Calibration of a Photometric Cloud Condensation Nucleus Counter Designed for Deployment on a Balloon Package

D. J. Delene* and T. Deshler

Department of Atmospheric Sciences, University of Wyoming, Laramie

 

Revised manuscript submitted to the Journal of Atmospheric and Oceanic Technology, June 11, 1999.

 

Corresponding Author:      David J. Delene

NOAA Climate Monitoring and Diagnostics Lab

R/E/CG1 325 Broadway, Boulder, CO 80303

Office Phone (303) 497-6189

FAX (303) 497-5590

email ddelene@cmdl.noaa.gov

 

___________

*Now at the Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado/NOAA, Boulder.


ABSTRACT

The importance of atmospheric aerosols in understanding global climate changes has renewed interest in measurements of cloud condensation nuclei (CCN).  To obtain high-resolution (125 m) vertical profiles of CCN number concentration, a balloon-borne instrument was developed.  The instrument deduces the CCN concentration from measurements of laser light scattered by water droplets that condense on CCN within a static thermal-gradient diffusion chamber.  The amount of light scattering is linearly proportional to the number of droplets within the diffusion chamber.  Correlating the number of droplets within the sample volume with the amount of light scattered by the droplets provides the calibration constant relating scattered light to CCN concentration.  The calibration was tested by comparisons between the CCN counter and a condensation nuclei (CN) counter when sampling monodisperse aerosol larger than the CCN counter’s critical activation size.  The calibration constant depends on supersaturation and slightly on the size of CCN that activate to form droplets.  For dry NaCl aerosol between 35 and 160 nm, the calibration constant varies by less than 10% at 1% supersaturation.  Calibration on ambient atmospheric aerosol is similar to calibration on laboratory-generated polydisperse NaCl aerosol indicating that the laboratory calibration can be applied to field measurements.  The time required for the activation and growth of droplets within the diffusion chamber is similar during field and laboratory measurements.  Overall, the uncertainty of the calibration constant for the balloon-borne CCN counter is approximately 10% at 1% supersaturation.


1.      Introduction

   Modification for the balloon-borne CCN counter.

Cloud condensation nuclei (CCN) have a major influence on the cloud droplet number concentration and hence the radiative properties of clouds.  Increases in CCN concentrations, resulting from increased SO2 emissions, has been suggested as a mechanism which could modify clouds properties sufficiently to affect global climate (Wigley, 1989; Twomey, 1991).  The indirect affect of CCN on climate has started to be incorporated into global climate models (Meehl et al., 1996; Chuang et al., 1997; Pan et al., 1998).  Pan et al., (1998) concluded from comparisons of climate models that refining input parameters might be more important than improving models to minimize uncertainties.  CCN measurements are an important link in relating changes in aerosol concentration to changes in cloud droplet number concentration (Boucher and Lohmann, 1995; Liu et al., 1996).  A balloon-borne CCN counter has been developed to provide vertical profiles of CCN with a resolution of approximately 125 m.  Since measurements obtained with the CCN counter are to be related to concurrent aerosol measurements instead of simply monitoring changes in CCN concentration, an accurate calibration of the CCN counter is critical.  The main objective here is to describe the calibration of the balloon-borne CCN counter and its influence on the accuracy of field measurements.

  Description of the CCN counter.

The balloon-borne CCN counter described here is similar to other static thermal-gradient diffusion chamber instruments (Radke and Hobbs, 1969; Lala and Jiusto, 1977; Bartlett and Ayers, 1981; Hoppel and Wojciechowski, 1981; Lala, 1981).  The instrument described here uses a 670 nm solid-state laser to illuminates the center of the chamber where the supersaturation is held at a prescribed value.  To keep the instrument lightweight, a photodetector, instead of a photographic or charged coupled device (CCD) camera, is used to measure the CCN concentration.  The photodetector voltage relates the amount of scattered light to the CCN concentration through the calibration constant for the instrument.

To obtain a CCN measurement at a single supersaturation requires 30 s.  At the start of a measurement, the bottom plate temperature is calculated based on the top plate temperature and the desired supersaturation.  The top plate temperature is allowed to float with the enclosed temperature of the CCN counter, and the bottom plate temperature is controlled using thermoelectric coolers to achieve a prescribed supersaturation.  The temperature difference between the top and the bottom plate is checked for 5 s to ensure that it is within the prescribed range (± 0.2 °C).  The chamber is flushed for 5 s to remove air from the previous sample.  A new air sample is captured and held within the chamber for 20 s.  When a new air sample enters the chamber, CCN activate and droplets form, grow, and fall out. 

