products is measured as the CH4 reservoir is depleted. This allows us to monitor the isotopic fractionation pathway during photochemical aerosol analog formation
Visualizing Nanoparticle Dissolution by Imaging Mass Spectrometry
We
demonstrate the ability to visualize nanoparticle dissolution
while simultaneously providing chemical signatures that differentiate
between citrate-capped silver nanoparticles (AgNPs), AgNPs forced
into dissolution via exposure to UV radiation, silver nitrate (AgNO<sub>3</sub>), and AgNO<sub>3</sub>/citrate deposited from aqueous solutions
and suspensions. We utilize recently developed inkjet printing (IJP)
protocols to deposit the different solutions/suspensions as NP aggregates
and soluble species, which separate onto surfaces <i>in situ</i>, and collect mass spectral imaging data <i>via</i> time-of-flight
secondary ion mass spectrometry (TOF-SIMS). Resulting 2D Ag<sup>+</sup> chemical images provide the ability to distinguish between the different
Ag-containing starting materials and, when coupled with mass spectral
peak ratios, provide information-rich data sets for quick and reproducible
visualization of NP-based aqueous constituents. When compared to other
measurements aimed at studying NP dissolution, the IJP-TOF-SIMS approach
offers valuable information that can potentially help in understanding
the complex equilibria in NP-containing solutions and suspensions,
including NP dissolution kinetics and extent of overall dissolution