Atmos. Meas. Tech., 5, 2237–2260, 2012 www.atmos-meas-tech.net/5/2237/2012/ doi:10.5194/amt-5-2237-2012 © Author(s) 2012. CC Attribution 3.0 License. Atmospheric Measurement Techniques Evaluating the capabilities and uncertainties of droplet measurements for the fog droplet spectrometer (FM-100) J. K. Spiegel1, P. Zieger2, N. Bukowiecki2, E. Hammer2, E. Weingartner2, and W. Eugster1 1ETH Zurich, Institute for Agricultural Sciences, Universitätstrasse 2, 8092 Zurich, Switzerland 2Paul Scherrer Institute, Laboratory of Atmospheric Chemistry, 5232 Villigen PSI, Switzerland Correspondence to:W. Eugster (eugsterw@ethz.ch) Received: 30 March 2012 – Published in Atmos. Meas. Tech. Discuss.: 7 May 2012 Revised: 21 August 2012 – Accepted: 24 August 2012 – Published: 20 September 2012 Abstract. Droplet size spectra measurements are crucial to obtain a quantitative microphysical description of clouds and fog. However, cloud droplet size measurements are subject to various uncertainties. This work focuses on the error anal- ysis of two key measurement uncertainties arising during cloud droplet size measurements with a conventional droplet size spectrometer (FM-100): first, we addressed the preci- sion with which droplets can be sized with the FM-100 on the basis of the Mie theory. We deduced error assumptions and proposed a new method on how to correct measured size distributions for these errors by redistributing the measured droplet size distribution using a stochastic approach. Second, based on a literature study, we summarized corrections for particle losses during sampling with the FM-100. We applied both corrections to cloud droplet size spectra measured at the high alpine site Jungfraujoch for a temperature range from 0◦C to 11◦C. We showed that Mie scattering led to spikes in the droplet size distributions using the default sizing pro- cedure, while the new stochastic approach reproduced the ambient size distribution adequately. A detailed analysis of the FM-100 sampling efficiency revealed that particle losses were typically below 10 % for droplet diameters up to 10 µm. For larger droplets, particle losses can increase up to 90 % for the largest droplets of 50 µm at ambient wind speeds below 4.4 m s−1 and even to>90 % for larger angles between the instrument orientation and the wind vector (sampling angle) at higher wind speeds. Comparisons of the FM-100 to other reference instruments revealed that the total liquid water con- tent (LWC) measured by the FM-100 was more sensitive to particle losses than to re-sizing based on Mie scattering, while the total number concentration was only marginally influenced by particle losses. Consequently, for further LWC measurements with the FM-100 we strongly recommend to consider (1) the error arising due to Mie scattering, and (2) the particle losses, especially for larger droplets depending on the set-up and wind conditions. 1 Introduction The cloud droplet size distribution is one of the key param- eter for a quantitative microphysical description of clouds (e.g.Pruppacher and Klett, 1997). It plays an important role for the radiative characteristic of the cloud and is, for ex- ample needed to describe the anthropogenic influence (Gunn and Philips, 1957; Twomey, 1977) and the cloud lifetime ef- fect (Albrecht, 1989; Rosenfeld and Lensky, 1998). More- over, the knowledge of droplet size distribution is crucial for a better understanding of the onset of precipitation (Gunn and Philips, 1957; Stevens and Feingold, 2009) as well as the occult deposition input of clouds to vegetation, which is known to be a relevant component in the hydrological budget of tropical mountain cloud forests (Bruijnzeel et al., 2005; Eugster et al., 2006). At this stage, there are two different approaches of measuring cloud droplet sizes: in-situ mea- surements using optical instruments on aircrafts or ground based stations (e.g.Knollenberg, 1981; Baumgardner, 1983; Baumgardner et al., 2003) and inverse retrieval techniques based on remote sensing measurements from satellites (e.g. Bennartz et al., 2011; Kokhanovsky and Rozanov, 2012). Al- though in-situ measurements have intrinsic difficulties, they are considered to be the best available method for measur- ing cloud droplets (Miles et al., 2000). The basic work- ing principle for the size detection used in these devices is Published by Copernicus Publications on behalf of the European Geosciences Union. 2238 J. K. Spiegel et al.: Evaluating the droplet measurements for FM-100 forward scattering of light, which was first mathematically solved by Gustav Mie (Mie, 1908). The first commercial available optical instrument for in-situ droplet measurements was build in the 1970s (Pinnick and Auvermann, 1979). The instruments have been developed further and their perfor- mance has been strongly improved in terms of precision and automatization since then. Today, a variety of instruments based on forward scattering are in use: the Forward Scat- tering Spectrometer Probe (FSSP; capable of measuring hy- drometeors with diametersD = 2 to 50 µm, e.g.Pinnick and Auvermann, 1979), the Cloud Droplet Probe (CDP; Model CDP-100,D = 2 to 50 µm, e.g.McFarquhar et al., 2007), the Cloud and Aerosol Spectrometer – also with Depolariza- tion CAS-DPOL – (CAS and CAS-DPOL;D = 0.5 to 50 µm, Baumgardner et al., 2011), the Cloud Particle Spectrometer with Depolarization (CPSD;D = 0.5 to 50 µm,Baumgardner et al., 2011), the Small Ice Detectors (SID model 1 and 2; D = 2 to 140 µm,Baumgardner et al., 2011) and the Fog Monitor 100 (FM-100;D = 2 to 50 µm, e.g.Burkard et al., 2002). Using light scattering interferometry, cloud droplets can also be measured in size, for example with the Phase Doppler Interferometer (PIP; 1 to 1000 µm,Baumgardner et al., 2011). However, for realistic operations a reasonable upper-bound was found to beD ≈ 100 µm (Chuang et al., 2008). Furthermore, imaging techniques can be used to cap- ture the cloud’s particle images. Beyond others, a Cloud Par- ticle Imager (CPI; SPEC Inc. Model 230X,Connolly et al., 2007) can be deployed to observe and record real-time CCD images (8-bit, gray-scale 1024× 1024 pixels with a pixel resolution of 2.3 µm) of the ice particles and supercooled droplets withD = 10 to 2300 µm present in the clouds. From these images, the ice crystal number and mass concentration can be determined. The two main groups are passively ven- tilated instruments, which are mainly installed on aircrafts (e.g.Lance et al., 2010) and actively ventilated instruments, which are mainly used for ground based or tower based mea- surements (e.g.Burkard et al., 2002; Eugster et al., 2006). In-situ measurements are very challenging due to various difficulties recently discussed for aircraft devices byLance et al.(2010) andBaumgardner et al.(2011) and for the FSSP in general byBaumgardner(1983) andBaumgardner et al. (1992). In this paper, we will focus on the Fog Monitor 100 (DMT FM-100, Droplet Measurement Technologies, Boulder, CO, USA), which is a ground based instrument with an active ventilation. We will present a detailed error analysis of two topics influencing the droplet measurements of this device: droplet sizing precision and particle losses. The question whether Mie scattering could be responsible for special fea- tures in measured droplet size distribution, for example caus- ing false bimodal size distributions is a common known prob- lem for optical particle counters (e.g.Jaenicke, 1993; Baum- gardner et al., 2010). In a first step, we will therefore evalu- ate how Mie scattering could influence the droplet size spec- tra collected with the FM-100 and propose a new procedure to reprocess already measured data. Second, we will evalu- ate droplet losses during sampling with the FM-100, and in a third step, apply both corrections to cloud droplet spectra collected during the CLACE 2010 (the CLoud and Aerosol Characterization Experiment 2010) campaign, performed at the Jungfraujoch (JFJ) in the Swiss Alps. Based on these campaign data, we will provide recommendations on how to improve the measurement quality in future instrument de- ployments with the FM-100. This is to the best of our knowl- edge the first work not only mentioning the errors but also proposing a suitable correction procedure, which can be ap- plied to the data after sampling. The paper is structured such that we first present the mea- surement site as well as the FM-100 and the instruments used for validation (Sect.2) which is followed by a methodology section (Sect.3), focusing on the proposed sizing and par- ticle loss corrections as well as the implementation of both corrections for the data collected at the JFJ (Sect.4). Finally, we will end with a discussion of the effects of the proposed corrections and provide recommendations how to improve the measurement quality in future instrument set-ups. 2 Instrumentation and site The study to validate and compare the FM-100 with other instruments was performed in the frame of CLACE 2010, which took place at the Jungfraujoch (JFJ, 46◦32′ N, 7◦59′ E) situated in the Bernese Alps at 3580 m a.s.l., Switzerland (Fig.1). Several intensive cloud characterization experiments have been conducted there for many years at different times of the year (e.g.Mertes et al., 2007; Verheggen et al., 2007; Cozic et al., 2008; Targino et al., 2009; Kamphus et al., 2010; Zieger et al., 2012). The aerosol measurements per- formed at the JFJ are part of the Global Atmosphere Watch (GAW) program of the World Meteorological Organization since 1995 (Collaud Coen et al., 2007). Long term studies have been conducted at the site, which indicated that the sta- tion is in clouds approximately 40 % of the time throughout the year (Baltensperger et al., 1998). CLACE 2010 took place in June–August 2010 (temperature range:−11 to 11◦C) and its main aims were to obtain an in-depth chemical, optical and physical characterization of the aerosols at the JFJ as well as to investigate the interaction of aerosol particles with cloud droplets for improving the understanding of the aerosol direct and indirect effects. 