Nucleation-mode particle pool and large increases in N cn and N ccn observed over the northwestern Pacific Ocean in the spring of 2014

Determination of the updated concentrations of atmospheric particles (N-cn) and the concentrations of cloud condensation nuclei (N-ccn) over the northwestern Pacific Ocean (NWPO) are important to accurately evaluate the influence of aerosol outflow from the Asian continent on the climate by considering the rapid changes in emissions of air pollutants therein. However, field observations in the last two decades are scarce. We conducted a cruise campaign over the NWPO to simultaneously measure N-cn, N-ccn and the size distribution of aerosol particles from day of year (DOY) 81 to DOY 108 of 2014. The mean values of N-ccn at supersaturation (SS) of levels 0.2% and 0.4% were 0.68 +/- 0.38 +/- 103 and 1.1 +/- 0.67 +/- 103 cm(3), respectively, with an average of 2.8 +/- 1.0 +/- 103 cm(3) for N-cn during the cruise over the NWPO. All are approximately 1 order of magnitude larger than spring observations made during the preceding two decades in the remote marine atmosphere. The larger values, against the marine natural background reported in the literature, imply an overwhelming contribution from continental inputs. The calculated activity ratios (ARs) of the cloud condensation nuclei (CCN) were 0.30 +/- 0.11 and 0.46 +/- 0.19 at SS levels of 0.2% and 0.4 %, respectively, which are almost the same as those of upwind semi-urban sites. High N-ccn and CCN activities were observed from DOY 98 to DOY 102, when the oceanic zone received even stronger continental input. Excluding biomass burning (BB) and dust aerosols, good correlation between N-ccn at 0.4% SS and the number concentrations of >60 nm particles (N>60 nm) was obtained during the entire cruise period, with a slope of 0.98 and (RD)-D-2 0.94, and the corresponding effective hygroscopicity parameter (+/-) was estimated to be 0.40. A bimodal size distribution pattern of the particle number concentration was generally observed during the entire campaign when the N>90 nm varied largely. However, the N<30 nm, accounting for approximately one-third of the total number concentration, varied narrowly, and two NPF events associated with vertical transport were observed. This implies that a pool of nucleation-mode atmospheric particles is aloft. BB and dust events were observed over the NWPO, but their aerosol contributions to N-cn and N-ccn were minor (i. e., 10% or less) on a monthly timescale.