Revisiting spontaneous Raman scattering for direct oxygen atom quantification

In this Letter, the counterintuitive and largely unknown Raman activity of oxygen atoms is evaluated for its capacity to determine absolute densities in gases with significant O-density. The study involves ${\rm CO}_2$ microwave plasma to generate a self-calibrating mixture and establish accurate cross sections for the $^3{\!P_2}{\leftrightarrow ^3}{\!P_1}$ and $^3{\!P_2}{\leftrightarrow ^3}{\!P_0}$ transitions. The approach requires conservation of stoichiometry, confirmed within experimental uncertainty by a 1D fluid model. The measurements yield ${\sigma _{J = 2 \to 1}} = 5.27 \pm _{{\rm sys}:0.53}^{{\rm rand}:0.17} \times {10^{- 31}}\;{{\rm cm}^2}/{\rm sr}$ and ${\sigma _{J = 2 \to 0}} = 2.11 \pm _{{\rm sys}:0.21}^{{\rm rand}:0.06} \times {10^{- 31}}\;{{\rm cm}^2}/{\rm sr}$, and the detection limit is estimated to be $1 \times {10^{15}}\;{{\rm cm}^{- 3}}$ for systems without other scattering species.