WITHDRAWN: Comprehensive assessment of atmospheric interactions between Criegee intermediate and simplest Imine (CH2NH) in gas and aqueous phase environments

The simplest Criegee intermediate (CH₂OO), produced through the ozonolysis (O₃) of ethylene in the Earth's troposphere, plays a crucial role as a precursor in new particle formation (NPF) and secondary organic aerosols (SOA). Recent experimental and theoretical findings suggest that Criegee intermediate (CI) with organic acid, carbonyl, and amines is important for organic aerosol formation. However, the reaction of CI with imine, especially CH₂NH, has not been reported so far. Therefore, we investigated the CH₂OO + CH₂NH system, which is also an isoelectronic reaction system of CH₂OO + CH₂O and CH₂OO +CH₂CH₂. The mechanism for CH₂OO + CH₂NH and CH₂OO + CH₂NH (+H₂O) were conducted using ab initio/MD. Our results indicate that the rate constants for CH₂OO + CH₂NH reaction fall within the range of its isoelectronic reaction systems. The product branching ratio analysis indicates that cy-H₂C(OO)NCH₂ (IMn) and NHCHOH are the primary products in the gas phase reaction of CH₂OO + CH₂NH, irrespective of temperature. Notably, the involvement of water in the reaction facilitates the formation of significant pressure-dependent products, such as HMF_n and IM_n. Born-Oppenheimer Molecular Dynamics (BOMD) simulations provide strong evidence for IMn formation in both the gas phase and the air-water interface, with a faster reaction rate at the interface. Furthermore, BOMD simulations of CH₂OO and CH₂NH interactions on water droplet surfaces highlight the generation of water-mediated loop-structured products, including N-hydroxyethanimine (H₂C=N-CH₂-OOH) and HMHP (OH-CH₂-OOH). This study highlights the potential significance of Criegee-Imine interactions in driving secondary aerosol formation, particularly in areas with elevated nitrogen-based emissions. The findings of this study may offer valuable insights into the CI-imine chemical processes in these regions.