2.1 FM-100: fog droplet size spectrometer The commercial FM-100 fog monitor is a forward scatter- ing spectrometer probe placed in a wind tunnel with active ventilation (Eugster et al., 2006). The instrument measures the number size distribution of cloud particles at high time resolution in the size range between 1.5 and 50 µm with a resolution of 10, 20, 30 or 40 channels which can be selected Atmos. Meas. Tech., 5, 2237–2260, 2012 www.atmos-meas-tech.net/5/2237/2012/ J. K. Spiegel et al.: Evaluating the droplet measurements for FM-100 2239 Fog Monitor (FM-100) PVM-100 Aerosol inlets (total & int.) Fig. 1. Position of the Fog monitor (FM-100), Particulate Volume Monitor (PVM-100) and aerosol inlets at the Sphinx platform at the Jungfraujoch (3580 m a.s.l.) during CLACE 2010 (photo courtesy of Boris Schneider,www.metair.ch). by the user. Channel thresholds and diameters are provided by the manufacturer for 10, 20, 30 and 40 channels, but can be defined by the user as well. Simultaneously, the tempera- ture as well as the sampled air volume is measured. A sketch of the working principle of the FM-100 is shown in Fig.2. A pump pulls ambient air through the wind tunnel of the instru- ment. First, the droplets reach the sizing region, where they pass a laser beam (wavelengthλ = 658 nm). The light which is scattered forward within approximately 3◦ to 12◦ from the beam direction is collected and directed to an optical splitter and then to a pair of photodetectors. These collectors trans- late the scattered radiance into a voltage pulse. Under the as- sumption that there are no saturation effects, the pulse height is proportional to the scattered light intensity. For correct siz- ing one needs to assure that the detected particle was inside the depth of field (DOF) of the instrument, which is the uni- form power region of the laser. To qualify a particle for sizing (meaning that the voltage from the sizer is saved for further processing) the two photodetectors are needed. The scattered light is split by the prism, such that one third is directed to the sizer and two thirds to the qualifier. The qualifier only records radiance that passed the optical mask in front of the detector. If the scattering particle was inside the DOF, the scattered signal of the qualifier exceeds the scattering signal of the sizer. For qualified particles the sizer voltage is di- rectly proportional to the scattered radiance into the solid an- gle with an inner opening angle of 3◦ to 4◦ and an outer open- ing angle of around 12.0◦ to 12.6◦ (see Fig.2). The scattered radiance is described by the scattering cross section, which can be calculated using Mie theory (Mie, 1908). The exact values of the scattering angles needed for the Mie calcula- tions differs among instruments. Additionally, they depend on where exactly the particle passes the laser beam (Lance et al., 2010). They need to be derived from glass bead cal- Table 1.Technical specifications of the FM-100 taken fromDroplet Measurement Technologies(2011). Fog Monitor FM-100 Laser wavelengthλ 658 nm Temperature range > 0◦C Sampling frequencya 0.1–10 Hz Inlet diameter (di ) 6.6 cm Contraction part length 16.1 cm Wind tunnel length until laser (Lw) 10.1 cm Wind tunnel diameter (do) 3.8 cm Sampling flow rate (TAS)b around 15 m s−1 Light collection anglesc from 3–4◦ to 12–12.6◦ a Depending on data retrieval software. Technical maximum observed during our field deployment is≈ 12.5 Hz with old instruments and≈ 14.5 Hz with newer ones. b Depending on external pump rate. The sampling flow rate corresponds to the traveling velocity of the droplets. c Light collection angles differ for different instruments. ibrations followed by Mie calculations to find the solid an- gle that fits best to the calibration results (D. Baumgardner, Centro de Ciencias de la Atḿosfera, Universidad Nacional Autónoma de Mexico, Mexico City, Mexico, personal com- munication, 2010). They are therefore one of the sources of uncertainty of the FM-100 that will be addressed in this pa- per. For further details on the electronic part of the FM-100, we refer toDroplet Measurement Technologies(2011). Behind the sizing region there is a pitot tube measuring the air speed in the tunnel. The air speed (which is the traveling velocity of the droplets) is needed in order to determine the sample volume to infer number concentrations and liquid wa- ter content per volume from the measured droplet numbers. Technical specifications are summarized in Table1. A series of parameters can be derived from the mea- sured droplet number size distribution such as total droplet number concentration (NFM), and total liquid water content (LWCFM). In this work we will useNFM (cm−3) which is defined as NFM = imax∑ i=1 ni (1) and the LWCFM (in mg m−3) which is calculated based on the assumption that the droplets are spherical: LWCFM = imax∑ i=1 1 6 π D3 i ni ρH2O, (2) whereimax is the number of channels used,ρH2O is the den- sity of water in kg m−3, Di the geometric mean diameter of each channel in µm, andni the droplet number concentration per channel in cm−3 as derived from the sizer signal. The FM-100 has been used in several ground based stud- ies so far especially as part of an eddy covariance system to quantify fog water deposition fluxes in tropical mountain www.atmos-meas-tech.net/5/2237/2012/ Atmos. Meas. Tech., 5, 2237–2260, 2012 www.metair.ch 2240 J. K. Spiegel et al.: Evaluating the droplet measurements for FM-100 cloud forests (e.g.Eugster et al., 2006; Holwerda et al., 2006; Beiderwieden, 2007; Beiderwieden et al., 2008; Schmid et al., 2010), in temperate ecosystems (Burkard et al., 2002; Thalmann, 2002; Burkard, 2003), and deposition fluxes in rather arid areas (Westbeld et al., 2009). It has also been used as a single instrument for microphysical studies of fog (Gonser et al., 2011; Liu et al., 2011) and compared to other devices (Holwerda et al., 2006; Schmid et al., 2010; Frumau et al., 2011). Most of the presented work used the channel configuration defined by the manufacturer in order to trans- late the voltage to a droplet size; whileNiu et al.(2010) used the 20 channel configuration, which is the one that is used by the manufacturer to calibrate the instrument, some of the authors (Burkard et al., 2002; Eugster et al., 2006; Beider- wieden, 2007; Beiderwieden et al., 2008; Westbeld et al., 2009; Frumau et al., 2011) used the 40 channel configura- tion in order to obtain a better resolved size distribution. A different approach was taken byGonser et al.(2011) – which is one of the most recent publications – who defined their own 23 channel sizes and widths by using Mie curves prior to sampling. Such a procedure has already been suggested earlier for the FSSP (Pinnick et al., 1981; Dye and Baum- gardner, 1984). Nevertheless, this has not been the standard procedure for the FM-100 so far. Here, we will propose a similar procedure that can be applied after sampling. The FM-100 was installed on the NW corner of the upper terrace of the observation platform (Sphinx station, Fig.1) and the inlet was turned into the mean wind direction (323◦) as was expected for June/July conditions based on a dataset from MeteoSwiss from 1990 to 2009. For the second part of the campaign, the device was inclined and a horizontal angle of 293◦ and a vertical angle of−25◦ were chosen in order to account for the pronounced upwind aspiration at this site. 2.2 Instrumentation used for validation of the FM-100 2.2.1 Aerosol inlets For the collection of aerosols an interstitial and a total in- let were installed at a fairly undisturbed place on the roof of the observation laboratory at the Jungfraujoch (Fig.1). The interstitial inlet was installed for collecting particles smaller than 2 µm. It uses an aerodynamic size discriminator with- out heating (Henning et al., 2002). Thus, all non-activated particles pass this inlet. The total inlet samples all particles smaller than 40 µm at wind speeds up to 20 m s−1 (Weingart- ner et al., 1999). Hence, the heated total inlet samples cloud droplets and non-activated (interstitial) aerosols. The con- densed water on the cloud droplets and aerosols is evaporated by heating up the total inlet to +20◦C (Henning et al., 2002). 2.2.2 PVM-100: Particulate Volume Monitor The Particulate Volume Monitor (PVM-100, Gerber Scien- tific Instruments Inc.) is an open path optical instrument that Laser diode Laser power monitorQuali�er Sizer optical mask outer opening angle inner opening angle droplets wind tunnel True Air Speed Fig. 2. Schematic view of the theory of operation of the FM-100 (modified from Droplet Measurement Technologies, 2011). Cloud droplets (blue dots) are pulled through the wind tunnel at constant speed (True Air Speed = TAS) and pass the laser beam. The scat- tered light (red) from the particle is directed through the optical system and then detected by the qualifier and sizer. The inner and outer opening angle depend on the individual instrument and the position where exactly the droplet passed the laser beam. measures the light scattered in the forward direction of all abundant particles in the sample volume. A detailed descrip- tion can be found inGerber(1991) andArends et al.(1994). The PVM-100 was installed on the eastern side of the sphinx roof (Fig. 1). Based a PVM-100 intercomparison during an earlier campaigns, we do not expect any considerable dif- ferences in the LWC measurements due to the different loca- tions at the building. The PVM-100 needs calibration in order to translate the scattering signal into an LWC. The instrument was periodically calibrated with a calibration disk provided by the manufacturer. Particles with a diameter of 3 to 45 µm are taken into account and the calibration is valid for an LWC range from 0.002 to 10 g m−3 and a measurement accuracy of 15 % (Allan et al., 2008). The LWC measured by the PVM is hereafter referred to as LWCPVM. 2.2.3 Dew point hygrometer The PVM-100 as well as the FM-100 both measure the LWC of a cloud using a similar optical method. In order to get another estimate of the LWC that is independent of poten- tial problems associated with light scattering techniques, we computed the condensed water content (CWC) of the cloud with a simple thermodynamic method based on the follow- ing assumptions: First, we assume that the cloud is liquid (no ice crystals). So the CWC is equivalent to the LWC of the cloud. Second, we assume that the water vapor pressure can be described by the ideal gas law, which is fulfilled for atmo- spheric conditions. Third, the cloud is saturated (= relative humidity 100 %). The first criterion is fulfilled in warm fog events, which we select via a temperature threshold of 0◦C for our analysis. By taking the ambient temperature mea- sured by the SwissMetNet station (operated by MeteoSwiss) the corresponding saturation vapor pressure for water can be calculated during cloud events. Using the ideal gas law Atmos. Meas. Tech., 5, 2237–2260, 2012 www.atmos-meas-tech.net/5/2237/2012/ J. K. Spiegel et al.: Evaluating the droplet measurements for FM-100 2241 equation and under the assumption of 100 % RH the water content in the vapor phase can be deduced (VWC). Simulta- neously, we measured the dew point temperature with a high accuracy dew point hygrometer (Dewmaster, Edgetech West Wareham, Massachusetts, USA; precision±0.1◦C) after the ambient air has passed a heated inlet. Thus, the air reaching the dew point hygrometer contains all the water present in the ambient air (i.e. the evaporated droplets and gas phase). Hence, by calculating the equilibrium pressure at the dew point we can deduce the total amount of water (TWC) of the ambient air parcel using the ideal gas law. The CWC of the ambient air parcel is then: CWC = TWC− VWC. 2.2.4 Scanning Mobility Particle Sizer (SMPS) Behind both inlets Scanning Mobility Particle Sizer (SMPS) systems were used to measure the number size distributions of the total and the interstitial aerosol between 17 and 900 nm (dry) diameter (Verheggen et al., 2007). The SMPS system behind the total inlet consisted of a Differential Mobility An- alyzer (DMA, TSI 3071) and a condensation particle counter (CPC, TSI 3022A). The other SMPS system behind the in- terstitial inlet consisted of a DMA (TSI 3071) and a CPC (TSI 3775). During cloud-free conditions the response of the total and interstitial inlets should be identical. The intersti- tial size spectrum was corrected towards the total spectrum by a size-dependent correction factor for the small system- atic difference in concentration between the two inlets (inter- stitial up to 25 % lower than total for particles smaller than 30 nm, concentrations within 5 % for larger particles), as par- ticle losses were expected to be higher in the interstitial in- let, due to a longer residence time in the sampling line. The integration of the respective distribution gives the total num- ber concentration of the total (Ntot) or non-activated aerosols (Nint). The difference (Ntot-int) is the number concentration of the cloud droplets and can be compared to the number con- centration of cloud droplets measured by the FM-100. The methodological accuracy of the SMPS number size distri- butions was± 10 % in concentration for particle diameters larger than 20 nm and± 20 % for smaller particles, respec- tively. Based on the cross-comparison of the two SMPS sys- tems, the precision inNtot-int (=Ncr for number concentration of cloud residuals later on) was estimated to be± 50 cm−3. 