2015
DOI: 10.1021/jacs.5b08636
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Relative Order of Sulfuric Acid, Bisulfate, Hydronium, and Cations at the Air–Water Interface

Abstract: Sulfuric acid (H2SO4), bisulfate (HSO4(-)), and sulfate (SO4(2-)) are among the most abundant species in tropospheric and stratospheric aerosols due to high levels of atmospheric SO2 emitted from biomass burning and volcanic eruptions. The air/aqueous interfaces of sulfuric acid and bisulfate solutions play key roles in heterogeneous reactions, acid rain, radiative balance, and polar stratospheric cloud nucleation. Molecular-level knowledge about the interfacial distribution of these inorganic species and thei… Show more

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Cited by 49 publications
(72 citation statements)
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“…The samples studied were the surfaces of hydrogen halide solutions probed by a broadband PS-SFVS setup (24,29) with S-, S-, and P-(SSP-) polarized SF, visible, and IR fields (see (14,15,30), whereas high precision of our measurements allows discernment of the ion-induced spectral changes on the millimolar level.…”
Section: Experiments and Theorymentioning
confidence: 99%
“…The samples studied were the surfaces of hydrogen halide solutions probed by a broadband PS-SFVS setup (24,29) with S-, S-, and P-(SSP-) polarized SF, visible, and IR fields (see (14,15,30), whereas high precision of our measurements allows discernment of the ion-induced spectral changes on the millimolar level.…”
Section: Experiments and Theorymentioning
confidence: 99%
“…Interestingly, experiments reporting Imχ (2) (ω) measured for the air-water interface in acidic conditions, either in presence of HCl, HI or H 2 SO 4 electrolytes [32,33], have reported a decrease in amplitude of the signal in the 3000-3600 cm −1 frequency range with respect to the neat interface. This is indeed what our simulations provide (one cation at the interface), see the total SFG signals for the two interfaces at the bottom of Figure 5.…”
Section: System L0 L1 L2 L3 Intra-2dnmentioning
confidence: 99%
“…The need to revisit this highly investigated acidic air-water interface stems from the fact that definitive conclusions on how protons affect the water arrangement in the BIL are still missing from the literature, while the enrichment/depletion in protons at the interface is still a matter of on-going debate within the scientific community: SFG [32][33][34] and Second Harmonic Generation (SHG) [35,36] spectroscopies suggest a higher propensity for the hydronium ion to bind to the surface, while electrokinetic experiments point towards a basic air-water interface [37][38][39][40][41][42][43]. Many theoretical investigations have also been dedicated to this topic, see e.g., the recent work and review from the Hassanali group [38], with conclusions ranging from a strong preference of protons for the interface [38] to a little or negligible preference of protons for the interface [39,40].…”
Section: Introductionmentioning
confidence: 99%
“…The adsorption of anions on hydrophobic interfaces controls important chemistry on aerosol surfaces and determines the stability of proteins, colloids and foams in a wide variety of environmental, physiological and engineered settings. Anion adsorption on the air/water interface, the paradigmatic hydrophobic surface, has been particularly well studied 1 11 . Perhaps the simplest question one can ask of this system is the following: Is anion adsorption at the air/water interface thermodynamically favourable?…”
Section: Introductionmentioning
confidence: 99%