The effect of rapid relative humidity changes on fast filter-based aerosol-particle light-absorption measurements: uncertainties and correction schemes

Abstract

Abstract. Measuring vertical profiles of the particle light-absorption coefficient by using absorption photometers may face the challenge of fast changes in relative humidity (RH). These absorption photometers determine the particle light-absorption coefficient due to a change in light attenuation through a particle-loaded filter. The filter material, however, takes up or releases water with changing relative humidity (RH in %), thus influencing the light attenuation. A sophisticated set of laboratory experiments was therefore conducted to investigate the effect of fast RH changes (dRH ∕ dt) on the particle light-absorption coefficient (σabs in Mm−1) derived with two absorption photometers. The RH dependence was examined based on different filter types and filter loadings with respect to loading material and areal loading density. The Single Channel Tricolor Absorption Photometer (STAP) relies on quartz-fiber filter, and the microAeth® MA200 is based on a polytetrafluoroethylene (PTFE) filter band. Furthermore, three cases were investigated: clean filters, filters loaded with black carbon (BC), and filters loaded with ammonium sulfate. The filter areal loading densities (ρ*) ranged from 3.1 to 99.6 mg m−2 in the case of the STAP and ammonium sulfate and 1.2 to 37.6 mg m−2 in the case the MA200. Investigating BC-loaded cases, ρBC* was in the range of 2.9 to 43.0 and 1.1 to 16.3 mg m−2 for the STAP and MA200, respectively. Both instruments revealed opposing responses to relative humidity changes (ΔRH) with different magnitudes. The STAP shows a linear dependence on relative humidity changes. The MA200 is characterized by a distinct exponential recovery after its filter was exposed to relative humidity changes. At a wavelength of 624 nm and for the default 60 s running average output, the STAP reveals an absolute change in σabs per absolute change of RH (Δσabs∕ΔRH) of 0.14 Mm−1 %−1 in the clean case, 0.29 Mm−1 %−1 in the case of BC-loaded filters, and 0.21 Mm−1 %−1 in the case filters loaded with ammonium sulfate. The 60 s running average of the particle light-absorption coefficient at 625 nm measured with the MA200 revealed a response of around −0.4 Mm−1 %−1 for all three cases. Whereas the response of the STAP varies over the different loading materials, in contrast, the MA200 was quite stable. The response was, for the STAP, in the range of 0.17 to 0.24 Mm−1 %−1 and, in the case of ammonium sulfate loading and in the BC-loaded case, 0.17 to 0.62 Mm−1 %−1. In the ammonium sulfate case, the minimum response shown by the MA200 was −0.42 with a maximum of −0.36 Mm−1 %−1 and a minimum of −0.42 and maximum −0.37 Mm−1 %−1 in the case of BC. A linear correction function for the STAP was developed here. It is provided by correlating 1 Hz resolved recalculated particle light-absorption coefficients and RH change rates. The linear response is estimated at 10.08 Mm−1 s−1 %−1. A correction approach for the MA200 is also provided; however, the behavior of the MA200 is more complex. Further research and multi-instrument measurements have to be conducted to fully understand the underlying processes, since the correction approach resulted in different correction parameters across various experiments. However, the exponential recovery after the filter of the MA200 experienced a RH change could be reproduced. However, the given correction approach has to be estimated with other RH sensors as well, since each sensor has a different response time. And, for the given correction approaches, the uncertainties could not be estimated, which was mainly due to the response time of the RH sensor. Therefore, we do not recommend using the given approaches. But they point in the right direction, and despite the imperfections, they are useful for at least estimating the measurement uncertainties due to relative humidity changes. Due to our findings, we recommend using an aerosol dryer upstream of absorption photometers to reduce the RH effect significantly. Furthermore, when absorption photometers are used in vertical measurements, the ascending or descending speed through layers of large relative humidity gradients has to be low to minimize the observed RH effect. But this is simply not possible in some scenarios, especially in unmixed layers or clouds. Additionally, recording the RH of the sample stream allows correcting for the bias during post-processing of the data. This data correction leads to reasonable results, according to the given example in this study.

Connecting the Light Absorption of Atmospheric Organic Aerosols with Oxidation State and Polarity

“…The attenuation of the sample collected on the membrane can be defined using the Beer−Lambert law. 64 The loading effect of MA200 due to particle accumulation on filter was automatically corrected by the dual spot measurements. 65 The performance of MA200 relies on strict calibrations that account for the intrinsic artifacts.…”

Observational data from uncrewed systems over Southern Great Plains

“…Previous studies have evaluated STAP's in-flight performance (Telg et al, 2017;Düsing et al, 2019;Pikridas et al, 2019). Düsing et al (2019) pointed out that artifacts in STAP data due to rapid changes in RH can be corrected using a correction factor of 10.08 Mm −1 s −1 for every 1 % change in RH. Note that no correction was applied to the flight data in 2021 because there was no significant RH variation during the flight.…”

“…Known as a "hot spot" for land-atmosphere interactions, the ARM Southern Great Plains (SGP) atmospheric observatory is located in central Oklahoma, where significant diurnal variability is observed in both thermodynamic and kinematic properties (Klein et al, 2015). ARM observations from this location are leveraged to understand the occurrence and impact of mesoscale disturbances on the ABL and connections between ABL processes and the life cycle of shallow convective clouds (Fast et al, 2019). In this sense, extending the surfacebased data collected at the SGP facility to include coincident airborne observations is critical in understanding the multitude of processes driving the ABL and its impacts on cloud development, weather, and climate.…”

Comment on acp-2021-21

“…Diffusional losses at the OPSS size-range are negligible. The aerosol was dried with a silica-bead based dryer similar to the one on ACTOS to dampen sudden changes in the RH of the aerosol stream, which can have significant influences on the filter-based absorption measurements of the STAP as shown, for instance, by Düsing et al (2019). They estimated a 375 deviation of around 10.08 (± 0.12) Mm −1 % -1 s (10.08 Mm -1 per unit change of RH (in %) per second), which is significant, especially under clean conditions.…”