Partitioning of Formic and Acetic Acids to the Gas/Aerosol Interface

Qian, Yue; Brown, Jesse B.; Wang, Hui; Huang-Fu, Zhi-Chao; Zhang, Tong; Narouei, Farideh Hosseini; McNeill, V. Faye; Rao, Yi

doi:10.1021/acsearthspacechem.3c00024

Cited by 4 publications

(2 citation statements)

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“…This section outlines the experiments for SHS, ,, ESFS, and VSFS ,, from droplets in the air as well as the difficulty of the experiments which arises from using droplets in air instead of in an emulsion or a planar surface. Additional details can be found in the literature. ,,,,, …”

Section: Second-order Nonlinear Optical Scattering From Droplets In Airmentioning

confidence: 99%

In Situ Probing of the Surface Properties of Droplets in the Air

et al. 2023

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Surface properties of nanodroplets and microdroplets are intertwined with their immense applicability in biology, medicine, production, catalysis, the environment, and the atmosphere. However, many means for analyzing droplets and their surfaces are destructive, non-interface-specific, not conducted under ambient conditions, require sample substrates, conducted ex situ, or a combination thereof. For these reasons, a technique for surface-selective in situ analyses under any condition is necessary. This feature article presents recent developments in second-order nonlinear optical scattering techniques for the in situ interfacial analysis of aerosol droplets in the air. First, we describe the abundant utilization of such droplets across industries and how their unique surface properties lead to their ubiquitous usage. Then, we describe the fundamental properties of droplets and their surfaces followed by common methods for their study. We next describe the fundamental principles of sum-frequency generation (SFG) spectroscopy, the Langmuir adsorption model, and how they are used together to describe adsorption processes at planar liquid and droplet surfaces. We also discuss the history of developments of second-order scattering from droplets suspended in dispersive media and introduce second-harmonic scattering (SHS) and sum-frequency scattering (SFS) spectroscopies. We then go on to outline the developments of SHS, electronic sum-frequency scattering (ESFS), and vibrational sum-frequency scattering (VSFS) from droplets in the air and discuss the fundamental insights about droplet surfaces that the techniques have provided. Finally, we describe some of the areas of nonlinear scattering from airborne droplets which need improvement as well as potential future directions and utilizations of SHS, ESFS, and VSFS throughout environmental systems, interfacial chemistry, and fundamental physics. The goal of this feature article is to spread knowledge about droplets and their unique surface properties as well as introduce second-order nonlinear scattering to a broad audience who may be unaware of recent progress and advancements in their applicability.

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Section: Second-order Nonlinear Optical Scattering From Droplets In Airmentioning

confidence: 99%

In Situ Probing of the Surface Properties of Droplets in the Air

et al. 2023

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“…SFG scattering (SFS) experiments have been successfully performed on suspensions and emulsions of water droplets in oil, , and thereby opened the door to studying small particles directly. The group of Yi Rao has worked on extending SFG scattering to free floating aqueous aerosol particles. − While there has been some discussion about the experimental limitations involved in measuring SFS spectra of free floating aerosol, , such experiments would promise an insight not only into the role of the particle size and geometry but may also allow to extend studies to include much more realistic systems and introducing reagents into the gasphase. In a similar vein, it would be very interesting to study, for example, suspensions of mineral particles in a liquid, since it has been shown repeatedly that decreasing the particle size of solid materials can lead to quite surprising effects.…”

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confidence: 99%

The Role of Sum-Frequency Generation Spectroscopy in Understanding On-Surface Reactions and Dynamics in Atmospheric Model-Systems

Saak,

Backus

2024

J. Phys. Chem. Lett.

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Surfaces, both water/air and solid/water, play an important role in mediating a multitude of processes central to atmospheric chemistry, particularly in the aerosol phase. However, the study of both static and dynamic properties of surfaces is highly challenging from an experimental standpoint, leading to a lack of molecular level information about the processes that take place at these systems and how they differ from bulk. One of the few techniques that has been able to capture ultrafast surface phenomena is time-resolved sum-frequency generation (SFG) spectroscopy. Since it is both surface-specific and chemically sensitive, the extension of this spectroscopic technique to the time domain makes it possible to study dynamic processes on the femtosecond time scale. In this Perspective, we will explore recent advances made in the field both in terms of studying energy dissipation as well as chemical reactions and the role the surface geometry plays in these processes.

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The Structure of Carbon Dioxide at the Air‐Water Interface and its Chemical Implications

Martins‐Costa,

Ruiz‐López

2024

Chemistry A European J

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The efficient reduction of CO2 into valuable products is a challenging task in an international context marked by the climate change crisis and the need to move away from fossil fuels. Recently, the use of water microdroplets has emerged as an interesting reaction media where many redox processes which do not occur in conventional solutions take place spontaneously. Indeed, several experimental studies in microdroplets have already been devoted to study the reduction of CO2 with promising results. The increased reactivity in microdroplets is thought to be linked to unique electrostatic solvation effects at the air‐water interface. In the present work, we report a theoretical investigation on this issue for CO2 using first‐principles molecular dynamics simulations. We show that CO2 is stabilized at the interface, where it can accumulate, and that compared to bulk water solution, its electron capture ability is larger. Our results suggests that reduction of CO2 might be easier in interface‐rich systems such as water microdroplets, which is in line with early experimental data and indicate directions for future laboratory studies. The effect of other relevant factors which could play a role in CO2 reduction potential is discussed.

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Partitioning of Formic and Acetic Acids to the Gas/Aerosol Interface

Cited by 4 publications

References 55 publications

In Situ Probing of the Surface Properties of Droplets in the Air

In Situ Probing of the Surface Properties of Droplets in the Air

The Role of Sum-Frequency Generation Spectroscopy in Understanding On-Surface Reactions and Dynamics in Atmospheric Model-Systems

The Structure of Carbon Dioxide at the Air‐Water Interface and its Chemical Implications

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