2.2.5 Ultrasonic anemometer The wind field around the FM-100 has an important influ- ence on the data quality of the FM-100. Therefore, a HS ul- trasonic anemometer (Gill Ltd., Solent, UK) was installed at 1.7 m away from the FM-100. The ultrasonic anemometer was run together with the FM-100 using an in-house data ac- quisition software (Eugster and Plüss, 2010) recording data at 12.5 Hz. Thus, microphysical processes can be studied at a high temporal resolution. 1 2 3 4 5 6 7 8 910 20 30 40 50 5 10 50 100 500 1000 2000 Droplet Diameter D [µm] Pu ls e A m pl itu de b [m V] D min D geo D dft D max D low b low b up default channels Mie channels Mie curves 10 −8 10 −7 10 −6 Sc at te rin g Cr os s Se ct io n [c m 2 ] 3 4 5 6 7 8 910 140 160 180 200 Fig. 3. Mie curves for a laser wavelength ofλ = 658 nm as well as the default channels from the manufacturer (pink) and the Mie chan- nels (green). The inset shows for channel 5 how the minimum di- ameterDmin and maximum diameterDmax are deduced from the intersections of the Mie curves withblow (Dlow) andbup (Dup). Additionally, the geometric mean diameterDgeo and the diameter of the default channels are depicted (Ddft). 3 Methods: sizing and counting corrections for the FM-100 3.1 Corrections for the size detections of the FM-100 due to Mie theory In order to deduce the size of each droplet from the measured signal, the scattering cross section (see Fig.3; Mie curves are shown in gray) needs to be inverted. As this curve is highly non-monotonic, this is not a trivial task. This is an inherent problem of all types of optical particle counters as seen by many previous studies (e.g.Pinnick et al., 1981; Dye and Baumgardner, 1984; Rosenfeld et al., 2012). The manufac- turer solved this problem as follows: the Mie curves were smoothed (by applying a running average) to an extent that yielded a monotonic function and then attributed four differ- ent channel ranges to it: 10, 20, 30 and 40 (D. Baumgard- ner, personal communication, 2010). So the user can decide whether to use 10, 20, 30 or 40 channels. This procedure does not account for sizing ambiguities, i.e. a particle with a diameter of around 3 µm has a similar scattering cross sec- tion as a particle with a diameter of around 8 µm. With this default configuration, the signal of both the 3 and the 8 µm particle are interpreted as a particle of 5 µm. In Fig.3, the pink boxes show the 40 channels that have been deduced in the described way for the used FM-100. The default chan- nels varied between 0.19 µm (first channel) and 2.13 µm in channel width with a mean value of 1.21 µm (see Table2 for more details). We will refer to these channels later on using the termdefault channels(with geometric mean diameters Ddft), and the LWC derived from this configuration we will be referred to as LWCdft. www.atmos-meas-tech.net/5/2237/2012/ Atmos. Meas. Tech., 5, 2237–2260, 2012 2242 J. K. Spiegel et al.: Evaluating the droplet measurements for FM-100 Table 2. Channel range of the default (ranging fromDdft,min to Ddft,max with a geometric mean diameterDdft) and the new Mie channels (ranging fromDmin to Dmax with a geometric mean di- ameterDgeo). Values are given in units of µm. Default channels Mie channels Ddft,min Ddft,max Ddft Dmin Dmax Dgeo 1 1.50 1.69 1.59 1 2.50 1.54 2 1.69 1.97 1.82 1.28 2.72 1.90 3 1.97 4.10 2.84 2.74 4.70 3.79 4 4.10 6.10 5.00 3.00 7.48 4.11 5 6.10 8.11 7.03 3.32 9.84 6.27 6 8.11 9.30 8.68 5.08 10 7.36 7 9.30 10.42 9.84 5.50 11.60 9.19 8 10.42 11.54 10.97 7.50 11.78 10.59 9 11.54 12.24 11.88 10.36 13.38 11.11 10 12.24 12.90 12.57 11.82 13.68 12.86 11 12.90 13.54 13.22 12 13.74 12.64 12 13.54 15.07 14.28 12.20 15.96 14.43 13 15.07 16.29 15.67 13.96 18.60 15.06 14 16.29 17.58 16.92 14.26 20.32 16.69 15 17.58 18.94 18.25 15.98 20.66 17.80 16 18.94 20.29 19.60 16.16 20.84 18.88 17 20.29 21.46 20.87 17.98 22.64 20.45 18 21.46 22.66 22.05 20.04 24.16 21.81 19 22.66 24.02 23.33 21.64 25.76 23.59 20 24.02 25.16 24.58 23.16 27.32 24.40 21 25.16 26.35 25.75 24.74 28.86 25.87 22 26.35 27.45 26.89 24.92 29.40 26.77 23 27.45 28.62 28.03 26.82 31.34 28.18 24 28.62 29.75 29.18 27.02 31.62 29.24 25 29.75 30.71 30.23 28.88 32.88 30.30 26 30.71 31.98 31.34 29.00 33.40 31.44 27 31.98 33.18 32.57 29.30 34.66 32.51 28 33.18 34.38 33.77 32.10 36.38 34.16 29 34.38 35.60 34.98 33.28 38.10 35.26 30 35.60 36.79 36.19 34.86 39.98 36.83 31 36.79 38.02 37.40 36.06 40.38 37.78 32 38.02 39.24 38.63 37.66 41.94 39.00 33 39.24 40.53 39.88 37.84 42.32 40.16 34 40.53 41.83 41.17 39.74 43.14 41.25 35 41.83 43.23 42.52 40.12 45.10 43.01 36 43.23 44.59 43.90 41.86 47.22 43.74 37 44.59 45.98 45.28 42.22 47.56 45.35 38 45.98 47.16 46.57 43.78 49.12 46.13 39 47.16 48.57 47.86 45.70 49.34 47.53 40 48.57 50.00 49.28 46.92 49.98 48.58 Throughout this text we will use the following terms: each channel is defined by a lower and an upper margin for the pulse amplitude, which we will later on refer toblow and bup (see Fig.3 for details).bup− blow will be referred to as “channel height”, i.e. with the term “channel width”, we refer to the droplet diameter range that is covered by this channel. In the next section, we suggest two approaches on how to take the Mie curve variations for sizing into account: one by using channels that are wide enough to cover the Mie variations (Sect.3.1.1) and another to obtain a new size dis- tribution by redistributing the measured counts per channel (Sect.3.1.2). 3.1.1 Widening of the size bins of the FM-100 and error calculations Redefining channel limits as well a combining channels to remove the ambiguity in sizing has been suggested for dif- ferent optical particle counters by previous studies (e.g.Pin- nick et al., 1981; Dye and Baumgardner, 1984). However, to the extend of our knowledge, none of them proposes over- lapping channels (as presented in this section) or the use of a stochastic approach (next section) in order to retrieve the droplet size distribution from the measured signal. The procedure to derive new channels is as follows: in a first step we made Mie calculations for the optical system using an algorithm further developed fromMätzler (2002) which in turn is based on the work byBohren and Huffman (1983). The derivation of the scattering cross section as well as detailed calculations can be found in the corresponding literature (e.g.,Mie, 1908; Van de Hulst, 1981; Bohren and Huffman, 1983; Liou, 2002). The inner and outer angles of the scattering cone (see Fig.2) were not clearly determined during manufacturing of the FM-100 (= instrumentation un- certainty) and hence needed to be estimated via glass bead calibrations. Additionally, these angles also depend on where exactly the droplet passes the laser beam (= spatial uncer- tainty). We therefore did several Mie calculations starting with a cone with an inner opening angle of 3◦ and an outer opening angle of 12◦. By increasing the angles stepwise by 0.1◦ to 4◦ for the inner angle and 12.6◦ for the outer angle, we obtained a set of Mie curves that represents the scatter- ing cross sections of the droplets including instrumental and spatial uncertainty (see Fig.3; the maximum and minimum of this Mie curve set are shown in dark gray). We then trans- lated this Mie band into a voltage as it is done in the FM-100 electronics by assuming a linear relationship between scat- tered light intensity and voltage signal and setting the scat- tering cross section of a 50 µm particle equal to 4096 mV (D. Baumgardner, personal communication, 2010). In a sec- ond step, we used the Mie band to reassign new droplet di- ameters to each of the channels. In the following we will use the values for channel 5 for illustration (inset Fig.3). As the FM-100 only determines whether a particle was detected in a certain channel while the exact light scattering signal is not recorded, we had to keep the channel boundariesblow (149 mV) andbup (192 mV) as they were configured dur- ing the measurements. Hence, for each channel we searched the lowest droplet diameter that still yielded a voltage signal within the height of the respective channel.blow intersects the Mie band at different diametersDlow (= 3.32 to 3.66 µm and 4.86 to 5.22 µm and 6.48 to 7.50 µm, see inset Fig.3 for details). The minimum of the set ofDlow is the minimum di- ameter of this channel (Dmin = min{Dlow} = 3.32 µm). Sim- ilarly, the maximum diameterDmax corresponding to this Atmos. Meas. Tech., 5, 2237–2260, 2012 www.atmos-meas-tech.net/5/2237/2012/ J. K. Spiegel et al.: Evaluating the droplet measurements for FM-100 2243 2.74 3.5 4.7 1 D [µm] P D F N 3 [− ] d) 60 80 b [m V ] Channel 3: 1.96 µm a) 3 4 5 6 7.48 0.3 0.6 D [µm] P D F N 4 [− ] e) 100 120 140 b [m V ] Channel 4: 4.48 µm b) 3.32 6 8 9.84 0.1 0.3 D [µm] P D F N 5 [− ] f) 160 180 b [m V ] Channel 5: 6.52 µm c) 3 4 5 0 5 10 Channels n [c m − 3 C ha nn el − 1 ] g) 2 4 6 8 10 0 5 10 h) D [µm] n* [c m − 3 µ m − 1 ] 2 4 6 8 10 0 5 10 i) D [µm] n [c m − 3 µ m − 1 ] n PDF,1µm n* Fig. 4. (a) to (c) Pulse amplitudeb versus diameter (shown in the range ofDmin to Dmax andblow andbup) for the channels 3, 4, and 5. (d) to (f) Normalized probability density function PDFNi for the same channels as in(a) to (c). (h) Discrete droplet size distributionn∗ with a resolution of 0.02 µm if the PDFN approach is used with the PDFNi functions from(d) to (f) and the number size distribution from(g). (i) Discrete