Following the suggestion of Katz and Mirabel (1975), the temperature and vapor pressure between the top and the bottom plates are assumed to be linear functions of the height above the bottom plate.  Both the top and the bottom plates are kept wet for up to 3 hours using saturated blotter papers.  Delene et al. (1998) provided an initial description of the balloon-borne CCN counter, described calibration at 1% supersaturation on NaCl aerosols, and presented some preliminary CCN profiles.  The focus here is on dependence of the instrument’s calibration on supersaturation, aerosol size, and aerosol type.

2.      Standard Calibration Procedure

   Description of the calibration setup and procedure.

Calibration of the CCN counter is accomplished using the method of Delene et al. (1998).  The CCN concentration is equated to the number of water droplets in a measured portion of the laser beam which are counted using a video camera and personal computer (PC) frame grabber card.  Concurrent with the video counts, the photodetector voltage is measured.  A least squares linear fit between photodetector voltage and droplet count determines the calibration slope.  The calibration constant for the CCN counter is defined to be the calibration slope divided by the video sample volume.  The calibration here differs from Delene et al. (1998) by using a new video camera with higher resolution, greater magnification, lower noise, and greater light sensitivity.  The new video camera counts more droplets within a 10 mm segment of the laser beam than does the old video camera.  Recent inquiries of the laser manufacturer indicated that the cross section of the laser beam was 5 x 1.8 mm instead of the 4 x 1 mm used by Delene et al. (1998).  Measuring the laser’s cross section is uncertain due to blooming of the laser beam on the measurement apparatus.  Our measurements of the laser beam width give 5.5 ± 0.5 mm which compares favorably to the laser manufacturer’s width of 5.0 mm.  Although the new video camera counts more droplets, a larger sample volume is used, which results in a reduction of the calibration constant by approximately 18% compared to the calibration constant determined with the old video camera.

The gain setting of the PC frame grabber card is used to test the sensitivity of the video camera.  The number of droplets counted with the new video camera does not increase with gain increases on the frame grabber card.  In contrast, the number of droplets counted with the old video camera does increase with gain increases on the frame grabber card.  Therefore, the new camera seems sensitive enough to count all droplets within the field of view of the laser beam without over counting due to video noise.

   Describe the setup of the lens focus and alignment of the video camera.

Correctly setting the video camera’s lens focus is critical for accurate calibrations; however, it is difficult to set the lens focus so that the whole depth of the laser beam is within focus.  The focus of the lens is set by focusing on hairs of a Q-tip placed within the video sample volume.  The focus is checked periodically during calibration by examining the video camera’s output on a monitor to ensure that no out of focus droplets (large droplets with dim centers) are present.  The laser beam is at a 45-degree angle with respect to the lens and the sample length along the laser beam is 10 mm, thus the depth of field needs to be 14 mm.  This is significantly larger than the 5 mm width of the laser beam.  In an attempt to decrease the sensitivity of the focus adjustment, the focal length was increased, which increases in the depth of field but reduces the magnification of droplets.  Increasing the distance from the center of the chamber to the lens from 46 to 52 mm results in a decrease of the 1% supersaturation calibration constant by approximately 10%.  The reduced magnification resulting from this small increase in length probably resulted in under counting because some droplets were now too small to be detected.  For all calibrations presented here the lens was placed at 46 mm from the center of the chamber to give the greatest magnification of droplets possible and the lens focus was carefully set to ensure that all droplets within the video sample were within focus.

  Talk about the CCN counter’s calibration at 1% supersaturation using NaCl aerosols (Figure 1).

Standard calibration of the CCN counter consists of obtaining several hundred comparisons of photodetector voltage and droplet concentration using laboratory aerosol produced from an ultrasonic vaporizer using a solution of 0.1 g/L of NaCl.  The aerosol concentration is varied during a measurement sequence by changing the amount of filtered air mixed with the generated aerosol.  Figure 1 presents an example of calibration data using the standard calibration method.  The number of droplets, at the time of the photodetector voltage peak, and the video sample volume are used to determine the CCN concentration.  The voltage peak method, instead of the voltage summation method of Delene et al. (1998), is used here because the resulting calibration constants are similar, and it simplifies examination of the calibration dependence on supersaturation.

3.      Testing the Standard Calibration Procedure

  Describe the verification of the CCN counter’s calibration using the TSI CCN counter.  Describe the production of monodisperse aerosol.

