Nucleation Rate of N2 and O2 in Cryogenic H2 and He

JO Song and JD Berry and E Goudeli, JOURNAL OF PHYSICAL CHEMISTRY B, 127, 9976-9984 (2023).

DOI: 10.1021/acs.jpcb.3c03364

The homogeneous nucleation of N-2 and O-2 in cryogenic H-2 and He is investigated by using classical molecular dynamics (MD) simulations. The nucleation kinetics of N-2 and O-2 clusters, including nucleation rate, critical cluster size, and cluster energy, are elucidated in H-2 and He carrier gas at thermalization temperatures of 30-80 K and initial gas densities of 5.65 x 10(24)-2 x 10(27) m(-3). The energy released from the clusters during nucleation increases the system temperature by 77-138%, consistent with N-2 nucleation experiments in supersonic nozzles and the mean-field kinetic nucleation theory. The nucleation rate derived by MD, J(sim), spans across 2.14 x 10(29)-5.25 x 10(36) m(-3) s(-1) for both N-2 and O-2 under all conditions. The MD-obtained homogeneous nucleation rate is in agreement with predictions from the self-consistent classical nucleation theory (CNT) at low temperature (<70 K) but is 3-7 orders of magnitude faster than the CNT when temperature exceeds 70 K, consistent with the literature. Increasing temperature and decreasing concentration of the nucleating vapors leads to larger critical cluster sizes. The CNT underpredicts the critical cluster size at cryogenic temperatures below 60 K by 200-700%. The present MD methodology can be used for the direct determination of the nucleation rate and critical cluster size of N-2 and O-2 under cryogenic conditions, circumventing the assumptions inherent in CNT.

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