droplet size distributionn∗ – gray area, same as in(h) – and the re-binned size distributionnPDF,1µm with the bin size of 1D = 1 µm (red bars). channel was derived by taking the maximum of the set of Dup (Dmax= max { Dup } = 9.84 µm). From the geometric mean (Dgeo= 6.27 µm) of the minimum and the maximum, we then obtained the new droplet diameter to be assigned to this channel. We then repeated this procedure for all other channels. By doing this we obtained three monotonic curves that can be easily inverted and used to evaluate the signal: the geometric mean curve, as a mean estimate for the size distribution, the minimum and the maximum as a lower and upper estimate for the size distribution, respectively. In that way the channels (later on referred to as Mie channels) be- came wider and therefore overlap, with channel width vary- ing from 1.44 µm to 6.52 µm with a mean channel width of 4.21 µm (see Table2 for more details). However, the differ- ences of the geometric means (Ddft, black bar in the pink boxes for the default channels, andDgeogreen crosses for the Mie channels in Fig.3) between the two configurations was always smaller than 1.32 µm (see Table2). Out of the maxi- mum 40 channels, 21 channels were smaller with the default channel configuration than the Mie channel configuration and 19 channels were wider. This way of translating the voltage signal has the advan- tage that it also provides the uncertainty of the droplet sizes associated with the Mie scattering, but at the expense of clear channel separation. The LWC derived using the mean chan- nels will hereafter be referred to as LWCgeo, the one us- ing the maximum curve as LWCmax and the one using the minimum curve as LWCmin. 3.1.2 Retrieving a new droplet size distribution using probability density functions With the method above it is possible to retrieve an appro- priate maximal error assumption for the LWC. However, the FM-100 was mainly designed for measuring droplet size dis- tributions. The question arises on how to retrieve a size dis- tribution for channels which overlap. In this section we there- fore present a new method on how size distributions that account for Mie scattering can be deduced from measured distributions. We consider this new approach to be the best way of dealing with the Mie uncertainties with respect to overlapping channels. Due to the channel overlap an adequate size distribution could be achieved by redistributing the number counts per channel over an adequate channel width. For this purpose we had a closer look at the channels, which were defined in the previous section. The procedure will be explained in the fol- lowing using channel 5 as an example (Fig.4c and f). Chan- nel 5 ranged fromDmin = 3.32 µm toDmax= 9.84 µm (see Fig. 3 inset). The Mie band of channel 5 was not uniformly distributed along the channel width (Fig.4c), e.g. droplets between 3.64 µm and 4.86 µm as well as between 8.04 µm www.atmos-meas-tech.net/5/2237/2012/ Atmos. Meas. Tech., 5, 2237–2260, 2012 2244 J. K. Spiegel et al.: Evaluating the droplet measurements for FM-100 and 9.12 µm did not produce a scattering signal that fell into this channel height. On the other hand, droplets be- tween 6.76 µm and 7.48 µm covered the entire channel height with their scattering signal. So if a scattering signal between 149 and 192 mV is detected, it is more likely that it came from a droplet that has a size between 6.76 µm and 7.48 µm than 3.64 µm and 4.86 µm. To account for this, we calcu- lated a probability density function based on the Mie band that represents the contribution of each droplet size to the scattering signal within the channel. It includes the assump- tion that each scattering cross section within the Mie band is equally probable, which we consider to be a reasonable first approximation. For the redistribution, the measured number concentration was multiplied with the normalized probabil- ity density function leading to a stochastic assumption of the droplets that could have produced the according scattering signal. The procedure was as follows: First, discrete proba- bility density functions (PDFi(D)) for each channel (i) were deduced from the Mie band. Each channel was divided in 1DR = 0.02 µm intervals fromDmin to Dmax. For each diam- eterD, the percentage of the Mie band relative to the pulse amplitude height (bup− blow) of the channel was calculated: PDFi(D) with D ∈ [Dmin(i), Dmax(i)] . (3) This resulted in a curve fromDmin to Dmax, which was 1 if the pulse covered the entire channel height. Second, this discrete probability density function was normalized (Fig.4c to f) such that 1DR × Dmax∑ D=Dmin PDFNi(D) = 1; (4) PDFNi(D) = PDFi(D) 1DR × Dmax∑ D=Dmin PDFi(D) with D ∈ [Dmin(i), Dmax(i)] . (5) Third, the amount of droplets measured per channelNi was redistributed fromDmin to Dmax based on the normalized probability density function. This was done for every chan- nel leading to a discrete droplet number distributionn∗ with a resolution of1DR = 0.02 µm: n∗(D) = imax∑ i=1 Ni × PDFNi(D). (6) In order to account for uncertainties (such as the equally probable Mie band or slightly different opening angles), a new droplet size distribution based on bins with the same size 1D should be retrieved (nPDF,aµm refers to channels with bin size1D =a µm). The liquid water content based on this method will be referred to as LWCPDF,aµm. This procedure was applied to one minute mean values of the collected cloud droplet spectra from CLACE 2010. 3.2 Particle losses While measuring droplets, one is facing the problem that cloud droplets are rather heavy and therefore are influenced by their inertia and gravity. Hence, depending on their size and volume, they do not necessarily follow exactly the same trajectories as gas molecules would. This means that there is a potential for particle losses during sampling from am- bient air (sampling efficiency,ηsmp(D)) and during trans- port through the system (transport efficiency,ηtsp(D)). One way of assessing this issue is to simulate particle transport through a system using computational fluid dynamics (CFD). Another approach is to use experimentally and theoretically derived formulas for different loss mechanisms within the different tube sections in order to calculate the overall effi- ciency. As CFD calculations are very time-consuming, we will therefore use the second approach for particle losses in the FM-100 as a first estimate. In general, the efficiencyη is the fraction of the num- ber concentration of droplets downstream of the loss mech- anism and the droplet number concentration upstream. The fraction of particle losses is then 1− η. The product of the sampling and the transport efficiency is the inlet efficiency ηtot, which describes the performance of the sampling device (von der Weiden et al., 2009). Sometimes the efficiencies are named differently, (e.g. inBrockmann, 2011). Nevertheless, throughout this text we will adhere to terms used byvon der Weiden et al.(2009): ηtot(D) = ηsmp(D) × ηtsp(D). (7) In general, different particle loss mechanisms contribute to the losses in the two parts of the measurement system. An overview of the different mechanisms was given, e.g. by von der Weiden et al.(2009). Here, we will only discuss the mechanisms which are relevant for the FM-100 (see Fig.5 for illustration): aspiration lossesηasp, transmission losses ηtrm, sedimentation lossesηgrav inside the FM-100, losses due to eddy formationηturb inside the FM-100, and inertial losses in the contractionηcont. In the following we shortly introduce sampling and transport losses and refer to the AppendixA for a detailed presentation of the used formulas. 3.2.1 Sampling losses During ideal sampling conditions, the sampling is isoaxial and isokinetic (Brockmann, 2011). Isoaxial means that the sampling inlet has no inclination with respect to the sur- rounding wind direction. The term isokinetic sampling in- dicates that the sampling speed (U ) is equal to the surround- ing wind speed (U0). If the sampling speed is smaller than the ambient wind speed, the term sub-kinetic sampling is used, while forU >U0 the term super-kinetic sampling is used. It will be used in the following for the turbulent as well as for the laminar regime as it has been done by oth- ers before (von der Weiden et al., 2009; Brockmann, 2011). Atmos. Meas. Tech., 5, 2237–2260, 2012 www.atmos-meas-tech.net/5/2237/2012/ J. K. Spiegel et al.: Evaluating the droplet measurements for FM-100 2245 pitot tube TAS f) g)d) c)e) vena contracta vena contracta b) sub iso-kinetic a) non iso-axial super iso-kinetic a) a) trajectory of a gas molecule trajectory of a droplet d) Turbulent deposi- tion in contraction a) Aspiration c) Inertial losses in contraction e) Sedimentation in contraction f ) Sedimentation g) Turbulent deposition b) Transmission E� ci en ci es φ θs θcont di do Lw contraction part wind tunnel transport tubing laser plane U0 U θ TAS: true air speed as measured by the pitot tube U: inlet velocity U0: ambient wind speed θ: angle of inclination corres- ponding to the horizontal θcont: contraction half angle θs: sampling angle φ: zenith angle di: inlet diameter do: wind tunnel diameter Lw: length of the wind tunnel until the laser plane Fig. 5. Illustration of the different particle loss mechanisms –(a) to (g) – as described in Sect.3.2 for the FM-100 (the small photograph shows the FM-100 at Jungfraujoch). Values for the FM-100 geometry are given in Table1. Detailed description of the formulas of the particle loss mechanisms are given in Appendix A. Both regimes need to be taken into account when setting up an inlet system and where and how to position the instru- ment (Brockmann, 2011). One way of addressing the isoax- ial sampling is to put the instrument onto a turntable and let- ting it continually turn into the main wind direction as done by Vong (1995), Kowalski et al.(1997), Kowalski (1999), Wrzesinsky(2000), Burkard et al.(2002), Thalmann(2002), Burkard (2003), Eugster et al.(2006), andHolwerda et al. (2006). Nevertheless, these procedures do not assure isoki- netic sampling conditions. Westbeld et al.(2009) andLiu et al. (2011) also installed the FM-100 in a fixed position for the entire measurement campaign. They established a quality criterion, by only ac- cepting data as good data if the horizontal wind direction does not differ by a certain degree from the actual inlet orien- tation.Westbeld et al.