The video counting of droplet in the CCN chamber, and hence the CCN calibrations, can be checked by comparing the CCN concentration against measurements made by a model 3010 TSI CN counter, when sampling monodisperse aerosol larger than the CCN counter’s critical activation size.  The model 3010 CN counter is a good instrument to compare the CCN counter with since the detection efficiency is greater than 0.999 and the systematic error due to coincidence is less than 2% for aerosols larger than 30 nm diameter and concentrations less than 3000 cm-3 (Mertes et al., 1995).  Monodisperse aerosol of selected sizes are produced by atomizing a NaCl solution, and passing the aerosol through a diffusion drier and a differential mobility analyzer (DMA) (Knutson and Whitby, 1975) into a conductive bag, partially filled with filtered air.  Sampling directly from the DMA was avoided because of the possibility that the counters will affect the flow rates of the DMA, and hence the aerosol size distribution.  The CCN and CN counters sample concurrently from the bag once it is filled.  During sampling, the aerosol concentration decreases due to wall losses.  Coagulation of aerosols within the bag is less than 2% for the concentrations (<1000 cm-3) and times (< 4 hr) of the laboratory comparisons (Willeke and Baron, 1993).  Therefore, the size of the aerosols within the bag is considered to remain constant throughout the laboratory tests.

  Describe the results for the comparison between the CCN and CN counter (figure 2).

Figure 2 presents an example of the CCN and CN counters measuring 125 nm monodisperse NaCl aerosol.  The CCN concentration is determined using the video camera to count droplets, at the time of the photodetector voltage peak, over a predetermined video sample volume.  Below a concentration of 500 cm-3, the averaged CCN concentrations agree with the CN concentrations.  Above a concentration of 500 cm-3, the CCN concentrations are low compared to the CN concentrations.  The low CCN concentrations may be the result of under counting droplets due to droplet coincidence within the viewing volume of the video camera.  For the 3.5 hours required to generate Fig. 2, the CCN counter was run continuously without rewetting the saturated blotter papers indicating that the saturated blotter papers on the top and the bottom plates will remain moist for over three hours, the duration of a balloon flight.

4.      Calibration Dependence on Supersaturation

  Discussion of the CCN counter’s calibration dependence on supersaturation (Figure 3).

The condensation growth rate of droplets is proportional to supersaturation; therefore, at higher supersaturations droplets will obtain sizes large enough to fall in a shorter amount of time.  This is confirmed by observations of droplets within our thermal-gradient diffusion chamber.  Changes in droplet size will affect the calibration slope since the amount of scattered laser light is proportional not only to droplet number but also to droplet size.  Figure 3 illustrates the dependence of the calibration slope on supersaturation, which is fitted following the method of de Oliveira and Vali (1995).  The increase in the calibration slope as the supersaturation decrease indicates that droplets decrease in size as the supersaturation decreases and that the effect of this decrease on scattering is not linear.

  Give example for the average ratio of photodector voltage to maximum photodector voltage for 1.0 and 0.3 % supersaturation (Figure 4).

The droplet size dependence on supersaturation is apparent in the time dependence of the ratio of droplet number, or photodetector voltage, to the maximum droplet number, or photodetector voltage.  Figure 4 shows averages of these ratios over hundreds of samples as the CCN counter’s chamber is flushed (first 5 s) and droplets activate, grow, and fall out.  Ratio averages never equal one since the peak ratio does not always occur at the same time for each sample.  The peak in droplet number (solid lines) occurs before the peak in photodetector voltage (dashed lines).  This indicates that droplets continue to grow larger, and hence scatter more light, after the occurrence of the droplet number peak.  Averages of the ratios at 1% supersaturation, compared to 0.3% supersaturation, have peaks that occur earlier in the measurement cycle and are narrower by a factor of 2.  This difference is due to the droplet size dependence on supersaturation that results from the supersaturation dependence of the condensation growth rate of droplets.  Broad peaks in the averages of the ratios of the droplet number indicate that it does not make a significant difference exactly where the count of the droplet number peak is obtained, however, with narrow peaks in the droplet number it may be more important.  This may be the reason that in Fig. 3 the data points, when compared to the data fit, show a slight (approximately 5%) under counting at high supersaturations and a slight (approximately 5%) over counting at lower supersaturations.

  Talk about how the time to the peak changes with supersaturation (Figure 5).  Talk about how the time between number and voltage peak changes with supersaturation (Figure Error! Bookmark not defined.).

