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1. Stratospheric contribution to the summertime high surface ozone events over the western united states

   https://doi.org/10.1088/1748-9326/abba53  

   Wang, Xinyue; Wu, Yutian; Randel, William; Tilmes, Simone (October 2020, Environmental Research Letters)

   Abstract The stratospheric influence on summertime high surface ozone ( ${\mathrm{O}}_3$) events is examined using a twenty-year simulation from the Whole Atmosphere Community Climate Model. We find that ${\mathrm{O}}_3$transported from the stratosphere makes a significant contribution to the surface ${\mathrm{O}}_3$variability where background surface ${\mathrm{O}}_3$exceeds the 95thpercentile, especially over western U.S. Maximum covariance analysis is applied to ${\mathrm{O}}_3$anomalies paired with stratospheric ${\mathrm{O}}_3$tracer anomalies to identify the stratospheric intrusion and the underlying dynamical mechanism. The first leading mode corresponds to deep stratospheric intrusions in the western and northern tier of the U.S., and intensified northeasterlies in the mid-to-lower troposphere along the west coast, which also facilitate the transport to the eastern Pacific Ocean. The second leading mode corresponds to deep intrusions over the Intermountain Regions. Both modes are associated with eastward propagating baroclinic systems, which are amplified near the end of the North Pacific storm tracks, leading to strong descents over the western U.S. 

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2. Global reconstruction reduces the uncertainty of oceanic nitrous oxide emissions and reveals a vigorous seasonal cycle

   https://doi.org/10.1073/pnas.1921914117  

   Yang, Simon; Chang, Bonnie X.; Warner, Mark J.; Weber, Thomas S.; Bourbonnais, Annie M.; Santoro, Alyson E.; Kock, Annette; Sonnerup, Rolf E.; Bullister, John L.; Wilson, Samuel T.; et al (May 2020, Proceedings of the National Academy of Sciences)

   Assessment of the global budget of the greenhouse gas nitrous oxide ( ${\mathrm{N}}_2$O) is limited by poor knowledge of the oceanic ${\mathrm{N}}_2$O flux to the atmosphere, of which the magnitude, spatial distribution, and temporal variability remain highly uncertain. Here, we reconstruct climatological ${\mathrm{N}}_2$O emissions from the ocean by training a supervised learning algorithm with over 158,000 ${\mathrm{N}}_2$O measurements from the surface ocean—the largest synthesis to date. The reconstruction captures observed latitudinal gradients and coastal hot spots of ${\mathrm{N}}_2$O flux and reveals a vigorous global seasonal cycle. We estimate an annual mean ${\mathrm{N}}_2$O flux of 4.2 ± 1.0 Tg N $\cdot {\mathrm{y}}^{-1}$, 64% of which occurs in the tropics, and 20% in coastal upwelling systems that occupy less than 3% of the ocean area. This ${\mathrm{N}}_2$O flux ranges from a low of 3.3 ± 1.3 Tg N $\cdot {\mathrm{y}}^{-1}$in the boreal spring to a high of 5.5 ± 2.0 Tg N $\cdot {\mathrm{y}}^{-1}$in the boreal summer. Much of the seasonal variations in global ${\mathrm{N}}_2$O emissions can be traced to seasonal upwelling in the tropical ocean and winter mixing in the Southern Ocean. The dominant contribution to seasonality by productive, low-oxygen tropical upwelling systems (>75%) suggests a sensitivity of the global ${\mathrm{N}}_2$O flux to El Niño–Southern Oscillation and anthropogenic stratification of the low latitude ocean. This ocean flux estimate is consistent with the range adopted by the Intergovernmental Panel on Climate Change, but reduces its uncertainty by more than fivefold, enabling more precise determination of other terms in the atmospheric ${\mathrm{N}}_2$O budget. 