(2009) used± 30◦ of the hourly mean wind direction andLiu et al. (2011) used± 7◦ for this cri- terion. However, a clear justification why they chose these angles was not given. Instead of excluding any data immedi- ately, we suggest to calculate the sampling efficiency for the FM-100 in order to estimate the losses and correct for those. The sampling efficiencyηsmp is defined as the fraction of par- ticles of interest (for the FM-100: the droplets), which reach the sampling probe from the surrounding air and successfully penetrate into the transport tubing. In general, the sampling efficiency itself consists of two different contributions: ηsmp(D) = ηasp(D) × ηtrm(D). (8) The aspiration efficiencyηasp is the ratio of the number con- centration of particles that enter the sampling probe cross section to the number concentration of particles in the am- bient air (von der Weiden et al., 2009; Brockmann, 2011). For the FM-100 we calculate the aspiration efficiency for the three different velocity regimes: (1) calm air (sur- rounding wind velocityU0 < 0.5 m s−1), (2) slow moving air (0.5 m s−1 ≤ U0 ≤ 2.18 m s−1, which corresponds to a veloc- ity ratio Rv =U0/U of up to 0.5; with inlet velocityU ), and (3) moving air (velocity ratioRv = 0.5 to 2) and different an- gle regimes. Details on the used formulas are given in the AppendixA1. The transmission efficiency (ηtrm) is the ratio of parti- cle concentration exiting the inlet to the particle concen- tration just past the inlet face (formulas are given in the AppendixA2). 3.2.2 Transport lossesηtsp(D) In contrast to the sampling losses, the transport losses do not depend on the flow conditions outside the sampling device. The transport losses are described by the transport efficiency of the tubing system which is the ratio of the number concen- tration of particles leaving the tubing system divided by the www.atmos-meas-tech.net/5/2237/2012/ Atmos. Meas. Tech., 5, 2237–2260, 2012 2246 J. K. Spiegel et al.: Evaluating the droplet measurements for FM-100 particles entering the tubing system. As different loss mech- anisms happen in the transport system, the overall transport efficiency of a tubing system is the product of the all particle loss mechanisms for all tubing sections (Brockmann, 2011): ηtsp(D) = ∏ sec [∏ mech ηsec,mech(D) ] , (9) whereηsec,mechare the different loss mechanisms per section. In the FM-100 there is a two-part tubing section: the contrac- tion zone of 16 cm length and the wind tunnel with constant diameter with a length of 10 cm (see Fig.5). For both parts we calculated transport losses due to sedimentationηgrav and turbulent inertial depositionηturb as well as inertial losses in the contraction partηcont. Detailed formulas are given in the AppendixA3. 3.2.3 Application of the corrections for particle losses to the FM-100 The described efficiencies were calculated numerically from the minimal diameter to the maximal diameter in 0.1 µm steps for each channel. Then we took the mean value of all these efficiencies and attributed them to each channel such that we get one efficiency for each channel. For the default channel configuration as well as for the channels based on the density distribution method, we did the efficiency calculation for each channel separately, using the according geometric mean values. For Stokes numbers smaller than the validity range of the correcting formulas (aspiration, transmission and inertial de- position efficiency in the contraction), we applied the pro- posed formulas as they yielded efficiencies close to 1. This would be an appropriate description as we assume that the particles are small enough to follow the same trajectory as gas molecules. The used formulas are valid for constant gas velocities (Brockmann, 2011). To conform with these assumptions as closely as possible, we calculated the efficiencies for 1-min intervals, with approximately constant wind velocity. As we basically only have anisoaxial sampling, we only used for- mulas for the anisoaxial regime. Unfortunately, the proposed equation for the calm flow regime (Eq.A4) is not valid for the second part of the CLACE 2010 period, when the FM-100 was installed with its inlet facing downwards (zenith angleφ = 115◦). Though, Grinshpun et al.(1993) only excluded angles larger than 90◦ because it was not common to use an inlet facing down- wards. However,Vts U cosφ correctly describes the sedimen- tation even if the zenith angle is larger than 90◦. We there- fore apply this formula also for the time the FM-100 faced downwards. With the same argumentation, we extend the for- mula for sedimentation losses for the downward sampling (Eq.A13). If ηtot could not be calculated for all droplet sizes (e.g. due to too high Stokes numbers), we excluded this size distribution from further analysis as it could not be corrected. 4 Results and discussion 4.1 The effect of the Mie correction to the channel widths of the FM-100 It is remarkable that the Mie channels were rather wide and overlapped especially in the range where we expect most of the droplets (3 to 20 µm; seeBruijnzeel et al., 2005). But, the default procedure of deducing the channel thresholds (as it is done by the manufacturer) did not result in substantially different mean points, indicating that the LWCgeo would not differ a lot from LWCdft. However, a proper error estimation of the LWCFM for the sizing uncertainty arising due to the non-monotonic Mie scattering curve can be deduced from the Mie channels. Consequently, our suggestion is to use the Mie channel approach if one is interested in the LWC including maximal error assumptions and not only in theN . The effect of the Mie channel configuration on two typical droplet size distributions for maritime and continental low stratus clouds described by a log normal distribution (nlog) is shown in Fig.6a and c. We used nlog(D) = Nt,log √ 2 π σlogD exp { − [ ln ( D/Dn,log )]2 2 σ 2 log } , (10) with Nt,log = 288 cm−3, σlog = 0.38 and Dn,log = 7.7 µm for continental and Nt,log = 74 cm−3, σlog = 0.38 and Dn,log = 13.1 µm for maritime droplet size distributions (according toMiles et al., 2000). For this purpose we modeled the sampling behavior of the FM-100 by first translating the droplet size (D) into a scatter- ing signal using the Mie band. If the Mie band of (D) fell into more than one channel,nlog(D) was distributed proportional to the coverage of the Mie band in comparison to the channel height over the involved channels. The received distribution was what the FM-100 would measure and was then trans- lated into a droplet size distribution by attributing the default diameter (Ddft) or the Mie diameter (Dgeo) to the channel. The droplet size distribution for the default channels (ndft) was shifted towards larger droplets for the continental size distribution (Fig.6a) while for the maritime distribution the shape was in rather good agreement except for some spikes between 10 and 15 µm which are similar to those that have been recently discussed as an artifact from Mie scattering (Baumgardner et al., 2010). This simulation supports the as- sumption that spikes like these are indeed an artifact resulting from Mie scattering. The distribution based on the Mie chan- nels (ngeo) is plotted with horizontal error bars indicating the width of the new channels (Fig.6a and c). As these channels were wider than the default ones, the droplet size distribution was flatter. However, it is obvious that this is not an appropri- ate approach if one is interested in droplet size distributions as the Mie channels overlap. For this aim it is more useful to use the method presented in Sect.3.1.2, which is shown in Fig. 6b and d. The Mie oscillations were still obvious in Atmos. Meas. Tech., 5, 2237–2260, 2012 www.atmos-meas-tech.net/5/2237/2012/ J. K. Spiegel et al.: Evaluating the droplet measurements for FM-100 2247 0 10 20 0 20 40 60 a) n [c m − 3 µ m − 1 ] 0 10 20 0 20 40 60 b) n [c m − 3 µ m − 1 ] Droplet Diameter D [µm] 0 10 20 30 0 5 10 c) 0 10 20 30 0 5 10 d) Droplet Diameter D [µm] n log (D) n dft (D) n geo (D) n*(D) n PDF,1 µm (D) n PDF,2 µm (D) n PDF,4 µm (D) n PDF,8 µm (D) Continental Maritime Fig. 6. Modeled sampling behavior of the FM-100 as described in Sect.4.3.1for an assumed typical continental (left panels) and maritime (right panels) cloud droplet size distributionnlog(D) (gray dashed lines).(a) and (c) Size distribution measured with default channels (ndft(D), magenta line) and the Mie channels (ngeo(D), green line) including maximal and minimal errors for each channel (see Sect.3.1.1). (b) and (d) Effect of the re-sizing on the apparent size distribution: the discrete droplet number distributionn∗(D) with a resolution of 0.02 µm (gray area) and four different re-binned size distributionsnPDF,aµm with bin size1D =a µm (a = 1, 2, 4 and 8, see Sect.3.1.2for details). n∗(D) (droplet number concentration with a resolution of 0.02 µm, Eq.6) and nPDF,1µm (nPDF,aµm refers to channels with bin size1D =a µm). However, the original curvenlog was adequately represented, if a bin size of 2 µm (nPDF,2µm) was used for the re-binning. For larger bin sizes used for the re-binning – 4 µm (nPDF,4µm) and 8 µm (nPDF,8µm) – the shape of nlog could no longer be adequately represented. Based on this theoretical exercise, we conclude that us- ing the probability density function method with a bin size of 2 µm is the best compromise if one is interested in droplet size distributions. The effect of this new approach on the measured LWCFM will be presented and discussed in Sect.4.3. 4.2 Particle loss mechanisms in the FM-100 Figure7 shows the efficiencies for the different particle loss mechanisms calculated for the FM-100 under standard at- mospheric conditions (T = 0◦C, P = 1013 hPa) for horizon- tal sampling using the formulas introduced in Appendix A. The ηasp and ηtrm were close to one for droplets smaller than≈ 20 µm independent of the wind speed regime. In the calm air regime (Fig.7c; U0 < 0.5 m s−1), ηasp was inde- pendent of wind speed (U0) and sampling angleθs. How- ever,ηasp,calmdecreased below 0.5 for droplets larger than 38 µm. In both, the moving air regime (Fig.7a) and the slow moving air regime (Fig.7b) ηasp decreased with in- creasingθs and increasing droplet diameter. Additionally, the transition from Eqs. (A1) to (A3) was obvious at 60◦ sampling angle. This step showed a rather unphysical be- havior from Rv = 0.11 to 0.8 as particles of the same size with sampling angles larger than 60◦ would reach the inlet with a higher probability than those with angles below 60◦. Both equations were deduced from experiments at discrete sampling angles (θs = 0◦, 30◦, 45◦, 60◦ and 90◦). Addition- ally, Eq. (A3) was originally only suggested for sub-kinetical sampling (1.25≤ Rv ≤ 6.25; 0.003≤ Stk≤ 0.2, Hangal and Willeke, 1990a) while Eq. (A1) fitted the measured data with 0.25≤ Rv ≤ 2; 0.01≤ Stk≤ 6 (Durham and Lundgren, 1980; Hangal and Willeke, 1990a) except forθs = 90◦. However, Eq. (A3) has been used recently for a much widerRv range (von der Weiden et al., 2009; Brockmann, 2011). Neverthe- less, we are interested in a reasonable physical description for the loss corrections for the FM-100 and we therefore de- cided to use Eq. (A1) for 0≤ θs< 90◦ as an additional option for particle loss corrections as this could also be deduced as the valid range based on the comparison to measurements (Durham and Lundgren, 1980; Hangal and Willeke, 1990a). By doing so, we also avoid thatηaspcould not be calculated due to Stokes limitations as Eq. (A1) has a