Figure 5 illustrates the time required to reach the droplet number and photodetector voltage peaks as a function of supersaturation.  The standard deviation of the average time to reach the photodetector voltage peak increases with decreasing supersaturation.  The increase in the variability in time to reach the peaks is due to broader peaks at lower supersaturation (Fig. 4).  The time between the average droplet number peak and the average photodetector voltage peak decreases linearly from 2.5 s at 0.3 % supersaturation to 1.0 s at 1.6% supersaturation (Fig. 5).  This further illustrates the dependence of condensation growth rate on supersaturation.  Droplets grow more quickly at higher supersaturations reducing the time between the droplet number and photodetector voltage peak.

5.      Calibration Dependence on Aerosol Type

  Talk about the aerosol size spectrum that we use to calibrate the instrument (Figure 6).

The size distribution and chemical composition of atmospheric aerosols is highly variable in space and time due to the complex interrelationships between many different sources and sinks (Singh, 1995).  Although the laboratory-generated calibration aerosol has a bimodal, polydisperse size spectrum, it consists of totally soluble aerosols, and the size distribution does not vary significantly from sample to sample.  Thus, the calibration aerosols are different from ambient atmospheric aerosols.  Figure 6 presents representative aerosol size spectra for the NaCl laboratory-generated aerosols produced with the vaporizer.  The aerosol spectra are obtained using a TSI differential mobility analyzer and CN counter (Birmili et al., 1997).

  Describe the systematic variability in the CCN counter’s calibration (Table 1).

To determine how the laboratory calibration is related to field measurements, the CCN counter was calibrated using different aerosol types.  Table 1 summarizes several different calibrations of the CCN counter.  The first three rows give the calibration results for three calibrations using the standard polydisperse NaCl aerosol.  Row one results are from March 1998, row two results are from June 1998, and row results are three from October 1998.  No changes in the configuration of the CCN counter were made between these calibrations; however, the CCN counter was removed from the laboratory calibration bench between each of these calibrations and used elsewhere.  The random errors of the calculated calibration slopes are given by the standard deviations in Columns 2 and 3.  The change in the calibration slopes (Column 2 and 3) for the standard calibration method (Rows 1-3) is larger than the random errors for any one calibration.  Systematic differences in the setup and alignment of the CCN counter with the video calibration system are believed to cause the variability between calibrations.  The observed variability in the standard calibration method (Rows 1-3) indicates that the calibration is repeatable to within 10%.

   Calibration dependence on aerosol size.

Roberts et al. (1997) observed a photodetector calibration dependence on the initial size of CCN in a static thermal-gradient diffusion chamber.  To check for a calibration dependence on CCN size, the instrument was calibrated using monodisperse aerosol of several different sizes.  The generation and sampling of monodisperse aerosol was described earlier.  Results of calibrations on different monodisperse aerosol sizes are given in Rows 4-9 of Table 1.  Aerosol size appears to have no detectable effect on the time to reach either the droplet number peak or the photodetector voltage peak (Columns 4 and 5); however, an approximate 10% change in the calibration slope is observed between 35 nm and 120/160 nm NaCl aerosol.  Further analysis of the measurements shows that there is no dependence between the time to reach the peaks and the aerosol concentration.

  Discussion of the observed calibration dependence on aerosol size.

The calibration slope dependence on aerosol size indicates that the CCN size affects droplet size at the time of the photodetector voltage peak.  This droplet size dependence on initial CCN size is not intuitive.  Droplets are a few micrometers in diameter at the photodetector voltage peak based on their fall velocities.  Since the diffusional droplet growth rate is proportional to the inverse of droplet radius, the droplet size spectrum becomes narrower as droplets grow to larger sizes (Howell, 1949). Intuitively, the narrowing of the droplet spectrum is expected to cause the droplets to be at approximately the same relative size at the photodetector voltage peak.  Therefore, the calibration should not depend on the initial CCN size.

   Show the CCN counter calibration on outside aerosol (Figure 7).

