气候变化领域集成服务门户(CCPortal): Modeling approaches for atmospheric ion-dipole collisions: all-atom trajectory simulations and central field methods

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DOI	10.5194/acp-22-11155-2022
	Modeling approaches for atmospheric ion-dipole collisions: all-atom trajectory simulations and central field methods
	Neefjes, Ivo; Halonen, Roope; Vehkamaki, Hanna; Reischl, Bernhard
发表日期	2022
ISSN	1680-7316
EISSN	1680-7324
起始页码	11155
结束页码	11172
卷号	22 期号:17 页码:18
英文摘要	Ion-dipole collisions can facilitate the formation of atmospheric aerosol particles and play an important role in their detection in chemical ionization mass spectrometers. Conventionally, analytical models, or simple parametrizations, have been used to calculate the rate coefficients of ion-dipole collisions in the gas phase. Such models, however, neglect the atomistic structure and charge distribution of the collision partners. To determine the accuracy and applicability of these approaches under atmospheric conditions, we calculated collision cross sections and rate coefficients from all-atom molecular dynamics collision trajectories, sampling the relevant range of impact parameters and relative velocities, and from a central field model using an effective attractive interaction fitted to the long-range potential of mean force between the collision partners. We considered collisions between various atmospherically relevant molecular ions and dipoles and charged and neutral dipolar clusters. Based on the good agreement between collision cross sections and rate coefficients obtained from molecular dynamics trajectories and a generalized central field model, we conclude that the effective interactions between the collision partners are isotropic to a high degree, and the model is able to capture the relevant physicochemical properties of the systems. In addition, when the potential of mean force is recalculated at the respective temperatures, the central field model exhibits the correct temperature dependence of the collision process. The classical parametrization by Su and Chesnavich (1982), which combines a central field model with simplified trajectory simulations, is able to predict the collision rate coefficients and their temperature dependence quite well for molecular systems, but the agreement worsens for systems containing clusters. Based on our results, we propose the combination of potential of mean force calculation and a central field model as a viable and elegant alternative to the brute force sampling of individual collision trajectories over a large range of impact parameters and relative velocities.
学科领域	Environmental Sciences; Meteorology & Atmospheric Sciences
语种	英语
WOS研究方向	Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences
WOS记录号	WOS:000848775200001
来源期刊	ATMOSPHERIC CHEMISTRY AND PHYSICS
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/273574
作者单位	University of Helsinki; Tianjin University; Tianjin University
推荐引用方式 GB/T 7714	Neefjes, Ivo,Halonen, Roope,Vehkamaki, Hanna,et al. Modeling approaches for atmospheric ion-dipole collisions: all-atom trajectory simulations and central field methods[J],2022,22(17):18.
APA	Neefjes, Ivo,Halonen, Roope,Vehkamaki, Hanna,&Reischl, Bernhard.(2022).Modeling approaches for atmospheric ion-dipole collisions: all-atom trajectory simulations and central field methods.ATMOSPHERIC CHEMISTRY AND PHYSICS,22(17),18.
MLA	Neefjes, Ivo,et al."Modeling approaches for atmospheric ion-dipole collisions: all-atom trajectory simulations and central field methods".ATMOSPHERIC CHEMISTRY AND PHYSICS 22.17(2022):18.