Amplified Secondary Organic Aerosol Formation Induced by Anthropogenic–Biogenic Interactions in Forests Around Megacities

Abstract

The amplification effect of anthropogenic-biogenic interactions on secondary organic aerosol (SOA) formation remains debated, particularly regarding the impact of anthropogenic emissions on biogenic SOA (BSOA) formation in forests near megacities. This study concurrently measured typical biogenic and anthropogenic SOA tracers during day and night at the summit (1,690 m a.s.l.) and foot (200 m a.s.l.) of the Nanling mountains, a large subtropical forest adjacent to the Pearl River Delta (PRD) in southern China. Results revealed unexpectedly high concentrations of BSOA tracers (149.9 ± 70.5 ng m⁻³ at the summit and 109.7 ± 51.2 ng m⁻³ at the foot), surpassing those at most other background sites worldwide. Daytime BSOA tracer levels at the foot were consistent with nighttime levels, whereas the summit showed significantly higher concentrations at night. Nighttime correlations between O₃ and BSOA tracers at the summit suggest that high O₃ levels stimulate BSOA formation. Conversely, a negative correlation between O₃ and isoprene derived SOA (SOA_I) tracers at the foot indicates that other oxidants may also influence SOA_I formation. BSOA tracer concentrations rose significantly with the arrival of anthropogenic pollutants (e.g., SO₂ and NO₂), indicating that anthropogenic pollution amplifies BSOA formation by enhancing aerosol acidity (pH < 3). This amplification effect could be mitigated by the reduction of aerosol acidity due to increased NH₃ and relative humidity (RH). Our findings provide valuable insights into the interactions between anthropogenic and biogenic emissions on SOA formation and vertical distribution in forests surrounding megacities.