Due to the dependence of the calibration on CCN size, the calibration may change if we calibrate on atmospheric aerosol instead of laboratory generated aerosol (Fig. 6).  Figure 7 shows calibration data using ambient atmospheric aerosols obtained from outside the laboratory building on three consecutive mornings in early October at Laramie, Wyoming.  The measurements were made around sunrise under meteorological conditions of clear skies and high pressure, similar to a typical balloon flight.  The ambient aerosol concentration was varied by diluting the aerosol sample with filtered air.  Calibration on outside aerosol does not show a significant difference from the laboratory-generated NaCl aerosol.  The calibration slope obtained using the outside air is within the range of slopes obtained for the 3 different calibrations on polydisperse laboratory aerosol (Table 1, Rows 1-3).  Furthermore, the average time to reach the peak values (Table 1, Columns 4 & 5) and shape of the average ratio peaks (not shown) are consistent with calibration on standard laboratory generated aerosol.  The consistency between the calibration on laboratory-generated aerosol and atmospheric aerosol measured at the surface in Laramie, Wyoming, suggests that the laboratory calibration can be applied to field measurements. 

It is unknown if atmospheric aerosols in the upper troposphere or at different geographic locations are different enough to invalidate the calibration.  While it is impossible to check the calibration on all types of aerosols, the average time to reach the photodetector voltage peak may indicate measurements that are not consistent with the laboratory calibration.  Table 2 gives the time to reach the photodetector voltage peak for various field measurements.  The surface and lower tropospheric time to reach the photodetector voltage peak are consistent with the laboratory calibrations (Table 1).  The upper tropospheric time to reach the photodetector voltage peak shows more variability than the laboratory calibration data, but are still within the range of the laboratory calibrations.  The increase in variability in the upper troposphere may be related to measurements being near the detection limit of the CCN counter.  The peak is less well defined near the detection limit since only a few particles are within the photodetector sample volume.

6.      Calibration Error

   Talk about the accuracy of the supersaturation within the thermal gradient diffusion chamber.

Accurate CCN measurements require accurate droplet concentrations from the scattered light signal and knowledge of the supersaturation within the thermal-gradient diffusion chamber.  The supersaturation within the chamber depends on the temperature difference between the top and bottom plates.  Measurements with a thermocouple placed on the top and the bottom saturated blotter papers, within the thermal-gradient diffusion chamber, confirm that the temperature difference is maintained to within ± 0.1 °C or ± 0.05% supersaturation at a supersaturation of 1%.  The supersaturation within the diffusion chamber, however, could be incorrect due to the occurrence of transient supersaturations before steady-state temperature and moisture gradients are established (Fitzgerald, 1970; Saxena et al., 1970).  To avoid transient supersaturations that exceed the steady-state peak value, it is advantageous to have air samples enter the diffusion chamber at the top plate temperature with a low relative humidity (Fitzgerald, 1970; Saxena et al., 1970).  The balloon-borne CCN counter’s top plate temperature is allowed to float with the instrument enclosure temperature.  Before an air sample enters the chamber, it travels though 5 mm, inside diameter, stainless steel tubing within the instrument enclosure for approximately 0.3 s.  Heat transfer calculations show that the air sample equilibrates with the enclosure temperature of the CCN counter before entering the chamber.  Heat produced by the electronics ensures that the enclosure temperature is higher (from approximately 3 °C at the surface to 30 °C or more in the upper troposphere) than the ambient air temperature.  Therefore, air entering at the enclosure temperature of the CCN counter also ensures that the relative humidity of the air sample is lower than the ambient relative humidity.  Since air samples enter the CCN chamber at the enclosure temperature, transient supersaturations above the steady-state peak values are believed not to occur within the chamber under field measurement conditions.

  Poisson counting error. Error due to not knowing the initial aerosol size.

The relative error in CCN concentration can be computed using Poisson counting statistics (Horvath et al., 1990).  The Poisson counting error can be significant at upper tropospheric concentrations since there are very few particles present in the laser beam.  The counting error is larger for video counting of droplets than for photodetector counting of droplets due to the photodetector sample volume being approximately twice the video sample volume.  The photodetector sample volume of 0.16 cm-3 determined by Delene et al (1998) was verified using measurements collected during laboratory calibrations on monodisperse aerosols.  The Poisson counting error agrees with the standard deviation of 10 min averages of CCN concentration.  Poisson counting statistics give a range of errors from 36 to 11% for CCN concentrations (at ambient pressure) of 50 to 500 cm-3.  The measurement threshold is approximately 20 cm-3, which corresponds to 3 droplets being within the photodetector sample volume.  Below this concentration, the photodetector peak is not discernible from the base line photodetector voltage determined during the chamber flush at the beginning of the sample.

