Kinetics and nucleation dynamics in ion-seeded atomic clusters

Rožman, Marko; Bredice, Mitchell; Smucker, Jonathan; Sadeghpour, H. R.; Vrînceanu, D.; Côté, Robin; Kharchenko, V.

doi:10.1103/physreva.105.022807

Cited by 2 publications

(11 citation statements)

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“…We ran 500 simulations with unique initial conditions for each temperature, with a total simulation time of 2.5 ns. In our previous work, we found that small clusters grew relatively quickly, in ∼2-5ns, at a temperature of 90K [52]. The rate of nucleation of nano-clusters was significantly increased at lower temperatures, such as 40K.…”

Section: Simulation Detailsmentioning

confidence: 89%

“…First, we notice the remarkable stability of the Ar 4 H + cluster, which has the first closed shell. This cluster generally does not demonstrate n → n − 1 transitions, as it is extremely stable with deep binding energies of the cluster Ar atoms [52]. Moreover, the Ar 4 H + cluster exists in the broad time-domain that overlaps significantly with timeregions that belong to other clusters.…”

Section: Formation Of Nascent Arnh + Clustersmentioning

confidence: 98%

“…To analyze the cluster parameters, we used the DBSCAN algorithm implemented in the Clustering.jl package of the Julia programming language. A more detailed discussion of the cluster definition and DBSCAN parameters can be found in [52]. However, for each cluster its total energy is calculated to ensure it is negative to indicate a true bound cluster.…”

Section: Simulation Detailsmentioning

confidence: 99%

“…To simulate the growth of independent clusters, only one H + ion is present in the simulation box, allowing for the formation and tracking of a single Ar n(t) H + cluster in the simulation time from each MD trajectory. This allows one to investigate the evolution of a single independent cluster and to avoid the additional complications arising due to simultaneous nucleation of many clusters around individual protons, where competition between the growth of different clusters leads to the coalescence regime [13,52].…”

Section: Formation Of Nascent Arnh + Clustersmentioning

confidence: 99%

“…Second, the growth of small clusters through the collision reaction Ar n−1 H + + Ar → Ar n H + , leads to a sharp increase in the cluster's internal energy. The average value of the release of internal kinetic energy approximately corresponds to the absolute value of the chemical potential of Ar atoms in the Ar n H + cluster [52]. For smallsized clusters, which can be considered as molecular ions Ar n H + , the n → n + 1 growth leads to multiple excitations of vibrational and rotational modes.…”

Section: Formation Of Nascent Arnh + Clustersmentioning

confidence: 99%

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Inner Energy Relaxation and Growth of Nano-Size Particles

Bredice¹,

Rozman²,

Smucker³

et al. 2023

Preprint

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In this study, molecular dynamics simulations were conducted to investigate the relaxation of the internal energy in nano-sized particles and its impact on the nucleation of atomic clusters. Quantummechanical potentials were utilized to analyze the growth and collision relaxation of the internal energy of ArnH + clusters in a metastable Ar gas. The results revealed that small nano-clusters are formed in highly excited rotational-vibrational states, and the relaxation of internal energy and growth of these nascent clusters are concurrent processes with a strong mutual influence. Under nonequilibrium growth conditions, the relaxation of internal energy can delay the cluster growth process. The rates of cluster growth and internal energy relaxation were found to be influenced by energytransfer collisions between cluster particles and free Ar atoms of the bath gas. Furthermore, the non-equilibrium growth and internal energy relaxation of small nano-clusters were found to depend on the structure of the cluster's atomic shells. An ensemble of molecular dynamics simulations were conducted to investigate the growth, time-evolution of kinetic and total energies of ArnH + clusters with specified n ≤ 11, and the results were explained by collisional relaxation processes described by the Boltzmann equation. Finally, the general relationship between the rates of internal energy relaxation and non-equilibrium growth of nano-particles is discussed.

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Section: Simulation Detailsmentioning

confidence: 89%

Section: Formation Of Nascent Arnh + Clustersmentioning

confidence: 98%

Section: Simulation Detailsmentioning

confidence: 99%

Section: Formation Of Nascent Arnh + Clustersmentioning

confidence: 99%

Section: Formation Of Nascent Arnh + Clustersmentioning

confidence: 99%

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