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The direct air capture (DAC) of CO2 using aqueous solvents is plagued by slow kinetics and interfacial barriers that limit effectiveness in combating climate change. Functionalizing air/aqueous surfaces with charged amphiphiles shows promise in accelerating DAC; however, insight into these interfaces and how they evolve in time remains poorly understood. Specifically, competitive ion interactions between DAC reagents and reaction products feedback onto the interfacial structure, thereby modulating interfacial chemical composition and overall function. In this work, we probe the role of glycine amino acid anions (Gly−), an effective CO2 capture reagent, that promotes the organization of cationic oligomers at air/aqueous interfaces. These surfaces are probed with vibrational sum frequency generation spectroscopy and molecular dynamics simulations. Our findings demonstrate that the competition for surface sites between Gly− and captured carbonaceous anions (HCO3−, CO32−, carbamates) drives changes in surface hydration, which in turn tunes oligomer ordering. This phenomenon is related to a hierarchical ordering of anions at the surface that are electrostatically attracted to the surface and their ability to compete for interfacial water. These results point to new ways to tune interfaces for DAC via stratification of ions based on relative surface propensities and specific ion effects. [ABSTRACT FROM AUTHOR]

The authors make the following additions and corrections to the paper, C. Baiz et al., Vibrational Spectroscopic Map, Vibrational Spectroscopy, and Intermolecular Interaction. Chem. Rev. 2020, 120, 7152?7218. 1. The below funding sources should be added to the Acknowledgments section on pages 7204 and 7205: NHG acknowledges support from the National Science Foundation (CHE-1905395). AT thanks the Advanced Materials for Energy-Water Systems (AMEWS) Center (DE-AC02-06CH11357) for support. Thus, the Acknowledgments should be as follows: This work was supported by IBS-R023-D1 (MC). BB wishes to thank the European Union’s Horizon 2020 under the Marie Sk?odowska-Curie Grant Agreement No. 665778, as well as the National Science Centre, Poland (grant no. 2016/23/P/ST4/01720). CRB acknowledges generous support from the National Science Foundation (CHE-847199, BIO-1815354 ) , the National Ins t i t u tes o f Hea l t h (R35GM133359), and the Welch Foundation (F-1891). NHG acknowledges support from the National Science Foundation (CHE-1905395). MWDH-H and JDH thank the University of Nottingham, Green Chemicals Beacon for funding toward this research. AT thanks the Advanced Materials for Energy-Water Systems (AMEWS) Center (DEAC02-06CH11357) for support. MCT acknowledges support from Department of Energy (DE-SC0018983), National Science Foundation (1552996), and National Institutes of Health (GM114500). AGD would like to thank Prof. Andrei Tokmakoff for discussing amide modes when he was a Ph.D. student. LW acknowledges the support from the National Institutes of Health through Award R01GM130697. SAC acknowledges support from National Science Foundation (CHE-1565471). 2. The affiliations of Minhaeng Cho and Kijeong Kwak on page 7201 should be corrected as follows: Minhaeng Cho ? Center for Molecular Spectroscopy and Dynamics, Institute for Basic Science (IBS), Seoul 02841, Republic of Korea; Department of Chemistry, Korea University, Seoul 02841, Republic of Korea Kijeong Kwac ? Center for Molecular Spectroscopy and Dynamics, Institute for Basic Science (IBS), Seoul 02841, Republic of Korea 3. Reference 329 on page 7214 should be replaced with the following paper: (329) Sul, S; Karaiskaj, D.; Jiang Y.; Ge, N.-H. Conformations of N-Acetyl-L-Prolinamide by Two-Dimensional Infrared Spectroscopy. J. Phys. Chem. B 2006, 110, 19891?19905. 4. A correction in the biography of Magnus Hanson-Heine on page 7203 should be made. MH-H received his Ph.D. in 2014, not 2010.

Vibrational spectroscopy is an essential tool in chemical analyses, biological assays, and studies of functional materials. Over the past decade, various coherent nonlinear vibrational spectroscopic techniques have been developed and enabled researchers to study time-correlations of the fluctuating frequencies that are directly related to solute-solvent dynamics, dynamical changes in molecular conformations and local electrostatic environments, chemical and biochemical reactions, protein structural dynamics and functions, characteristic processes of functional materials, and so on. In order to gain incisive and quantitative information on the local electrostatic environment, molecular conformation, protein structure and interprotein contacts, ligand binding kinetics, and electric and optical properties of functional materials, a variety of vibrational probes have been developed and site-specifically incorporated into molecular, biological, and material systems for time-resolved vibrational spectroscopic investigation. However, still, an all-encompassing theory that describes the vibrational solvatochromism, electrochromism, and dynamic fluctuation of vibrational frequencies has not been completely established mainly due to the intrinsic complexity of intermolecular interactions in condensed phases. In particular, the amount of data obtained from the linear and nonlinear vibrational spectroscopic experiments has been rapidly increasing, but the lack of a quantitative method to interpret these measurements has been one major obstacle in broadening the applications of these methods. Among various theoretical models, one of the most successful approaches is a semiempirical model generally referred to as the vibrational spectroscopic map that is based on a rigorous theory of intermolecular interactions. Recently, genetic algorithm, neural network, and machine learning approaches have been applied to the development of vibrational solvatochromism theory. In this review, we provide comprehensive descriptions of the theoretical foundation and various examples showing its extraordinary successes in the interpretations of experimental observations. In addition, a brief introduction to a newly created repository Web site (http://frequencymap.org) for vibrational spectroscopic maps is presented. We anticipate that a combination of the vibrational frequency map approach and state-of-the-art multidimensional vibrational spectroscopy will be one of the most fruitful ways to study the structure and dynamics of chemical, biological, and functional molecular systems in the future.

We analyze the effect of transparency of past trading volumes in markets where an informed long-lived seller can repeatedly trade with short-lived uninformed buyers. Transparency allows buyers to observe previously sold quantities. In markets with intraperiod monopsony (single buyer each period), transparency reduces welfare if the ex ante expected quality is low but improves welfare if the expected quality is high. The effect is reversed in markets with intraperiod competition (multiple buyers each period). This discrepancy in the efficiency implications of transparency is explained by how buyer competition affects the seller's ability to capture rents, which, in turn, influences market screening. (JEL D40, D82, D83, G14, L15) [ABSTRACT FROM AUTHOR]