The agreement between the CCN counter and a laboratory standard, commercially built TSI CN counter seen in Fig. 2 indicates a good absolute calibration of the CCN counter.  It also indicates that the video sample volume is correct, and the video camera/lens system is adequate to calibrate the CCN counter at 1% supersaturation.   The variability, approximately 5-10%, between standard calibrations of the CCN counter (Table 1, Rows 1-3) is thought to result from systematic differences in the setup and alignment of the CCN counter with the video calibration system.  Counting droplets using the photodetector to measure the scatter light signal, instead of counting droplets with a video camera system, has a small dependence on aerosol size.  This size dependence is approximately the same as the systematic error in the standard laboratory calibration.  The calibration dependence on aerosol size does not seem to have a great affect in the real atmosphere since calibration on real atmospheric aerosol produces a calibration similar to the standard laboratory calibrations.

Considering all calibration results presented here, the calibration constant relating photodetector voltage to CCN concentration for the standard laboratory calibration of the balloon-borne CCN counter is believed to have an accuracy of 10% at 1% supersaturation.  The video calibration of the CCN counter appears to work at supersaturations down to 0.2%.  The calibration slopes fit nicely to a power law function (Fig. 3); however, video counting of droplets is difficult at low supersaturation, due to the smaller droplets, and the dependence of the calibration constant on aerosol size may be more significant at supersaturations lower than at 1%.  The video calibration method should be verified at low supersaturations.

7.      Conclusions

A photometric CCN counter was calibrated using a video camera and PC frame grabber card to count droplets.  Droplet number is linearly related to the amount of laser light scattered by the droplets.  The standard calibration procedure for the CCN counter is repeatable to better than 10% accuracy.  The calibration relationship between droplet number and photodetector voltage was verified by a comparison between the CCN counter and a CN counter when sampling monodisperse aerosol.  Calibration of the CCN counter is found to depend on supersaturation and to have a slight dependence on the size of CCN that activate to form droplets.  The dependence on supersaturation is easily accounted for using a power law function to relate the calibration slope to supersaturation.  The calibration dependence on CCN size is less than 10% at 1% supersaturation.  Calibration on ambient atmospheric aerosol appears similar to the standard calibration procedure.  Laboratory calibration measurements, compared to field measurements at various locations and within different atmospheric layers, give average photodetector voltage peaks that occur at similar times after an air sample enters the thermal gradient-diffusion chamber.  Therefore, it appears that within the diffusion chamber atmospheric CCN behave similar to laboratory produced CCN.  Random errors in measured CCN concentration can be computed using Poisson counting statistics and range from 36 to 11% for CCN concentrations in the range of 50 to 500 cm-3.  The calibration constant that relates photodetector voltage to CCN concentration is believed to have an accuracy of 10% at 1% supersaturation.

8.      Acknowledgments

Lyle Womack and Jason Gonzales provided engineering support in conducting balloon flights and assistance in laboratory work.  Special thanks to Fred Brechtel of Colorado State University for sharing his computer programs to obtain aerosol size spectrums and CN concentrations.  Fred Brechtel also provided advice in using the differential mobility analyzer to generate monodisperse aerosols.  Greg Roberts profiled a copy of his AAAR poster and valuable discussions about his experience in calibrating a photometric CCN counter.  Jefferson Snider, Perry Wechsler, and Gabor Vali provided support, suggestion, and comments during this research.  This research was supported by a grant from the National Aeronautics and Space Administration.


9.      References

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10.  Figure Captions

Figure 1.  The photodetector voltage peak versus the number of droplets counted within the video sample volume and the corresponding droplet concentration.  Droplets are counted at the time of the photodetector voltage peak.  The droplets nucleated on polydisperse NaCl aerosols produced using a solution of 0.1 g/L of NaCl in an ultrasonic vaporizer.  The calibration slope (solid line) is the least squares linear fit to the data with a forced zero y-intercept.

Figure 2.  Measurements of the concentration of 120 nm monodisperse NaCl aerosols using the CCN counter at 1% supersaturation (circles) and CN counter (solid line).   The CCN concentration is measured using the video camera to count droplets over a predetermined video sample volume.  The CCN concentration is averaged over approximately 20 samples (10 min) with the standard deviation given by the error bars.  The decrease in concentration with time is the result of aerosol being removed to the walls of the sampling bag.  Filtered air was continuously added to the sampling bag after 115 minutes

Figure 3.  The CCN counter’s calibration slope dependence on supersaturation.  The data are fitted using the equation, C = Alpha + Beta/SS, where Alpha and Beta are calibration constants, SS is the chamber supersaturation, and C is the calibration slope.  Error bars represent one standard deviation in the calculated calibration slope.

