Calibration and evaluation of broad supersaturation scanning (BS2) cloud condensation nuclei counter for rapid measurement of particle hygroscopicity and CCN activity

Najin Kim, Yafang Cheng, N. Ma, M. Pöhlker, T. Klimach, T. Mentel, Ovid O. Krüger, U. Pöschl, H. Su
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Abstract

Abstract. For understanding and assessing aerosol-cloud interactions and their impact on climate, reliable measurement data of aerosol particle hygroscopicity and cloud condensation nuclei (CCN) activity are required. The CCN activity of aerosol particles can be determined by scanning particle size and supersaturation (S) in CCN measurements. Compared to the existing differential mobility analyzer (DMA)-CCN activity measurement, a broad supersaturation scanning CCN (BS2-CCN) system, in which particles are exposed to a range of S simultaneously, can measure the CCN activity with a high time-resolution. Based on a monotonic relation between the activation supersaturation of aerosol particles (Saerosol) and the activated fraction (Fact) of the BS2-CCN measurement, we can derive κ, a single hygroscopicity parameter, directly. Here, we describe how the BS2-CCN system can be effectively calibrated and which factors can affect the calibration curve (Fact – Saerosol). For calibration, size-resolved CCN measurements with ammonium sulfate and sodium chloride particles are performed under the three different thermal gradient (dT) conditions (dT = 6, 8, and 10 K). We point out key processes that can affect the calibration curve and thereby need to be considered as follows: First, the shape of the calibration curve is primarily influenced by Smax, the maximum S in the activation tube. We need to determine appropriate Smax depending on particle size and κ to be investigated. To minimize the effect of multiply charged particles, small geometric mean diameter (𝐷𝑔) and 𝜎𝑔 geometric standard deviation (𝜎𝑔) in number size distribution are recommended when generating the calibration aerosols. Last, Fact is affected by particle number concentration and has a decreasing rate of 0.02/100 cm−3 due to the water consumption in the activation tube. For evaluating the BS2-CCN system, inter-comparison experiments between typical DMA-CCN and BS2-CCN measurement were performed with the laboratory-generated aerosol mixture and ambient aerosols. Good agreements of κ values between DMA-CCN and BS2-CCN measurements for both experiments show that the BS2-CCN system can measure CCN activity well compared to the existing measurement, and can measure a broad range of hygroscopicity distribution with a high time-resolution (~1 second vs. few minutes for a standard CCN activity measurement). As the hygroscopicity can be used as a proxy for the chemical composition, our method can also serve as a complementary approach for fast and size-resolved detection/estimation of aerosol chemical composition.
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用于快速测量粒子吸湿性和CCN活性的广泛过饱和扫描(BS2)云凝结核计数器的校准和评价
摘要为了理解和评估气溶胶与云的相互作用及其对气候的影响,需要可靠的气溶胶颗粒吸湿性和云凝结核(CCN)活动的测量数据。气溶胶颗粒的CCN活性可以通过扫描CCN测量中的颗粒大小和过饱和(S)来确定。与现有的差分迁移率分析仪(DMA)-CCN活度测量相比,一种同时暴露于S范围内的宽过饱和扫描CCN (BS2-CCN)系统可以以高时间分辨率测量CCN活度。基于气溶胶粒子的活化过饱和度(Saerosol)与BS2-CCN测量的活化分数(Fact)之间的单调关系,我们可以直接导出单个吸湿性参数κ。在这里,我们描述了如何有效地校准BS2-CCN系统以及哪些因素会影响校准曲线(Fact - Saerosol)。为了校准,在三种不同的热梯度(dT = 6、8和10 K)条件下,使用硫酸铵和氯化钠颗粒进行尺寸分辨CCN测量。我们指出了影响校准曲线的关键过程,因此需要考虑如下:首先,校准曲线的形状主要受激活管中最大S Smax的影响。我们需要根据要研究的颗粒大小和κ来确定适当的Smax。为了尽量减少多重带电粒子的影响,在产生校准气溶胶时,建议采用较小的几何平均直径(𝐷𝑔)和相对较小的几何标准差(𝑔)。最后,Fact受颗粒数浓度的影响,由于活化管中用水量的影响,其下降速率为0.02/100 cm−3。为了评估BS2-CCN系统,在实验室产生的气溶胶混合物和环境气溶胶中进行了典型DMA-CCN和BS2-CCN测量的相互比较实验。两个实验中DMA-CCN和BS2-CCN测量值之间的κ值一致,表明与现有测量相比,BS2-CCN系统可以很好地测量CCN活性,并且可以以高时间分辨率测量大范围的吸湿性分布(约1秒,而标准CCN活性测量为几分钟)。由于吸湿性可以作为化学成分的代表,我们的方法也可以作为快速和大小分辨的气溶胶化学成分检测/估计的补充方法。
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