broader validity range than Eq. (A3). For the ηtrm one panel for super-kinetical sampling (Fig. 7d) and one for sub-kinetical sampling (Fig.7e) is shown as those two regimes differ in terms of loss mech- anisms due to the formation of the vena contracta in the super-kinetical regime. In the sub-kinetical regime,ηtrm de- creased quickly for droplets larger than around 10 µm and angles larger than 30◦. For largerRv this transition de- creased to smaller sampling angles and smaller droplet di- ameters. In the super-kinetical regime (Rv < 1), the forma- tion of the vena contracta decreasedηtrm for smaller an- gles in a way thatηtrm was nearly independent of the sam- pling angle. In recent publications (von der Weiden et al., 2009; Brockmann, 2011), Eq. (A9) was stated to only be www.atmos-meas-tech.net/5/2237/2012/ Atmos. Meas. Tech., 5, 2237–2260, 2012 2248 J. K. Spiegel et al.: Evaluating the droplet measurements for FM-100 Droplet diameter D [ µm] θ s [° ] a) Rv=1.2 0 30 60 Droplet diameter D [ µm] θ s [° ] b) Rv=0.4 0 30 60 Droplet diameter D [µm] θ s [° ] c) Rv=0.1 10 20 30 40 50 0 30 60 Droplet diameter D [ µm] θ s [° ] d) Rv=1.2 0 30 60 Droplet diameter D [µm] θ s [° ] e) Rv=0.4 10 20 30 40 50 0 30 60 E�ciency [−] 0 0.5 1 R v U 0 [m s −1] Aspiration E�ciency Transmission E�ciency 4 2 1 0.5 0.25 0.1 17.5 8.7 4.4 2.2 1.1 0.5 Droplet diameter D [µm] E� ci en cy [− ] g) 10 20 30 40 50 0.6 0.7 0.8 0.9 1 η trp f)E� ci en cy [− ] 0.65 0.7 0.75 0.8 0.85 0.9 0.95 1 Transport E�ciency η cont η grav,cont η turb,cont η grav η turb Fig. 7. Efficiencies for the different particle loss mechanisms for the FM-100 calculated under standard atmospheric conditions (p = 1013 mbar,T = 0◦C) using the equations presented in Appendix A for sampling anglesθs∈ [0◦, 90◦]. For gray colors the efficiency is 1, decreasing from 0.99 (red) to 0 (blue), shaded area indicates efficiency>1.05. White indicates that the efficiencies could not be calcu- lated, as the input variables were not inside the range of validity. For each velocity range ofηasp, one representative panel (values in brackets) is shown:(a) moving air (U0 = 5.24 m s−1 which corresponds to a velocity ratioRv =U0/U=1.2),(b) slow moving air (U0 = 1.7 m s−1 which is equal toRv = 0.4) and(c) calm air (U0 = 0.43 m s−1 which corresponds to a velocity ratioRv of 0.1). Forηtrm one panel for sub-kinetical sampling(d) and one for super-kinetical sampling(e) is shown. The positioning of the panels(a) to (e) versus theRv-axis on the left rep- resents the range of the different velocity ranges forηaspandηtrm. The different mechanisms contributing (ηcont, ηgrav,cont, ηturb,cont, ηgrav andηturb) to transport efficiencyηtsp are shown individually in(f) and cumulative in(g). valid for Rv >0.25 (corresponding toU0 = 1.1 m s−1), al- though there were no such limitations in the original pub- lication (Hangal and Willeke, 1990b). As wind speeds are often very low in fogs (especially in radiation fogs;Fuzzi et al., 1985) this would mean that particle losses could not be calculated for this range and could not be used for fur- ther analysis. There are, however, two options available as an approximation to solve this issue: (1) we setηtrm = 1 for Rv < 0.25 and consider the calculatedηtot as an upper limit, or (2) we use Eq. (A9) also forRv < 0.25. A careful analysis of Eq. (A9) for Rv < 0.25 for the FM-100 revealed thatηtrm got closer to one for decreasingRv and that therefore pos- sibility (2) should be considered the more appropriate one. Nevertheless, we included both versions ofηtrm for our anal- ysis of the CLACE 2010 data and will refer to the two options with TR1 to case (1) and TR to case (2). The dominating contribution to theηtsp wasηcont, while ηgrav andηturb for the contraction part as well as for the wind tunnel did not decrease below 0.95 (Fig.7f). However, the product of all five loss mechanismsηtsp, already decreased below 0.9 for droplets around 14 µm, emphasizing that parti- cle losses within the FM-100 should not be neglected even if the FM-100 is placed on a turning table. The resultingηtot with the implementation ofηtrm for the whole super-kinetical regime andηasp(0–90◦) =ηasp(0–60◦) (later on referred to as ASP09TR) for the three differentRv regimes treated above are shown in Fig.8a to c. Indepen- dent of the wind regime,ηtot > 0.9 for droplets smaller than 10 µm. Interestingly, for droplets larger than 10 µmηtot de- creased fastest with droplet size for the slow moving regime. So the common idea that sampling in calm air does not need any corrections for particle losses might be correct for aerosols, but for droplets, corrections appear to be essential. In the moving air regimeηtot decreased with sampling angle. While for the slow motion regime the sampling angle played a minor role in comparison to the droplet size, in the moving regime,ηtot rapidly decreased with increasing sampling an- gle. The counter-intuitive fact, thatηtot for Rv > 1 was higher Atmos. Meas. Tech., 5, 2237–2260, 2012 www.atmos-meas-tech.net/5/2237/2012/ J. K. Spiegel et al.: Evaluating the droplet measurements for FM-100 2249 a) θ s [° ] 0 30 60 90 b) θ s [° ] 0 30 60 Droplet diameter D [µm] c) θ s [° ] 10 20 30 40 50 0 30 60 Inlet E�ciency [−] 0 0.5 1 R v U 0 [m s −1]R v U 0 [m s −1] 1.2 0.4 0.09 d) θ s [° ] 0 30 60 90 g) 0 30 60 90 j) 0 30 60 90 e) θ s [° ] 0 30 60 h) 0 30 60 k) 0 30 60 Droplet diameter D [µm] f) θ s [° ] 10 20 30 40 50 0 30 60 Droplet diameter D [µm] i) 10 20 30 40 50 0 30 60 Droplet diameter D [µm] l) 10 20 30 40 50 0 30 60 Contribution to total losses [%] 0 10 20 30 40 50 60 70 80 90 100 L tsp L trm L asp Fig. 8. (a)to (c)Total inlet efficiencies as a function of sampling angleθs versus droplet diameterD for three different representative velocities (Rv = 1.2, 0.4 and 0.09) of each velocity range. The individual percentaged contributions of aspiration losses(d) to (f), transmission losses(g) to (i) and transport losses(j) to (l) are shown as percentaged values (see black and white color bar). for larger droplets for sampling angles below≈ 30◦ than for Rv < 1, could be explained in the way thatηasp increases above 1 in the sub-kinetical regime, which increasedηtot. Nevertheless,ηtot was never above one for the regime we correct. The contributions of the different loss mechanisms to the overall losses (Lasp= 1−ηasp 1−ηtot , Ltrm = 1−ηtrm 1−ηtot , andLtsp= 1−ηtsp 1−ηtot ; Fig. 8d to l) depend onRv, sampling angle and droplet diam- eter. ForRv > 1 and sampling angles below≈ 30◦, the losses were dominated by particle losses within the FM-100 asLtrp was 1 (Fig.8j to l). For Rv > 1 and sampling angles above 30◦ and droplet diameters> 20 µm losses were dominated by transmission lossesLtrm, with a small contribution of as- piration lossesLasp. In the slow moving regime, the contri- butions of the different mechanisms were comparable. How- ever, in the calm regime for droplets& 15 µm, most losses happen due to aspiration. To summarize, based on the theoretical framework of the description of particle loss mechanisms, it is important to consider particle losses when it comes to droplet size mea- surements with the FM-100. Losses of 40 % for droplets ≈ 20 µm should be expected for calm air (U0 < 0.5 m s−1). The losses decrease with increasing wind speeds for sam- pling angles. 30◦ and increase for sampling angles& 30◦. In the sub-kinetical regime, the sampling angle is the criti- cal parameter when it comes to particle losses. We therefore assume that it is more appropriate to evaluate the quality of the collected data with the presented approach, then to di- rectly exclude data collected under larger sampling angles as we could show that even droplets collected at small sampling angles can be subject to major particle losses due to losses in the FM-100 as well as due to non-isokinetical sampling. In the next section these loss calculations will be used to correct measured data from the CLACE 2010 campaign. We evaluated the particle losses for the four different categories summarized in Table3. 4.3 Implementation of the Mie corrections and the particle losses for the CLACE 2010 campaign The effect of the different corrections for particle losses and re-sizing as discussed in the previous sections on the CLACE 2010 data will be described in this section. In order to evaluate our procedure of error attribution due to Mie scattering as well as due to particle losses, we ap- ply our corrections to measured cloud droplet spectra from CLACE 2010. In contrast toLance et al.(2010, who only used data with LWC> 100 mg m−3), we decided to choose a rather weak cloud criterion. The presence of a cloud was www.atmos-meas-tech.net/5/2237/2012/ Atmos. Meas. Tech., 5, 2237–2260, 2012 2250 J. K. Spiegel et al.: Evaluating the droplet measurements for FM-100 Table 3.Description of the different particle loss categories applied to the CLACE 2010 data. Abbreviation Description STANDARD ηtot based on the equations from Appendix A TR1 similar as STANDARD except (Rv < 0.25) = 1 TR similar as STANDARD except (Rv < 0.25) continued ASP09TR similar as STANDARD except (Rv < 0.25) continued andηasp(0–90◦) =ηasp(0–60◦) 0 500 1000 0 500 1000 1500 m= 1.85 t= 16.36 R2 = 0.42 LW C P V M [m g m − 3 ] LWC dft [mg m−3] a) 0 200 400 0 100 200 300 400 500 m= 1.31 t= −96.27 R2 = 0.32 N cr [c m − 3 ] N FM [cm−3] b) 0 30 60 90 120 150 180 0 1 2 3 4 5 F re qu en cy [% ] θ s [°] c) 0 2 4 6 8 0 1 2 3 4 5 6 F re qu en cy [% ] Wind U 0 [m s−1] d) Fig. 9. Overview of the measured data during CLACE 2010.(a) Liquid water content measured by the PVM-100 (LWCPVM) versus the FM-100 measurements using the default channel configuration (LWCdft); (b) number concentrations of cloud residuals (Ncr) versus cloud droplet number concentration measured by the FM-100 (NFM). The solid red line in(a) and (b) represents a geometric mean regression with m: slope,t : intercept andR2: squared correlation coefficient.