Figure 4.  Time versus the averages of ratios of droplet number (dashed line) and photodetector voltage (solid line) to the maximum number and voltage observed during the sample.  The legends give the average and standard deviation times for the peak number of droplets and peak photodetector voltage.  Time zero is at the beginning of a 5 s chamber flush.  Following the chamber flush, an air sample is captured within the chamber, CCN active and droplets form, grow and begin to fall.

Figure 5.  Supersaturation of the CCN counter versus the average time to reach the number or voltage peak.  The error bars on the photodetector voltage time are one standard deviation of the average.  Error bars (not shown) on the average time to reach the droplet number peak are similar.  The left axis and solid triangles denote the time between the droplet number peak and photodetector voltage peak.

Figure 6. Examples of the aerosol size spectrum generated using a solution of 0.1 g/L of NaCl in an ultrasonic vaporizer.  The legend gives the total number concentration (in cm-3) for each aerosol size spectrum.

Figure 7.  CCN counter calibration data using aerosol from the ambient atmosphere outside the laboratory building in Laramie, Wyoming. The photodetector voltage peak versus the number of droplets counted within the video sample volume and the corresponding droplet concentration are shown.  Droplets are counted at the time of the photodetector voltage peak.  The calibration slope (solid line) is the least squares linear fit to the data with a forced zero y-intercept.


 

11.  Table Captions

Table 1.  Calibration of the balloon-borne CCN counter at 1% supersaturation.  The first column gives the calibration aerosol type: laboratory produced aerosol using a solution of 0.1 g/L NaCl in a vaporizer, monodisperse NaCl aerosol of different diameters, or aerosol from the ambient atmosphere outside the laboratory building.  The second column gives the calibration slope using the photodetector voltage peak.  The third column gives the calibration slope using a three-point sum around the photodetector voltage peak (Delene et al., 1998).  The fourth column gives the average time to reach the number peak in seconds since the beginning of the sample.  The last column gives the average time to reach the voltage peak in seconds since the beginning of the sample.  The first 3 rows give the results of the standard calibration of the CCN counter in March, June, and, October 1998.  The CCN counter was removed from the laboratory calibration bench between each standard calibration of the CCN counter and used elsewhere.  The calibrations

presented in rows 3-10 were preformed using the same focus and video camera alignment with the CCN counter.

Table 2.  Time to reach the photodetector volage peak for field measurements in Laramie, Wyoming (41 °N), Lauder, New Zealand (45 °S), and Fairbanks, Alaska (65 °N).  Due to a clear difference in aerosol concentration, the field measurements are divided into summer and winter seasons.  The third column gives the average and standard deviation of the time to reach  the photodetector voltage peak.  The fourth column gives the number of samples used to compute the average.

 


Figure 1.  The photodetector voltage peak versus the number of droplets counted within the video sample volume and the corresponding droplet concentration.  Droplets are counted at the time of the photodetector voltage peak.  The droplets nucleated on polydisperse NaCl aerosols produced using a solution of 0.1 g/L of NaCl in an ultrasonic vaporizer.  The calibration slope (solid line) is the least squares linear fit to the data with a forced zero y-intercept.


Figure 2.  Measurements of the concentration of 120 nm monodisperse NaCl aerosols using the CCN counter at 1% supersaturation (circles) and CN counter (solid line).   The CCN concentration is measured using the video camera to count droplets over a predetermined video sample volume.  The CCN concentration is averaged over approximately 20 samples (10 min) with the standard deviation given by the error bars.  The decrease in concentration with time is the result of aerosol being removed to the walls of the sampling bag.  Filtered air was continuously added to the sampling bag after 115 minutes

Figure 3.  The CCN counter’s calibration slope dependence on supersaturation.  The data are fitted using the equation, C = Alpha + Beta/SS, where Alpha and Beta are calibration constants, SS is the chamber supersaturation, and C is the calibration slope.  Error bars represent one standard deviation in the calculated calibration slope.


 

Figure 4.  Time versus the averages of ratios of droplet number (dashed line) and photodetector voltage (solid line) to the maximum number and voltage observed during the sample.  The legends give the average and standard deviation times for the peak number of droplets and peak photodetector voltage.  Time zero is at the beginning of a 5 s chamber flush.  Following the chamber flush, an air sample is captured within the chamber, CCN active and droplets form, grow and begin to fall.

Figure 5.  Supersaturation of the CCN counter versus the average time to reach the number or voltage peak.  The error bars on the photodetector voltage time are one standard deviation of the average.  Error bars (not shown) on the average time to reach the droplet number peak are similar.  The left axis and solid triangles denote the time between the droplet number peak and photodetector voltage peak.

