Impact of a hydrophobic ion on the early stage of atmospheric aerosol formation

Feketeová, Linda; Bertier, Paul; Salbaing, Thibaud; Azuma, T.; Calvo, F.; Farizon, B.; Farizon, M.; Märk, T.D.

doi:10.1073/pnas.1911136116

Cited by 10 publications

(7 citation statements)

References 58 publications

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“…[1][2][3][4][5][6] Atmospheric new particle formation (NPF) through gas-to-particle conversion constitutes over half of the global aerosol budget. [1][2][3][4][5][6][7][8][9][10][11][12] It is widely accepted that gaseous sulfuric acid (SA) formed from SO2 oxidation plays a key role in atmospheric NPF, 3,5,6,[13][14][15][16][17][18][19][20][21][22] and a broad variety of atmospheric compounds such as ammonia, amines, and organic acids efficiently enhance SA-driven NPF by stabilizing the newly formed molecular clusters. 3,13,14,20,[23][24][25][26][27][28] However, significant gaps remain between the observed particle formation rates in the field and laboratories and the rates predicted by simulations.…”

Section: Introductionmentioning

confidence: 99%

“…Aerosols have significant effects on the global climate, visibility, and human health. − Atmospheric new particle formation (NPF) through gas-to-particle conversion constitutes over half of the global aerosol budget. − It is widely accepted that gaseous sulfuric acid (SA) formed from SO 2 oxidation plays a key role in atmospheric NPF, ,,,− and a broad variety of atmospheric compounds such as ammonia, amines, and organic acids efficiently enhance SA-driven NPF by stabilizing the newly formed molecular clusters. ,,,,− However, significant gaps remain between the observed particle formation rates in the field and laboratories and the rates predicted by simulations. ,,,− Therefore, there is a need to consider the involvement of other gaseous precursors in NPF to reduce the gaps between experiments and simulations.…”

Section: Introductionmentioning

confidence: 99%

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Structural Effects of Amines in Enhancing Methanesulfonic Acid-Driven New Particle Formation

Shen

Elm

Xie

et al. 2020

Environ. Sci. Technol.

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Atmospheric amines can enhance methanesulfonic acid (MSA)-driven new particle formation (NPF), but the mechanism is fundamentally different compared to the extensively studied sulfuric acid (SA)-driven process. Generally, the enhancing potentials of amines in SA-driven NPF follow the basicity, while this is not the case for MSA-driven NPF, where structural effects dominate making MSA-driven NPF more prominent for methylamine (MA) compared to dimethylamine (DMA). Therefore, probing structural factors determining the enhancing potentials of amines on MSAdriven NPF is key to fully understanding the contribution of MSA on NPF. Here, we performed a comparative study on DMA and MA enhancing MSA-driven NPF by examining cluster formation using computational methods. The results indicate that DMA-MSA clusters are more stable than the corresponding MA-MSA clusters for cluster size up to (DMA)2(MSA)2, indicating that the basicity of amines dominates the initial cluster formation. The methyl groups of DMA were found to present significant steric hindrance beyond the (DMA)2(MSA)2 cluster and this adds to the lower hydrogen bonding capacity of DMA making the cluster growth less favorable compared to MA.This study implies that several amines could synergistically enhance MSA-driven NPF by maximizing the advantage of different amines in different amine-MSA cluster growth stages.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Structural Effects of Amines in Enhancing Methanesulfonic Acid-Driven New Particle Formation

Shen

Elm

Xie

et al. 2020

Environ. Sci. Technol.

