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Interpretation of NO3–N2O5 observation via steady state in high-aerosol air mass: the impact of equilibrium coefficient in ambient conditions
Steady-state approximation for interpreting NO3 and N2O5 has large uncertainty under complicated ambient conditions and could even produce incorrect results unconsciously. To provide an assessment and solution to the dilemma, we formulate datasets based on in situ observations to reassess the applicability of the method. In most of steady-state cases, we find a prominent discrepancy between Keq (equilibrium coefficient for reversible reactions of NO3 and N2O5) and correspondingly simulated [N2O5]/[NO2]×[NO3], especially under high-aerosol conditions in winter. This gap reveals that the accuracy of Keq has a critical impact on the steady-state analysis in polluted regions. In addition, the accuracy of γ (N2O5) derived by steady-state fit depends closely on the reactivity of NO3 (kNO3) and N2O5(kN2O5). Based on a complete set of simulations, air mass of kNO3 less than 0.01 s−1 with high aerosol and temperature higher than 10 ∘C is suggested to be the best suited for steady-state analysis of NO3–N2O5 chemistry. Instead of confirming the validity of steady state by numerical modeling for every case, this work directly provides appropriate concentration ranges for accurate steady-state approximation, with implications for choosing suited methods to interpret nighttime chemistry in high-aerosol air mass.
Steady-state approximation for interpreting NO3 and N2O5 has large uncertainty under complicated ambient conditions and could even produce incorrect results unconsciously. To provide an assessment and solution to the dilemma, we formulate datasets based on in situ observations to reassess the applicability of the method. In most of steady-state cases, we find a prominent discrepancy between Keq (equilibrium coefficient for reversible reactions of NO3 and N2O5) and correspondingly simulated [N2O5]/[NO2]×[NO3], especially under high-aerosol conditions in winter. This gap reveals that the accuracy of Keq has a critical impact on the steady-state analysis in polluted regions. In addition, the accuracy of γ (N2O5) derived by steady-state fit depends closely on the reactivity of NO3 (kNO3) and N2O5(kN2O5). Based on a complete set of simulations, air mass of kNO3 less than 0.01 s−1 with high aerosol and temperature higher than 10 ∘C is suggested to be the best suited for steady-state analysis of NO3–N2O5 chemistry. Instead of confirming the validity of steady state by numerical modeling for every case, this work directly provides appropriate concentration ranges for accurate steady-state approximation, with implications for choosing suited methods to interpret nighttime chemistry in high-aerosol air mass.