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Novel techniques and applications in single particle mass spectrometry /

  • Author(s): Cahill, John Francis
  • et al.

In the environment, aerosol particles can affect climate directly though scattering and absorbing radiation and indirectly by influencing cloud formation, albedo, and lifetime. Beyond the environment, aerosols are commonly used as a delivery mechanism for a variety of products, such as inhalers and spray paints. Chemically characterizing aerosols is a difficult endeavor, and relatively few instrumental methods are capable of doing so. A unique subset of instrumentation and techniques exist to measure aerosol chemical and physical properties. Among these, the aerosol time-of-flight mass spectrometer (ATOFMS) can measure single particle chemistry and size in real time. The ATOFMS was developed for the study atmospheric aerosols, and data acquired by the ATOFMS over the years since its creation has provided significant insight into many atmospheric phenomena; however, the application of this technique into disciplines other than atmospheric chemistry has been relatively unexplored. In this dissertation the ATOFMS is used in a conventional sense, to provide insight into atmospheric particle chemistry through two field studies in California, but also in an unconventional way by using the ATOFMS to answer outstanding questions in other disciplines, including nanomaterials and biochemistry. Often the chemistry of a single unit, rather than of the bulk, is needed in these disciplines, and the ATOFMS is uniquely suited to provide this information. The ATOFMS was used to chemically characterize single particles of a unique class of nanomaterials, called metal organic frameworks (MOFs), comprised of functionalized organic linkers and metal ions or metal ion clusters. ATOFMS data was able to show the presence of MOFs with mixed functionality, and show the exchange of functional groups between materials. Cell processes can be monitored by measuring small molecules that are part of cell metabolism, which can provide insight into cell functions, environment, and disease. Using an ATOFMS with a modified aerodynamic lens inlet, single microalgae cells 4-10 µm in diameter of various types have been be characterized. Compared to other single cell mass spectrometry techniques, the modified ATOFMS has unprecedented throughput, up to 50 Hz. Time-resolved measurements of cells undergoing nitrogen deprivation further highlight the abilities of the technique for single cell analysis

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