Aerosol hygroscopicity and CCN properties at remote sites

Page 66

Chapter 4. Measured and modeled properties of CCN at Stordalen

A

„Externally Mixed“

B

Involving full GF-PDF into the CCN prediction

„Internally Mixed“

C

Involving averaged GF into the CCN prediction

„Constant Chemistry“

D

„Unknown Chemistry“ Assuming

Involving mean of

κ = 0.1, 0.2, 0.3, or 0.6

all averaged GFs

for the CCN prediction

into the CCN prediction

GF

size dependence: temporal variability: mixing state:

Mean of all Avg GF (at Dp)

PDF

GF

   

   

chemistry proxy:

Avg GF (at Dp)

PDF

GF-PDF (at Dp)

PDF

HTDMA data

PDF

κ = 0.1, 0.2, 0.3, or 0.6

GF

GF

   

   

Size distribution measured

Dp

Dp

Dp

Dp

sharp cut, constant in time

#CN, #CCN

sharp cut, constant in time

#CN, #CCN

sharp cut, variable in time

#CN, #CCN

#CN

#CN, #CCN

gradual cut, variable in time

Dp

Figure 4.1.: Schematic of the different CCN prediction approaches. The approaches involve A) the full measured GF-PDF from HTDMA measurements (”Externally Mixed”), B) the time dependent averaged GF of the GF-PDFs from HTDMA measurements (”Internally Mixed”), and C) the temporal mean of all averaged GF s from HTDMA measurements (”Constant Chemistry”) as a proxy for the aerosol’s chemical composition. The time dependence of the hygroscopic behavior is illustrated by showing two cases (solid and dotted lines) in A), B) and C). Additionally, in approach D) a CCN prediction was done by assuming the whole aerosol to have a constant κ of 0.1, 0.2, 0.3, or 0.6 (”Unknown Chemistry”). measurements, in order to describe the hygroscopic behavior of the particles in each size bin of the CN number size distribution at a certain time. Figure 4.2 illustrates the calculation of fCCN at Dp = 75 nm with one example. Particles of this dry diameter can, according to K¨ohler theory, only act as CCN at SS = 0.70% and 0.40% if their growth factor at RH = 85% is larger than 1.08 and 1.23, respectively. fCCN is 1 at the higher SS because all particles have a growth factor > 1.1. fCCN is < 1 at the lower SS because a considerable fraction of particles has a growth factor < 1.23. Taking the mixing state into account results in a gradual transition of the activated fraction from 0 to 1 with increasing dry diameter, as shown in Figure 4.3A (same example as in Figure 4.2). The activation transition occurs between Dp ≈ 32–71 nm and Dp ≈ 47–93 nm at SS = 0.70%, and 0.40%, respectively (grey and black solid lines in Figure 4.3A). The predicted CCN number concentration NCCN is obtained by integrating the number size distribution weighted with the activated fraction: Z ∞ dNCN NCCN (SS, t) = fCCN (SS, Dp , t) (Dp , t)d log Dp (4.3) d log Dp 0 This integration is in practice approximated by a summation over the size bins of the measured number size distribution and the integration boundaries are limited to the diameter range covered by the measurement. Externally mixed aerosols with multimodal GF-PDFs as 56


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