Figure 6. Examples of the aerosol size spectrum generated using a solution of 0.1 g/L of NaCl in an ultrasonic vaporizer.  The legend gives the total number concentration (in cm-3) for each aerosol size spectrum.

Figure 7.  CCN counter calibration data using aerosol from the ambient atmosphere outside the laboratory building in Laramie, Wyoming. The photodetector voltage peak versus the number of droplets counted within the video sample volume and the corresponding droplet concentration are shown.  Droplets are counted at the time of the photodetector voltage peak.  The calibration slope (solid line) is the least squares linear fit to the data with a forced zero y-intercept.


 





Aerosol Type

Peak Method

Summation Method

Droplet Peak

Voltage Peak

0.1 g/L NaCl

9.44 ± 0.09

3.57 ± 0.03

10.6 ± 1.7 (s)

12.5 ± 1.5 (s)

0.1 g/L NaCl

10.08 ± 0.08

3.78 ± 0.02

10.5 ± 1.9 (s)

12.4 ± 1.4 (s)

0.1 g/L NaCl

9.73 ± 0.13

3.64 ± 0.03

10.6 ± 1.6 (s)

12.2 ± 1.1 (s)

35 nm

10.20 ± 0.18

3.94 ± 0.05

10.2 ± 1.2 (s)

12.1 ± 1.1 (s)

50 nm

9.84 ± 0.11

3.66 ± 0.03

10.5 ± 1.5 (s)

12.6 ± 1.1 (s)

60 nm

9.60 ± 0.13

3.55 ± 0.04

10.7 ± 1.5 (s)

12.5 ± 1.2 (s)

80 nm

9.21 ± 0.12

3.40 ± 0.03

10.5 ± 1.4 (s)

12.4 ± 1.2 (s)

120 nm

9.09 ± 0.08

3.39 ± 0.02

10.8 ± 1.7 (s)

12.5 ± 1.4 (s)

160 nm

9.12 ± 0.09

3.37 ± 0.03

10.4 ± 1.6 (s)

12.2 ± 1.2 (s)

Outside

9.85 ± 0.10

3.72 ± 0.03

10.4 ± 1.7 (s)

12.2 ± 1.4 (s)

Table 1.  Calibration of the balloon-borne CCN counter at 1% supersaturation.  The first column gives the calibration aerosol type: laboratory produced aerosol using a solution of 0.1 g/L NaCl in a vaporizer, monodisperse NaCl aerosol of different diameters, or aerosol from the ambient atmosphere outside the laboratory building.  The second column gives the calibration slope using the photodetector voltage peak.  The third column gives the calibration slope using a three-point sum around the photodetector voltage peak (Delene et al., 1998).  The fourth column gives the average time to reach the number peak in seconds since the beginning of the sample.  The last column gives the average time to reach the voltage peak in seconds since the beginning of the sample.  The first 3 rows give the results of the standard calibration of the CCN counter in March, June, and, October 1998.  The CCN counter was removed from the laboratory calibration bench between each standard calibration of the CCN counter and used elsewhere.  The calibrations presented in rows 3-10 were preformed using the same focus and video camera alignment with the CCN counter.


 


Layer

Location

Season

Voltage Peak

Samples

Surface

Laramie, Wyoming

Summer

12.2 ± 1.4 (s)

400

Surface

Fairbanks, Alaska

Winter

12.7 ± 1.8 (s)

144

Lower Troposphere

Laramie, Wyoming

Summer

12.5 ± 1.1 (s)

86

Lower Troposphere

Laramie, Wyoming

Winter

12.3 ± 1.0 (s)

18

Lower Troposphere

Lauder, New Zealand

Summer

12.4 ± 0.7 (s)

23

Upper Troposphere

Laramie, Wyoming

Summer

11.8 ± 1.6 (s)

117

Upper Troposphere

Laramie, Wyoming

Winter

13.1 ± 2.7 (s)

68

Upper Troposphere

Lauder, New Zealand

Summer

12.1 ± 1.3 (s)

67

Table 2.  Time to reach the photodetector volage peak for field measurements in Laramie, Wyoming (41 °N), Lauder, New Zealand (45 °S), and Fairbanks, Alaska (65 °N).  Due to a clear difference in aerosol concentration, the field measurements are divided into summer and winter seasons.  The third column gives the average and standard deviation of the time to reach  the photodetector voltage peak.  The fourth column gives the number of samples used to compute the average.