Evaluation and improvement of CAMS-derived CCN number concentrations using in-situ measurements
Abstract. Cloud condensation nuclei (CCN) are essential components of aerosol-cloud interactions (ACI). Thus, a precise knowledge about their number concentrations (Nccn) is crucial for climate models and ACI studies. This study presents a comprehensive evaluation of the recently published CAMS-derived total Nccn using direct observations from 25 ground-based sites. The analysis specifically focuses on the temporal variability, the applicability of CAMS-derived Nccn across different environments and pollution regimes and in particular, the sensitivity of CCN to supersaturation. For the latter aspect, a bias shift is identified in simulated Nccn that correlates to the ratio of the two dominant CCN species, likely reflecting assumptions in the underlying size distributions and/or emissions fractions. To address this issue, we developed an observation-based parametrization that is applied to CAMS-derived total Nccn without modifying aerosol size distributions or species concentrations. This approach substantially reduces biases leading the way to an improved version of CAMS-derived Nccn.
The paper addresses two relevant scientific modelling questions that are relevant to GMD, namely the performance of CAMS derived CCN number concentrations with respect to in-situ ground-station observations and possible corrections to improve that performance. Both the evaluation against a large set of ground-station observations from varied environments, and the proposed correction are novel and present important advances for the field.
While the evaluation against in-situ observations is very valuable and well documented, the level of agreement between CAMS and observations is overstated as follows:
Regarding the method of comparison between CAMS and observations, CAMS derived NCCN are at 0UTC only, but the full diurnal cycle of in-situ observations is used (Section 2.3 Data Treatment). It is worth questioning whether diurnal cycles in observed NCCN lead to a bias here. The approach of longer temporal averaging taken here is not sufficient to remove such a bias. If hourly observations are available from the stations, it should be straightforward to test this.
The method for deriving the correction factor is well justified in terms of justifying an s-dependent k parameter, and in using empirical fits of the Nccn-s spectrum to derive this. Limitations in this method being unable to use the full 3-hourly CAMS reanalysis data or change the underlying size distribution are well justified. However, aspects of the method seem unjustified and sensitivities to the large uncertainties involved not fully investigated. Details of these are as follows:
More minor comments are as follows:
Daily 11day month Block2024 (daily)
SGP 0.069 0.133 0.709 0.24
PVC 0.296 (0.098) (0.360) 0.66
PGH 0.532 0.623 (0.480) 0.41