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Abstract. Pyrocumulonimbus clouds (pyroCbs) generated by intense wildfires can serve as a direct pathway for the injection of aerosols and gaseous pollutants into the lower stratosphere, resulting in significant chemical, radiative, and dynamical changes. Canada experienced an extremely severe wildfire season in 2023, with a total area burned that substantially exceeded those of previous events known to have impacted the stratosphere (such as the 2020 Australian fires). This season also had record-high pyroCb activity, which raises the question of whether the 2023 Canadian event resulted in significant stratospheric perturbations. Here, we investigate this anomalous wildfire season using retrievals from multiple satellite instruments, ACE-FTS (Atmospheric Chemistry Experiment – Fourier transform spectrometer), OMPS LP (Ozone Mapping and Profiler Suite Limb Profiler), and MLS (Microwave Limb Sounder), to determine the vertical extents of the wildfire smoke along with chemical signatures of biomass burning. These data show that smoke primarily reached the upper troposphere, and only a nominal amount managed to penetrate the tropopause. Only a few ACE-FTS occultations captured elevated abundances of biomass-burning products in the lowermost stratosphere. OMPS LP aerosol measurements also indicate that any smoke that made it past the tropopause did not last long enough or reach high enough to significantly perturb stratospheric composition. While this work focuses on Canadian wildfires given the extensive burned area, pyroCbs at other longitudes (e.g., Siberia) are also captured in the compositional analysis. These results highlight that despite the formation of many pyroCbs in major wildfires, those capable of penetrating the tropopause are extremely rare; this in turn means that even a massive area burned is not necessarily an indicator of stratospheric effects.more » « less
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Seo, Jinyoung; Ukani, Rahil; Zheng, Juanjuan; Braun, Jason D.; Wang, Sicheng; Chen, Faith E.; Kim, Hong Ki; Zhang, Selena; Thai, Catherine; McGillicuddy, Ryan D.; et al (, Journal of the American Chemical Society)Barocaloric effects─solid-state thermal changes induced by the application and removal of hydrostatic pressure─offer the potential for energy-efficient heating and cooling without relying on volatile refrigerants. Here, we report that dialkylammonium halides─organic salts featuring bilayers of alkyl chains templated through hydrogen bonds to halide anions─display large, reversible, and tunable barocaloric effects near ambient temperature. The conformational flexibility and soft nature of the weakly confined hydrocarbons give rise to order–disorder phase transitions in the solid state that are associated with substantial entropy changes (>200 J kg–1 K–1) and high sensitivity to pressure (>24 K kbar–1), the combination of which drives strong barocaloric effects at relatively low pressures. Through high-pressure calorimetry, X-ray diffraction, and Raman spectroscopy, we investigate the structural factors that influence pressure-induced phase transitions of select dialkylammonium halides and evaluate the magnitude and reversibility of their barocaloric effects. Furthermore, we characterize the cyclability of thin-film samples under aggressive conditions (heating rate of 3500 K s–1 and over 11,000 cycles) using nanocalorimetry. Taken together, these results establish dialkylammonium halides as a promising class of pressure-responsive thermal materials.more » « less
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