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Abstract. Secondary inorganic aerosols (sulfate, nitrate, and ammonium, SNA) are major contributors to fine particulate matter. Predicting concentrations of these species is complicated by the cascade of processes that control their abundance, including emissions, chemistry, thermodynamic partitioning, and removal. In this study, we use 11 flight campaigns to evaluate the GEOS-Chem model performance for SNA. Across all the campaigns, the model performance is best for sulfate (R2 = 0.51; normalized mean bias (NMB) = 0.11) and worst for nitrate (R2=0.22; NMB = 1.76), indicating substantive model deficiencies in the nitrate simulation. Thermodynamic partitioning reproduces the total particulate nitrate well (R2=0.79; NMB = 0.09), but actual partitioning (i.e., ε(NO3-)= NO3- / TNO3) is challenging to assess given the limited sets of full gas- and particle-phase observations needed for ISORROPIA II. In particular, ammonia observations are not often included in aircraft campaigns, and more routine measurements would help constrain sources of SNA model bias. Model performance is sensitive to changes in emissions and dry and wet deposition, with modest improvements associated with the inclusion of different chemical loss and production pathways (i.e., acid uptake on dust, N2O5 uptake, and NO3- photolysis). However, these sensitivity tests show only modest reduction in the nitrate bias, with no improvement to the model skill (i.e., R2), implying that more work is needed to improve the description of loss and production of nitrate and SNA as a whole.
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Inspired Beyond Nature: Three Decades of Spherical Nucleic Acids and Colloidal Crystal Engineering with DNA
The conception, synthesis, and invention of a nanostructure, now known as the spherical nucleic acid, or SNA, in 1996 marked the advent of a new field of chemistry. Over the past three decades, the SNA and its analogous anisotropic equivalents have provided an avenue for us to think about some of the most fundamental concepts in chemistry in new ways and led to technologies that are significantly impacting fields from medicine to materials science. A prime example is colloidal crystal engineering with DNA, the framework for using SNAs and related structures to synthesize programmable matter. Herein, we document the evolution of this framework, which was initially inspired by nature, and describe how it now allows researchers to chart paths to move beyond it, as programmable matter with real-world significance is envisioned and created.
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- Award ID(s):
- 2104353
- PAR ID:
- 10510546
- Publisher / Repository:
- ACS Nano
- Date Published:
- Journal Name:
- ACS Nano
- Volume:
- 17
- Issue:
- 17
- ISSN:
- 1936-0851
- Page Range / eLocation ID:
- 16291 to 16307
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
-
Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1021/acsnano.3c06564
