4.6 Article

Limited Formation of CO3+through Strong-Field Ionization and Coulomb Explosion of Formic Acid Clusters

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JOURNAL OF PHYSICAL CHEMISTRY A
卷 126, 期 43, 页码 7954-7961

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AMER CHEMICAL SOC
DOI: 10.1021/acs.jpca.2c06141

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  1. ASU Lightworks

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Femtosecond laser pulses were used to drive multiple ionization in gas-phase formic acid clusters. The results showed that the clusters formed higher charge states and had increased kinetic energy release values compared to individual molecules. The stability of certain clusters was found to be enhanced at lower laser intensities. Molecular dynamics simulation indicated that highly charged atomic ions mostly originated from larger clusters, while the production of CO3+ was more likely from molecules.
Femtosecond laser pulses are utilized to drive multiple ionization in gas-phase formic acid clusters (FA)n. Experimental measurements of the kinetic energy release (KER) of the ions through Coulomb explosion are studied using time-of-flight mass spectrometry and compared to the values recorded from molecules. Upon interacting with 200 fs linearly polarized laser pulses of 400 nm, formic acid clusters facilitate the formation of higher charge states than the formic acid dimer, reaching both C3+ and O3+ and also increasing the KER values to several hundred electronvolts in magnitude for such ions. At a lower laser intensity (3.8 x 1014 W/cm2), we record an enhancement in the signal of the (FA)5(H2O)H+ cluster, which suggests that it has a higher stability, in agreement with previous studies. A molecular dynamics simulation of the Coulomb explosion shows that the highly charged atomic ions arise from larger clusters, whereas the production of CO3+ is more likely to arise from the molecular case. Thus, the relative production of CO3+ is reduced in comparison to the highly charged ions upon clustering and is likely due to the higher ionization levels achieved, which facilitate dissociation.

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