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  1. Free, publicly-accessible full text available December 1, 2023
  2. Free, publicly-accessible full text available October 1, 2023
  3. Abstract Understanding the chemical and physical properties of particles is an important scientific, engineering, and medical issue that is crucial to air quality, human health, and environmental chemistry. Of special interest are aerosol particles floating in the air for both indoor virus transmission and outdoor atmospheric chemistry. The growth of bio- and organic-aerosol particles in the air is intimately correlated with chemical structures and their reactions in the gas phase at aerosol particle surfaces and in-particle phases. However, direct measurements of chemical structures at aerosol particle surfaces in the air are lacking. Here we demonstrate in situ surface-specific vibrational sum frequency scattering (VSFS) to directly identify chemical structures of molecules at aerosol particle surfaces. Furthermore, our setup allows us to simultaneously probe hyper-Raman scattering (HRS) spectra in the particle phase. We examined polarized VSFS spectra of propionic acid at aerosol particle surfaces and in particle bulk. More importantly, the surface adsorption free energy of propionic acid onto aerosol particles was found to be less negative than that at the air/water interface. These results challenge the long-standing hypothesis that molecular behaviors at the air/water interface are the same as those at aerosol particle surfaces. Our approach opens a new avenue inmore »revealing surface compositions and chemical aging in the formation of secondary organic aerosols in the atmosphere as well as chemical analysis of indoor and outdoor viral aerosol particles.« less
    Free, publicly-accessible full text available December 1, 2023
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  5. Abstract The basal level of the plant defense hormone jasmonate (JA) in unstressed leaves is low, but wounding causes its near instantaneous increase. How JA biosynthesis is initiated is uncertain, but the lipolysis step that generates fatty acid precursors is generally considered to be the first step. Here, we used a series of physiological, pharmacological, genetic, and kinetic analyses of gene expression and hormone profiling to demonstrate that the early spiking of JA upon wounding does not depend on the expression of JA biosynthetic genes in Arabidopsis (Arabidopsis thaliana). Using a transgenic system, we showed how decoupling the responses to wounding and JA prevents the perpetual synthesis of JA in wounded leaves. We then used DEFECTIVE IN ANTHER DEHISCENCE1 (DAD1) as a model wound-responsive lipase to demonstrate that although its transient expression in leaves can elicit JA biosynthesis to a low level, an additional level of activation is triggered by wounding, which causes massive accumulation of JA. This wound-triggered boosting effect of DAD1-mediated JA synthesis can happen directly in damaged leaves or indirectly in undamaged remote leaves by the systemically transmitted wound signal. Finally, protein stability of DAD1 was influenced by wounding, α-linolenic acid, and mutation in its catalytic site.more »Together, the data support mechanisms that are independent of gene transcription and translation to initiate the rapid JA burst in wounded leaves and demonstrate how transient expression of the lipase can be used to reveal changes occurring at the level of activity and stability of the key lipolytic step.« less
    Free, publicly-accessible full text available April 11, 2023
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