Predicting Absorption and Diffusion of Plasma-Generated O( 3 P), O( 1 D), and Other RONS in Aqueous Environments Using Molecular Simulations

We study the interactions of plasma-generated Reactive Oxygen and Nitrogen Species (RONS) with water due to their importance for applications in health and agriculture. Atomic oxygen, a key RONS, is produced by plasma in both its triplet ground state, O(3P), and its singlet excited state, O(1D). Experimental studies indicate that when plasma interacts with water, atomic oxygen can remain sufficiently stable to enter the aqueous phase. Recent measurements show that ground-state oxygen atoms can persist for tens of microseconds and penetrate hundreds of micrometres into the aqueous phase. However, quantitative data on the solubility and diffusion of atomic oxygen remain scarce. This is likely due to limitations in experimental diagnostics and the challenges that the complex electronic structure of atomic oxygen presents to modeling approaches. To overcome these challenges, we developed state-specific force fields to model the interactions of O(3P) and O(1D) with water to account for quantum-state-dependent interactions. Using these force fields, we provide the first estimates of temperature- and quantum-state-dependent self-diffusion and Henry coefficients of atomic oxygen in aqueous environments. Building upon these results, we propose a general framework to estimate the solubility and diffusion of other plasma-generated charge-neutral RONS in water by representing each species as a charge-neutral Lennard-Jones particle. The influence of particle size, solute-solvent interaction strength, and temperature on the transport and thermodynamic properties of RONS was systematically investigated. This approach enables the estimation of the Henry coefficients and the diffusion coefficients of RONS in water based on particle size, solute-solvent interactions, and temperature. These estimates provide key parameters for device-level plasma-liquid simulations and offer molecular-scale insight for interpreting experimental findings.