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“…Figure 5 shows the time correlation function ⟨ K ( t ) K (0)⟩/⟨ K 2 (0)⟩ averaged from 1000 independent trajectories and compares the results obtained for differently sized pyridinium–water cluster ions, together with earlier results obtained for the protonated water tetramer cluster ion. 29 Typical average relaxation times for the neat water clusters are on the order of some picoseconds, and times for the pyridinium–water clusters are found to lie at least one order of magnitude higher. Moreover, it is interesting to see that for these pyridinium–water cluster ions studied, the relaxation is faster for clusters containing more water molecules.…”

Section: Resultsmentioning

confidence: 96%

“…Additional molecular dynamics simulations were performed to characterize the redistribution kinetics, by evaluating the time variations K ( t ) of the kinetic energy in the ionic impurity after its excitation at time t = 0. Figure shows the time correlation function ⟨ K ( t ) K (0)⟩/⟨ K 2 (0)⟩ averaged from 1000 independent trajectories and compares the results obtained for differently sized pyridinium–water cluster ions, together with earlier results obtained for the protonated water tetramer cluster ion . Typical average relaxation times for the neat water clusters are on the order of some picoseconds, and times for the pyridinium–water clusters are found to lie at least one order of magnitude higher.…”

Section: Resultsmentioning

confidence: 96%

Energy Dispersion in Pyridinium–Water Nanodroplets upon Irradiation

et al. 2022

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Postirradiation dissociation of molecular clusters has been mainly studied assuming energy redistribution in the entire cluster prior to the dissociation. Here, the evaporation of water molecules from out-of-equilibrium pyridinium–water cluster ions was investigated using the recently developed correlated ion and neutral time-of-flight (COINTOF) mass spectrometry technique in combination with a velocity-map imaging (VMI) device. This special setup enables the measurement of velocity distributions of the evaporated molecules upon high-velocity collisions with an argon atom. The distributions measured for pyridinium–water cluster ions are found to have two distinct components. Besides a low-velocity contribution, which corresponds to the statistical evaporation of water molecules after nearly complete redistribution of the excitation energy within the clusters, a high-velocity contribution is also found in which the molecules are evaporated before the energy redistribution is complete. These two different evaporation modes were previously observed and described for protonated water cluster ions. However, unlike in the case of pure water clusters, the low-velocity part of the distributions for pyridinium-doped water clusters is itself composed of two distinct Maxwell–Boltzmann distributions, indicating that evaporated molecules originate in this case from out-of-equilibrium processes. Statistical molecular dynamics simulations were performed to (i) understand the effects caused in the ensuing evaporation process by the various excitation modes at different initial cluster constituents and to (ii) simulate the distributions resulting from sequential evaporations. The presence of a hydrophobic impurity in water clusters is shown to impact water molecule evaporation due to the energy storage in the internal degrees of freedom of the impurity.

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“…Neutral molecular clusters are produced by adiabatic expansion of a molecular vapor of either glycine and water or a dry (anhydrous) vapor of glycine 23 (see the Experimental Section in the Supporting Information). The ions formed by electron impact ionization of the neutral cluster beam are analyzed by mass spectrometry.…”

Section: ■ Methodsmentioning

confidence: 99%

Glycine Peptide Chain Formation in the Gas Phase via Unimolecular Reactions

et al. 2023

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Peptide chain formation from amino acids such as glycine is a key step in the emergence of life. Unlike their synthesis by living systems, how peptide chains grow under abiotic conditions is an open question given the variety of organic compounds discovered in various astrophysical environments, comets and meteorites. We propose a new abiotic route in the presence of protonated molecular dimers of glycine in a cold gaseous atmosphere without further need for a solid catalytic substrate. The results provide evidence for the preferential formation of mixed protonated dimers of glycine consisting of a dipeptide and a glycine molecule instead of pure protonated glycine dimers. Additional measurements mimicking a cosmic-ray impact in terms of internal excitation show that a single gas-phase collision induces polymerization via dehydration in both the mixed and pure dimer ions. Peptide chain growth is thus demonstrated to occur via a unimolecular gas-phase reaction in an excited cluster ion.

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Impact of a hydrophobic ion on the early stage of atmospheric aerosol formation

Cited by 10 publications

References 58 publications

Structural Effects of Amines in Enhancing Methanesulfonic Acid-Driven New Particle Formation

Structural Effects of Amines in Enhancing Methanesulfonic Acid-Driven New Particle Formation

Energy Dispersion in Pyridinium–Water Nanodroplets upon Irradiation

Glycine Peptide Chain Formation in the Gas Phase via Unimolecular Reactions

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