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Eddy correlation air/sea flux measurements of trace gases using atmospheric pressure chemical ionization mass spectrometry.

机译:使用大气压化学电离质谱法对痕量气体进行涡流相关空气/海通量测量。

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Air/sea gas exchange is an important component in the biogeochemical cycles of many trace gases. Eddy correlation is a direct flux measurement technique that has not been widely used for air/sea exchange due to a lack of chemical sensors with sufficient sensitivity and temporal resolution. Atmospheric pressure chemical ionization mass spectrometry (API-CIMS) is a sensitive analytical method which has the potential to measure fluxes by eddy correlation. In this research, field measurements of air/sea flux and concentration gradients of dimethyl sulfide (DMS) and acetone were made using API-CIMS in the equatorial and North Pacific Ocean.; The cruise was from May-July 2004 from Guam to Oregon. The flux of DMS (0.43-6.60 mumol m-2 d-1) was always out of the ocean and was correlated to both the surface seawater DMS concentrations and horizontal wind speed. Surface ocean DMS concentrations were higher in regions with higher chlorophyll content, such as the equatorial upwelling region and across the polar front. The gas exchange coefficient derived from the measurements increased with horizontal wind speed, but the functionality of this dependence is not well constrained. The gas transfer coefficients were mostly in the range between the Wanninkhof (1992) and Liss and Merlivat (1986) parameterizations.; Previous studies suggested that the ocean may be a source of acetone to the atmosphere. In this study, the acetone air/sea concentration gradient also implied that the ocean should be a source to the atmosphere in the equatorial Pacific Ocean. However, the measured acetone fluxes (1.3-16.1 mumol m -2 d-1) were always into the ocean and were correlated with the atmospheric acetone concentration. A global acetone ocean sink of 62 Tg yr-1 was estimated from this data. These results suggest that the ocean is a major sink for atmospheric acetone, about half of the total global budget. The discrepancy between the acetone concentration gradient and the acetone flux suggests near surface gradients, indicating the need to investigate the surface ocean acetone budget.
机译:空气/海洋气体交换是许多微量气体的生物地球化学循环中的重要组成部分。涡流相关是一种直接通量测量技术,由于缺少具有足够灵敏度和时间分辨率的化学传感器,因此尚未广泛用于空气/海洋交换。大气压化学电离质谱法(API-CIMS)是一种灵敏的分析方法,具有通过涡流相关性测量通量的潜力。在这项研究中,使用API​​-CIMS在赤道和北太平洋对空气/海洋通量和二甲基硫醚(DMS)和丙酮的浓度梯度进行了现场测量。这次航行是从2004年5月至7月,从关岛飞往俄勒冈州。 DMS的通量(0.43-6.60 mumol m-2 d-1)总是出海,并且与地表海水DMS浓度和水平风速相关。在叶绿素含量较高的地区,例如赤道上升区和极地前缘,地表海洋DMS浓度较高。从测量得出的气体交换系数随着水平风速的增加而增加,但是这种依赖性的功能并未得到很好的约束。气体传输系数主要在Wanninkhof(1992)和Liss and Merlivat(1986)参数化之间。先前的研究表明,海洋可能是大气中丙酮的来源。在这项研究中,丙酮的空气/海洋浓度梯度也暗示海洋应该是赤道太平洋大气的来源。但是,测得的丙酮通量(1.3-16.1μmolm -2 d-1)总是进入海洋,并与大气中的丙酮浓度相关。根据该数据,全球丙酮海洋汇为62 Tg yr-1。这些结果表明,海洋是大气丙酮的主要汇源,约占全球总预算的一半。丙酮浓度梯度和丙酮通量之间的差异表明接近地表梯度,这表明需要研究地表海洋丙酮预算。

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