Modeling the formation and growth of atmospheric molecular clusters: A review

Elm, Jonas; Kubečka, Jakub; Besel, Vitus; Jääskeläinen, Matias J.; Halonen, Roope; Kurtén, Theo; Vehkamäki, Hanna

doi:10.1016/j.jaerosci.2020.105621

Cited by 128 publications

(179 citation statements)

References 306 publications

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“…The heating of the clusters with respect to the bath temperature, DT n = T n À T, is more pronounced for the densest simulated systems due to more frequent growth events. The efficiency of thermalisation is similar in simulations at different densities and same temperature, when the ratio of CO 2 to carrier gas remains roughly constant, as seen in eqn (17). Fig.…”

Section: Cluster Analysissupporting

confidence: 64%

“…In this work, the nucleation rates calculated using eqn ( 7)-( 13), ( 16), (17), and (19) are denoted by J CNT .…”

Section: Theoretical Framework Of Nucleationmentioning

confidence: 99%

“…For very small clusters, minimum energy structures at 0 K can be calculated using quantum chemical methods, and free energies can be obtained using principles of statistical mechanics. 17 For larger clusters, atomistic interactions can be described using classical force fields, and free energies can be obtained from Monte Carlo methods. 16,18 These free energetics can then be combined with the standard kinetic scheme of nucleation to calculate actual nucleation rates.…”

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Homogeneous nucleation of carbon dioxide in supersonic nozzles II: molecular dynamics simulations and properties of nucleating clusters

Halonen

Tikkanen

Reischl

et al. 2021

Phys. Chem. Chem. Phys.

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Section: Cluster Analysissupporting

confidence: 64%

“…In this work, the nucleation rates calculated using eqn ( 7)-( 13), ( 16), (17), and (19) are denoted by J CNT .…”

Section: Theoretical Framework Of Nucleationmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Homogeneous nucleation of carbon dioxide in supersonic nozzles II: molecular dynamics simulations and properties of nucleating clusters

Halonen

Tikkanen

Reischl

et al. 2021

Phys. Chem. Chem. Phys.

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“…The development of GO as implemented in ABCluster, has eliminated this obstacle to a large extent, making a series of productive NPF studies possible [32, 96, 167, 172–197] and revealing valuable insights into atmospheric chemistry (see Figure 7 for some examples). ABCluster has been regarded as a standard tool in this field [198–200]. In a work by Zhang, Francisco, and Zeng [176], the GMs of (H 2 NSO 3 H) x (H 2 SO 4 ) y ((CH 3 ) 2 NH) z (0 ≤ x + y ≤ 3, 0 ≤ z ≤ 2) were searched with ABCluster and were subsequently used in quantum chemical and ACDC simulations.…”

Section: Applicationsmentioning

confidence: 99%

Global optimization of chemical cluster structures: Methods, applications, and challenges

Zhang

Glezakou

2020

Int J of Quantum Chemistry

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Chemical clusters are relevant to many applications in catalysis, separations, materials, and energy sciences. Experimentally, the structure of clusters is difficult to determine, but it is very important in understanding their chemistry and properties. Computational methods can be used to examine cluster structure, however finding the most stable structure is not simple, particularly as the cluster size increases. Global optimization techniques have long been used to tackle the problem of the most stable structure, but such approaches would have to look for a global minimum, while sampling local minima over the whole potential energy surface as well. In this review, the state‐of‐the‐art theory of global optimization theory is summarized. First, the definition, significance, relation to experiments, and a brief history of global optimization is presented. We then discuss, in more detail, three versatile global optimization methods: the basin hopping, the artificial bee colony algorithm, and the genetic algorithm. We close with some representative application examples of global optimization of clusters since 2016 and the challenges, open questions and opportunities in this field.

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“…One approach is to compute the cluster formation free energy using quantum chemistry (QC) and then calculate the evaporation rate using detailed balance (together with the collision rate). 21 Unfortunately, the evaporation rates obtained with this approach depend exponentially on the free energies, and even small uncertainties in the latter can cause errors of several orders of magnitude in the former. Advances in computational power and recent improvements in computational chemistry have, however, helped overcome these obstacles.…”

mentioning

confidence: 99%

New Particle Formation from the Vapor Phase: From Barrier-Controlled Nucleation to the Collisional Limit

Dingilian

Lippe

Kubečka

et al. 2021

J. Phys. Chem. Lett.

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Studies of vapor phase nucleation have largely been restricted to one of two limiting cases—nucleation controlled by a substantial free energy barrier or the collisional limit where the barrier is negligible. For weakly bound systems, exploring the transition between these regimes has been an experimental challenge, and how nucleation evolves in this transition remains an open question. We overcome these limitations by combining complementary Laval expansion experiments, providing new particle formation data for carbon dioxide over a uniquely broad range of conditions. Our experimental data together with a kinetic model using rate constants from high-level quantum chemical calculations provide a comprehensive picture of new particle formation as nucleation transitions from a barrier-dominated process to the collisional limit.

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Modeling the formation and growth of atmospheric molecular clusters: A review

Cited by 128 publications

References 306 publications

Homogeneous nucleation of carbon dioxide in supersonic nozzles II: molecular dynamics simulations and properties of nucleating clusters

Homogeneous nucleation of carbon dioxide in supersonic nozzles II: molecular dynamics simulations and properties of nucleating clusters

Global optimization of chemical cluster structures: Methods, applications, and challenges

New Particle Formation from the Vapor Phase: From Barrier-Controlled Nucleation to the Collisional Limit

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