(c) Frequency of observed sampling angleθs; (d) frequency of observed horizontal wind speedU0. Both parameters were determined by ultrasonic measurements. The solid red line represents the median, while the dashed lines show the 25th and 75th percentile, respectively. defined if the one minute mean values fulfilled the following criterion: LWCPVM > 5 mg m−3 and NFM > 10 cm−3. We are aware of the risk of including very thin and hence inho- mogeneous clouds by using this criterion, which might cause problems for comparing the LWC results especially at low values. We also tried to use a stricter cloud criterion in terms of higher thresholds, but found a strong selection bias in such comparisons and hence decided to keep the threshold as low as possible. Due to the mounting position of the FM-100, the inlet often was completely closed by frozen cloud droplets as the cold and humid updraft blew into the inlet of the FM-100. We therefore excluded periods with temperatures below 0◦C from data evaluation in order to exclude potential measure- ment artifacts that might arise due to freezing. The cloud criterion was fulfilled for 106 h of the CLACE 2010 campaign (data collection period 56 days). During 71 h of the cloudy period (which was 66 % of the cloud time), the FM-100 was positioned horizontally. An overview of the LWC and theN during cloud sampling as well as the wind conditions around the FM-100 inlet are shown in Fig.9. We chose geometric mean regressions as a tool to compare the LWC andN as we assume that all meth- ods used to deduce LWC andN were error-prone. Based on the geometric mean regression, the FM-100 measured a smaller LWC than the PVM-100 (Fig.9a). A compari- son of the LWCPVM with the CWC (R2 = 0.59, with slope m = 0.93 and interceptt = 0 not shown) revealed a good agreement between the two alternative approaches to mea- sure the LWC. Hence, the PVM-100 can be considered an Atmos. Meas. Tech., 5, 2237–2260, 2012 www.atmos-meas-tech.net/5/2237/2012/ J. K. Spiegel et al.: Evaluating the droplet measurements for FM-100 2251 0 500 1000 1500 0 500 1000 1500 LW C PV M [m g m −3 ] LWC min [mg m −3] m = 2.62 t = 63.57 R 2 = 0.40 a) 0 500 1000 1500 0 500 1000 1500 LWC geo [mg m −3] m = 1.92 t = 31.65 R 2 = 0.41 b) 0 500 1000 1500 0 500 1000 1500 LW C PV M [m g m −3 ] LWC max [mg m −3] m = 1.32 t = −8.40 R 2 = 0.43 c) 0 500 1000 1500 0 500 1000 1500 LWC PDF,2 µ m [mg m −3] m = 1.86 t = 17.21 R 2 = 0.41 d) calm regime slow motion regime (θ s >60°) other data Fig. 10. Effect of the Mie corrections on the LWC during CLACE 2010 (blue circle:U0 < 0.5 m s−1; green crosses: 0.5< Rv < 0.8 and θs> 60◦; gray dots: rest of the data fulfilling the cloud criterion).(a) to (c) LWC measured by the PVM-100 (LWCPVM) versus LWC deduced from the FM-100 measurements using the channel widening method (Sect. 3.1.1).(d) LWCPVM versus LWC deduced from the FM-100 measurements using the stochastic approach (Sect.3.1.2). The solid red line represents a geometric mean regression to the entire data withm: slope,t : intercept andR2: squared correlation coefficient. appropriate reference to validate our corrections for the FM- 100 measurements. The sampling angle of the FM-100 was large during most of the time, such that only 4 % of the cloudy data were within the sampling angle criteria (below 30◦) used byWestbeld et al.(2009). This is remarkable, as the inlet faced the expected mean wind direction during the first part of the campaign. Nevertheless, the median horizon- tal sampling angle during the first part was 38◦, indicating that the mean wind direction as measured by MeteoSwiss was not representative for the wind field at the FM-100 mounting position. The high vertical sampling angle (median 42◦ relative to the FM-100), which resulted from strong up- drafts, contributed additionally leading to the high sampling angles (Fig.9d). Based on the sampling angles and the anal- ysis presented in Sect.4.2, we expect that significant parti- cle losses during sampling could explain the difference be- tween LWCFM and LWCPVM, although the wind speed was not too high (Fig.9d). However, from the comparison ofNcr to NFM, we would not necessarily expect large particle losses (see Fig.9b). Therefore, we will first present the effect of re- sizing in order to investigate whether improper sizing could explain the lower LWCFM before continuing with the effect of particle losses. 4.3.1 Corrections for droplet sizing and its effect on LWC FM The difference betweenDgeoandDdft was minor (Sect.4.1), so the regression lines for LWCgeo and LWCdft were simi- lar (Figs.9a and10b). However, the spread of the LWCFM based onDgeo was large if we consider LWCmin (Fig. 10a) as a minimal estimate and LWCmax as an upper estimate (Fig. 10c) of the LWCFM. Nevertheless, the linear regres- sion line of LWCPVM versus LWCmax was still clearly differ- ent from unity, meaning that even within the range of max- imal error assumption (LWCFM ∈ [LWCmin, LWCmax]), the difference between LWCPVM and LWCFM could not be ex- plained by incorrect sizing. A similar conclusion can be drawn from the comparison of the LWC based on probability density functions with dif- ferent bin sizes for re-binning: the slope and intercept were in the same range as for LWCdft and LWCgeo; the same was true for the squared Pearson correlation coefficientR2 (see Table4). The LWCFM was still in the appropriate range, if www.atmos-meas-tech.net/5/2237/2012/ Atmos. Meas. Tech., 5, 2237–2260, 2012 2252 J. K. Spiegel et al.: Evaluating the droplet measurements for FM-100 Table 4.Slope, intercept andR2 for geometric mean regressions between LWCPVM and LWCgeoas well as LWCPDF,aµm for non-corrected data as well as for the different correction categories presented in Table3. Brackets indicate whether all cloud data from CLACE 2010 (all) or only data during horizontal sampling (hori) or downward sampling (down) were used. LWCgeo LWCPDF,1µm LWCPDF,2µm LWCPDF,4µm LWCPDF,8µm slope intercept slope intercept slope intercept slope intercept slope intercept non-corrected (all) 1.92 31.65 1.84 21.09 1.86 17.21 1.86 18.82 1.95 24.81 R2 = 0.41 R2 = 0.42 R2 = 0.41 R2 = 0.41 R2 = 0.40 non-corrected (hori) 1.99 5.7 1.91 −4.89 1.93 −9.99 1.94 −8.45 2.06 −4.72 R2 = 0.47 R2 = 0.47 R2 = 0.46 R2 = 0.46 R2 = 0.45 non-corrected (down) 1.76 84.81 1.69 74.61 1.69 72.74 1.70 74.43 1.73 83.35 STANDARD (all) 1.29 −19.23 1.2 −21.86 1.24 −30.09 1.24 −32.56 1.25 −29.24 R2 = 0.49 R2 = 0.42 R2 = 0.45 R2 = 0.62 R2 = 0.59 STANDARD (hori) 1.37 −35.12 1.28 −38.76 1.32 −48 1.28 −45.6 1.3 −42.99 R2 = 0.56 R2 = 0.48 R2 = 0.51 R2 = 0.67 R2 = 0.65 STANDARD (down) 0.91 56.99 0.89 51.28 0.89 50.46 0.89 49.8 0.88 54.09 R2 = 0.23 R2 = 0.24 R2 = 0.24 R2 = 0.25 R2 = 0.22 TR1 (all) 1.32 50.97 1.27 43.27 1.28 39.07 1.22 41.47 1.24 46.37 R2 = 0.30 R2 = 0.26 R2 = 0.28 R2 = 0.42 R2 = 0.39 TR (all) 1.29 50.75 1.24 43.35 1.25 38.91 1.21 40.11 1.22 44.93 R2 = 0.29 R2 = 0.25 R2 = 0.27 R2 = 0.42 R2 = 0.39 ASP09TR (all) 1.18 54.94 1.14 45.33 1.15 41.90 1.14 44.53 1.12 52.23 R2 = 0.39 R2 = 0.39 R2 = 0.39 R2 = 0.39 R2 = 0.36 ASP09TR (hori) 1.17 31.63 1.13 22.18 1.15 17.95 1.13 21.14 1.10 29.30 R2 = 0.49 R2 = 0.49 R2 = 0.48 R2 = 0.49 R2 = 0.46 ASP09TR (down) 1.17 107.27 1.14 97.62 1.13 96.13 1.13 97.24 1.14 103.34 R2 = 0.21 R2 = 0.23 R2 = 0.23 R2 = 0.23 R2 = 0.21 the bin width> 2 µm was used, although the size distribution was no longer appropriately represented (Sect.4.1). So, in- dependent of how we derived the droplet size distributions from our measured signal, the LWCFM did not rise to a level suggested by LWCPVM. Interestingly, the correlation between LWCFM and LWCPVM is higher for horizontal sampling in comparison to the downward sampling period (see Table4). As the sam- pled cloud time for horizontal sampling was nearly twice as long as for downward sampling, we do not consider this as an error that can be related to counting statistics. We rather take this as an additional indicator of particle losses for downward sampling conditions as the gravitational losses are supposed to be higher. After particle loss corrections this difference should vanish. Consequently, for the CLACE 2010 data, par- ticle losses during sampling could be considered as the main reason for the under-sampling of the FM-100, although this was not expected based on droplet number concentrations. As a general conclusion, the influence of the presented sizing correction methods is negligible, if the LWC is the only quantity of interest. However, if an error estimation of LWCFM is an object of the study, then LWCgeowith the max- imal error assumption by LWCFM ∈ [LWCmin, LWCmax] should be used; if one is interested in size distributions, LWCPDF,2µm should be used. 4.3.2 Changes of LWCFM due to particle loss corrections Table4 summarizes the results of the different particle loss corrections. For the STANDARD correction the correlation slightly increased as a result of the decreasing fraction of cloud data that could be corrected (around 42 % of cloud data). Reasons why the correction could not be applied were either that the sampling angle> 90◦ (11 % of the cloud data), Rv was smaller than 0.25 (42 % of cloud data) or droplets with Stokes numbers larger than the Stokes limitations were abundant (5 % of the cloud data). For horizontal sampling the numbers were similar, while for downward sampling only around 20 % of the cloud data could be corrected as most of the data fell into theRv < 0.25 regime. However, the corrections for the remaining downward sampling data were such that LWCgeo as well as LWCPDF,aµm were similar to LWCPVM. Although this is a promising result, it needs to be treated with care, as first, the correlation was small (R2 ≈ 0.2), second, the LWC was always below 700 mg m−3 and third, the counting statistics was small. Besides the fact that we could only correct around 40 % of the CLACE 2010 data with this correction, the agreement between LWCgeo and LWCPVM as well as between LWCPDF,aµm and LWCPVM improved, but still differed from one. Atmos. Meas. Tech., 5, 2237–2260, 2012 www.atmos-meas-tech.net/5/2237/2012/ J. K. Spiegel et al.: Evaluating the droplet measurements for FM-100 2253 0 500 1000 1500 0 500 1000 1500 LW C PV M [m g m −3 ] LWC e� min [mg m −3] m = 1.66 t = 82.19 R 2 = 0.27 a) 0 500 1000 1500 0 500 1000 1500 LWC e� geo [mg m −3] m = 1.29 t = 50.75 R 2 = 0.29 b) 0 500 1000 1500 0 500 1000 1500 LW C PV M [m g m −3 ] LWC e� max [mg m −3] m = 0.94 t = 10.28 R 2 = 0.31 c) 0 500 1000 1500 0 500 1000 1500 LWC e� PDF,2 µ m [mg m −3] m = 1.25 t = 38.91 R 2 = 0.27 d) calm regime slow motion regime (θ s >60°) other data Fig. 11. Effect of particle losses (using TR corrections – see Table3 – for all data) on the LWC for LWCmin, LWCgeo, LWCmax and LWCPDF,2µm for CLACE 2010 (blue circle:U0 < 0.5 m s−1; green crosses: 0.5< Rv < 0.8 andθs> 60◦; gray dots: rest of the data fulfilling the cloud criterion). The solid red line represents a geometric mean regression withm: slope,t : intercept andR2: squared correlation coefficient. By replacingηtrm (Rv < 0.25) = 1 (TR1 in Table4) or con- tinuingηtrm for Rv < 0.25 (TR in Table4, as well as Fig.11) a correction for nearly 85 % of the collected data was possi- ble. Both approaches TR and TR1 did remarkably decrease the slope, however, they also decreasedR2. As the slopes for TR were steeper than for TR1, we would suggest to use TR for the transmission regime. Moreover, this would also avoid any sharp steps forηtrm when decreasingRv below 0.25. However, data with 0.5> Rv > 0.8 andθs> 60◦ (green crosses in Fig.11, which was the regime whereηasp shows an unphysical behavior) still had a higher slope (m = 1.55 for LWCgeo andm = 1.52 for LWCPDF,2µm, not shown). Apply- ing the ASP09TR correction moved those points closer to the one to one line and changed the slopes to around 1.1 for LWCgeo as well as LWCPDF,aµm, andR2 were compa- rable to the uncorrected data. For the horizontal sampling, slopes and intercepts were similar while theR2 was even around 0.5. For the downward sampling, slopes were similar but intercepts were higher andR2 