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© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 30 Jul 2018

Research article | 30 Jul 2018

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This discussion paper is a preprint. A revision of the manuscript is under review for the journal Atmospheric Chemistry and Physics (ACP).

New particle formation in marine atmosphere during seven cruise campaigns

Yujiao Zhu1, Kai Li2, Yanjie Shen1, Yang Gao1, Xiaohuan Liu1, Yang Yu1, Huiwang Gao1, and Xiaohong Yao1 Yujiao Zhu et al.
  • 1Key Lab of Marine Environmental Science and Ecology, Ministry of Education, Ocean University of China, Qingdao 266100, China
  • 2National Marine Environmental Forecasting Center, Beijing, 100081, China

Abstract. To study the particle number concentration, size distribution and new particle formation (NPF) events in marine atmosphere, we made measurements during six cruise campaigns over the marginal seas of China in 2011–2016 and one campaign from the marginal seas to the Northwest Pacific Ocean (NWPO) in 2014. We observed relatively frequent NPF events in the atmosphere over the marginal seas of China, i.e., 23 out of 126 observational days with the highest occurrence frequency in fall, followed by spring and summer. 22 out of 23 NPF events were analyzed to be associated with the long-range transport of continental pollutants based on 24-hr air mass back trajectories and the preexisting particle number concentrations largely exceeding the clean marine background, leaving one much weaker NPF event to be likely induced by oceanic precursors alone and supported by multiple independent evidences. Although the long-range transport signal of continental pollutants can be clearly observed in the remote marine atmosphere over the NWPO, NPF events were observed only in 2 days out of 36 days. The nucleation mode particles (<30nm), however, accounted for as high as 40%±13% of the total particle number concentration during the NWPO cruise campaign, implying that there were many undetected NPF events in the sea-level atmosphere or above.

To better characterize NPF events, we introduced a term, i.e., the net maximum increase in nucleation mode particles number concentration (NMINP) and correlated it with formation rate of new particles (FR). We found a moderately good linear correlation between NMINP and FR at FR ≤8cm−3s−1, but there was no correlation at FR >8cm−3s−1. The possible mechanisms were argued in terms of roles of different vapor precursors. We also found a ceiling existing for the growth of new particles from 10nm to larger size in most of NPF events. We thereby introduce a term, i.e., the maximum geometric median diameter of new particles (Dpgmax) and correlate it with the growth rate of new particles (GR). A moderately good linear correlation was also obtained between Dpgmax and GR, and only GR larger than 7.9nmh−1 can lead to new particles growing with Dpgmax beyond 50nm. Combining simultaneous measurements of the particle number size distributions and cloud condensation nuclei (CCN) at different super saturations (SS), we indeed observed a clear increase in CCN when the Dpg of new particles exceeded 50nm at SS=0.4%. However, it was not the case for SS=0.2%. Consistent with previous studies in continental atmosphere, our results implied that 50nm can be used as the threshold for new particles to be activated as CCN in the marine atmosphere. Moreover, the κ decreased from 0.4 to 0.1 during the growth period of new particles, implying that organics likely overwhelmed the growth of new particle to CCN size. The chemical analysis of nano-MOUDI samples revealed TMA and oxalic acid may play the important role in the growth of new particles.

Yujiao Zhu et al.
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Status: final response (author comments only)
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Yujiao Zhu et al.
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Short summary
In this paper, we investigate new particle formation (NPF) events during seven cruises including the marginal seas of China and the Northwest Pacific Ocean. NPF events were observed in 25 days and were most likely associated with the long-range transport of anthropogenic air pollutants, while the weakest one may be derived by ocean precursors. The probability of the grown new particles to activate as CCN was low. This study improves the understanding of NPF events in the marine atmosphere.
In this paper, we investigate new particle formation (NPF) events during seven cruises including...