Abstract

Ultrafine particles (UFPs) are ubiquitously distributed throughout the global atmosphere. Their dimensions, often less than 100 nm, vary significantly from the surface. New particle formation (NPF) is a key process occurring in the planetary boundary layer (PBL). Newly formed particles are an important source of aerosols and cloud condensation nuclei (CCN) that influence clouds and climate, while the distribution of these new particles at different altitudes has rarely been studied. In-situ measurements of ultrafine particles (UFP) and New particle formation (NPF) observed at the ground and at the top of the Canton Tower (454 m) and Shenzhen tower located in southern China,both were analyzed using the measurements of multiple meteorological and physicochemical quantities, as both observed during a field campaign and simulated with the WRF-chem model. We found that turbulence and NPF characters vary considerably with heights, with UFP concentration diminishing by half from the surface to the tower top. This indicates the UFP transports upward from the ground in the lower boundary layer. A consistent relationship is established between the occurrences of NPF and the evolution of turbulence. The correlation between the exchange ratio at the tower top has correlated well with nucleation growth, suggesting that turbulence can play an important role in the episodes of NPF growth, whose growth rate is closely related to the turbulence exchange ratio, effectively dictating the ultrafine particle concentration before and during the lockdown period. A new mechanism is thus hypothesized: NPF happens eailer near the surface and grows faster at the upper PBL, attributed to condensable vapors being transported by turbulent vertical mixing in the boundary layer. Model simulations using the WRF-Chem model reveal that the exchange ratio changed the NPF parameters, supporting the proposed mechanism that the evolution of the PBL variation has a significant impact on NPF, which should not be omitted in the NPF research, since this physical factor could be a dominant one in the NPF mechanism.

Full Text
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