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3. Estimating future climate change impacts on human mortality and crop yields via air pollution

   https://doi.org/10.1073/pnas.2400117121  

   Murray, Lee T; Leibensperger, Eric M; Mickley, Loretta J; Tai, Amos; P_K (September 2024, Proceedings of the National Academy of Sciences)

   Future climate change may bring local benefits or penalties to surface air pollution, resulting from changing temperature, precipitation, and transport patterns, as well as changes in climate-sensitive natural precursor emissions. Here, we estimate the climate penalties and benefits at the end of this century with regard to surface ozone and fine particulate matter (PM ${}_{2.5}$; excluding dust and smoke) using a one-way offline coupling between a general circulation model and a global 3-D chemical-transport model. We archive meteorology for the present day (2005 to 2014) and end of this century (2090 to 2099) for seven future scenarios developed for Phase 6 of the Coupled Model Intercomparison Project. The model isolates the impact of forecasted anthropogenic precursor emission changes versus that of climate-only driven changes on surface ozone and PM ${}_{2.5}$for scenarios ranging from extreme mitigation to extreme warming. We then relate these changes to impacts on human mortality and crop production. We find ozone penalties over nearly all land areas with increasing warming. We find net benefits due to climate-driven changes in PM ${}_{2.5}$in the Northern Extratropics, but net penalties in the Tropics and Southern Hemisphere, where most population growth is forecast for the coming century. 

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4. Ultrasensitive multispecies spectroscopic breath analysis for real-time health monitoring and diagnostics

   https://doi.org/10.1073/pnas.2105063118  

   Liang, Qizhong; Chan, Ya-Chu; Changala, P. Bryan; Nesbitt, David J.; Ye, Jun; Toscano, Jutta (October 2021, Proceedings of the National Academy of Sciences)

   Breath analysis enables rapid, noninvasive diagnostics, as well as long-term monitoring of human health, through the identification and quantification of exhaled biomarkers. Here, we demonstrate the remarkable capabilities of mid-infrared (mid-IR) cavity-enhanced direct-frequency comb spectroscopy (CE-DFCS) applied to breath analysis. We simultaneously detect and monitor as a function of time four breath biomarkers— ${\mathrm{C}\mathrm{H}}_3$OH, ${\mathrm{C}\mathrm{H}}_4$, ${\mathrm{H}}_2$O, and HDO—as well as illustrate the feasibility of detecting at least six more ( ${\mathrm{H}}_2$CO, ${\mathrm{C}}_2{\mathrm{H}}_6$, OCS, ${\mathrm{C}}_2{\mathrm{H}}_4$, ${\mathrm{C}\mathrm{S}}_2$, and ${\mathrm{N}\mathrm{H}}_3$) without modifications to the experimental apparatus. We achieve ultrahigh detection sensitivity at the parts-per-trillion level. This is made possible by the combination of the broadband spectral coverage of a frequency comb, the high spectral resolution afforded by the individual comb teeth, and the sensitivity enhancement resulting from a high-finesse cavity. Exploiting recent advances in frequency comb, optical coating, and photodetector technologies, we can access a large variety of biomarkers with strong carbon–hydrogen-bond spectral signatures in the mid-IR. 

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5. Structural phase purification of bulk HfO ₂ :Y through pressure cycling

   https://doi.org/10.1073/pnas.2312571121  

   Musfeldt, J. L.; Singh, Sobhit; Fan, Shiyu; Gu, Yanhong; Xu, Xianghan; Cheong, S.-W.; Liu, Z.; Vanderbilt, David; Rabe, Karin M. (January 2024, Proceedings of the National Academy of Sciences)

   We combine synchrotron-based infrared absorption and Raman scattering spectroscopies with diamond anvil cell techniques and first-principles calculations to explore the properties of hafnia under compression. We find that pressure drives HfO ${}_2$:7%Y from the mixed monoclinic ( $P{2}_1/c$) $+$antipolar orthorhombic ( $\mathit{Pbca}$) phase to pure antipolar orthorhombic ( $\mathit{Pbca}$) phase at approximately 6.3 GPa. This transformation is irreversible, meaning that upon release, the material is kinetically trapped in the $\mathit{Pbca}$metastable state at 300 K. Compression also drives polar orthorhombic ( $Pca{2}_1$) hafnia into the tetragonal ( $P{4}_2/nmc$) phase, although the latter is not metastable upon release. These results are unified by an analysis of the energy landscape. The fact that pressure allows us to stabilize targeted metastable structures with less Y stabilizer is important to preserving the flat phonon band physics of pure HfO ${}_2$. 

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