lower, which would mean that the applied corrections did not have the same effect as for horizontal sampling. We could think of different explanations for that: first, as the correlation for downward sampling was already worse for uncorrected sampling and still persisted the corrections for particle losses; it could be that the FM-100 was more protected by the building due to its tilting and therefore the cloud sampling was less representative than for the first pe- riod. Second, for the same reason, it could be that the wind field as measured by the ultrasonic anemometer was less rep- resentative for the wind field around the FM-100 inlet. Con- sequently, the corrections would not be as successful for the downward sampling as for the horizontal sampling. There- fore, it is difficult to evaluate whether the corrections for particle losses were appropriate for the downward sampling or whether the data themselves were worse for the down- ward sampling. Further studies with the PVM-100, the FM- 100 and the ultrasonic anemometer mounted in close vicinity would be needed to further evaluate the performance of the particle loss corrections. Although the effect of the particle losses on the LWC were considerable, the corrections did not change the rela- tion betweenNcr andNeff FM (total droplet number concentra- tion deduced from the FM-100 withDgeo and corrections for particle loss) in a way that it was measurable by means of geometric mean regressions orR2 (see Fig.12). Larger droplets were mainly affected by particle loss calculations, www.atmos-meas-tech.net/5/2237/2012/ Atmos. Meas. Tech., 5, 2237–2260, 2012 2254 J. K. Spiegel et al.: Evaluating the droplet measurements for FM-100 0 100 200 300 400 500 600 0 100 200 300 400 500 600 m = 1.32 t = −101.87 R2 = 0.30 N FM eff [cm−3] N cr [c m − 3 ] Fig. 12. Number concentrations of cloud residuals (Ncr) deduced from two SMPS systems and corrected for particle losses as de- scribed in Sect.2.2.4 versus cloud droplet number concentra- tion measured by the FM-100 corrected for particle losses using ASP09TR – see Table3 – for all data (Neff FM). as they were too heavy to follow the gas stream lines. Obvi- ously, these particles play a minor role forNFM, which would mean that the ambient amount of larger droplets during CLACE 2010 was small. Nevertheless, these larger droplets determine the LWC, which is why the LWCFM was very sen- sitive to particle loss corrections. To summarize, if the FM- 100 is used to study LWC rather thanN , we strongly recom- mend making particle loss calculations. 4.4 Recommendation for future deployments of the FM-100 Based on the analysis presented here we have the following recommendations for future installations of the FM-100: 1. A careful analysis of the sampling system revealed that there is a considerable error in the LWCFM arising from the measurement principle. A possibility of reducing the errors from Mie scattering is to choose the 40 thresh- olds in such a way that they correspond better to the Mie curve, similar to what was done byGonser et al. (2011). This is already a common procedure for other optical particle counters (e.g.Pinnick et al., 1981; Dye and Baumgardner, 1984) but has only been used by Gonser et al.(2011) when measuring with the FM-100. Additionally, the signal should be redistributed using probability density functions as proposed here. How- ever, one needs to know the instrumental response of the FM-100 in detail as they differ between the individ- ual instruments (e.g. range of detected scattering angles or laser wavelength). We therefore recommend to use a Mie band deduced from a set of scattering angles rather than a single Mie curve. Moreover, this needs to be done before the installation of the FM-100, as the channel thresholds can no longer be changed afterwards. 2. Additionally, not all droplets of the ambient air reach the sampling device due to aspiration and transmission losses. Moreover, a considerable amount of particles gets lost within the instrument before reaching the sam- pling region. While isoaxial sampling can be more or less achieved by mounting the FM-100 on a turnable platform, isokinetical sampling cannot be achieved with a pump running at constant speed. We therefore rec- ommend doing loss calculations for the droplet mea- surements even if the instrument can be turned into the wind direction. In order to perform such calculations, use of an ultrasonic anemometer close by the FM-100 is crucial as well as a reference for the LWC such as a PVM-100. 5 Conclusions In this work, the accuracy of the commercially available fog monitor FM-100 was investigated by focusing on the effect of Mie scattering on droplet sizing and on particle losses occurring during the operation. The conclusions based on the analysis of both uncertainties individually as well as the CLACE 2010 data set are the following: 1. Concerning the sizing procedure, the default (manufac- turer’s) channel selection is sufficient for the determina- tion of the total droplet number concentration (NFM) or the total liquid water content (LWCFM). For a maximal error estimate of the LWC, the choice would be LWCgeo as an appropriate estimate of the LWC and LWCmin and LWCmax as the maximal error assumption. Moreover, we showed that a redistribution of the measured scatter- ing signal using a stochastic approach (based on proba- bility density functions) leads to a more appropriate re- production of the ambient droplet size distributions than conventional methods. 2. Depending on sampling angles and wind speeds, parti- cle losses due to sampling losses and losses within the FM-100 can be as high as 100 %. Consequently, particle loss corrections (in the ASP09TR version, see Table3 for details) for the FM-100 are needed if the focus of the study is the LWCFM or fluxes calculated based on the LWCFM. Future studies should also explore whether a passive open- path droplet size spectrometer, e.g. as used on aircrafts, would yield better results even at the low wind speeds typ- ically found near the ground surface under foggy conditions. Atmos. Meas. Tech., 5, 2237–2260, 2012 www.atmos-meas-tech.net/5/2237/2012/ J. K. Spiegel et al.: Evaluating the droplet measurements for FM-100 2255 Appendix A Formulas used for particle losses A1 Aspiration efficiency For the moving air regime, we use the formulas which were based on a literature survey and experiments done byHangal and Willeke(1990a,b). For a sampling angleθs between 0◦ and 60◦ (60◦ included) they deduced: ηasp,move(D) = 1 + [( U0 U ) cos θs − 1 ] f, (A1) where f = 1 − [ 1 + ( 2 + 0.617 U U0 ) Stk′ ]−1 1 − [ 1 + 2.617Stk′ ]−1 × { 1 − [ 1 + 0.55Stk′ exp ( 0.25Stk′ )]−1 } . (A2) With Stk the Stokes number of the sampling in- let (see Brockmann, 2011, for detailed information) and Stk′ = Stkexp (0.022θs). This equation is valid for 0.01≤ Stk≤ 6 and 0.5≤ Rv ≤ 2. For sampling angles from 61◦ to 90◦, Hangal and Willeke (1990a) suggested (based on measurements with 90◦ sam- pling angle): ηasp,move(D) = 1 + (Rv cos θs − 1) ( 3 Stk √ Rv ) , (A3) for 0.003≤ Stk≤ 0.2 and Rv ≥ 1.25. However, in more recent publications the validity range was extended to 0.02≤ Stk≤ 0.2 and 0.5≤ Rv ≤ 2 (von der Weiden et al., 2009; Brockmann, 2011). For the calm air regime, we decided to use the empirical equation deduced byGrinshpun et al.(1993) based on sev- eral experiments, as the one bySu and Vincent(2004, 2005) is only applicable for aspiration efficiencies larger than 0.75 and the alternative one byDunnett and Wen(2002) was nu- merically deduced for larger particle diameters (40 µm to 110 µm): ηasp,calm(D) = Vts U cosφ + exp ( 4 Stk1+ √ Vts/U 1 + 2 Stk ) , (A4) where Vts is the terminal settling velocity (seeBrock- mann, 2011 for detailed information), andφ is the zenith angle of the inlet (φ = 90◦ for horizontal sam- pling). The first term describes gravitational settling of particles dependent on the inlet orientation and the sec- ond term addresses inertial and gravitational losses in- dependent of inlet orientation. This equation is valid for 10−3 ≤ Vts/U ≤ 1 and 0.001≤ Stk≤ 100 for angles 0◦ ≤ φ ≤ 90◦. For Vts/U < 10−3 we setηasp(D) = 0 in the calm air regime as we then assume that the particles are small enough that they can follow the stream lines. In the literature the slow moving air regime is not clearly defined (von der Weiden et al., 2009). So we choose the boundaries such that they fill the gap between calm air and slow mov- ing air (0.5 m s−1 ≤ U0 andRv ≤ 0.5). The formulas used are based on the work byGrinshpun et al.(1993, 1994): ηasp(D) = ηasp,move(D) (1 + δ)0.5 fmove + ηasp,calm(D) fcalm, (A5) fmove = exp ( − Vts U0 ) , (A6) fcalm = 1 − exp ( − Vts U0 ) , (A7) δ = Vts U0 [ Vts U0 + 2 cos (θs + φ) ] , (A8) for 10−3 ≤ Vts/U ≤ 1 and 10−3 ≤ Stk≤ 100, 10−3 ≤ Rv ≤ 10 with zenith angle 0◦ ≤ φ ≤ 90◦. A2 Transmission efficiency Hangal and Willeke(1990b) proposed that the transmission efficiency consist of an inertial and a gravitational part. How- ever, von der Weiden et al.(2009) suggest that the grav- itational effect is better described as part of the transport efficiency. Hence, we only take into account the inertial effect with the following formula in the validity range of 0.02≤ Stk≤ 4, 0.25≤ Rv ≤ 4, and 0◦ ≤ θs≤ 90◦: ηtrm(D) = exp [ −75 (Iv + Iw)2 ] , (A9) whereIv are the losses in the vena contracta. The vena con- tracta only forms when the sampling conditions are super- isokinetic: Iv = 0.09 ( Stk U − U0 U0 cos θs )0.3 , (A10) for 0.25≤ Rv ≤ 1 otherwiseIv = 0. Iw are the losses from di- rect impaction to the wall: Iw = Stk √ Rv sin (θs + α) sin ( θs + α 2 ) , (A11) for 0.02≤ Stk≤ 4, and 0.25≤ Rv ≤ 4, where α = 12 [( 1 − θs 90◦ ) − exp (−θs) ] . (A12) A3 Transport losses The FM-100 consists of a two-part tubing system: a contrac- tion zone and a wind tunnel with constant diameter (Fig.5). For the second part with constant diameter there are two contributions to the loss mechanisms: www.atmos-meas-tech.net/5/2237/2012/ Atmos. Meas. Tech., 5, 2237–2260, 2012 2256 J. K. Spiegel et al.: Evaluating the droplet measurements for FM-100 – Sedimentationηgrav Particles deposit due to gravitational forces on the lower wall of the FM-100 wind tunnel. There are different cor- rection formulas available, depending on the flow con- ditions and the tube orientation. As the flow in the wind tunnel of the FM-100 is turbulent (Reynolds number, Re≈ 23 000 for CLACE 2010,Re≈ 21 000 at sea level pressure and 25◦C), we use the formulas presented by Schwendiman et al.(1975): ηgrav(D) = exp ( − 4 Vts Lw cos θ TAS do π ) , (A13) whereLw is the length of the wind tunnel (till the laser region),do is the diameter of the wind tunnel, True Air Speed TAS = 13.15 m s−1, which is the mean value of the flow velocity in the wind tunnel measured by the pitot tube, andθ angle of inlet inclination (= 0◦ for hor- izontal flow). This equation is valid forVts sin θ TAS � 1. – Turbulent inertial depositionηturb Depending on the size of the particle there are two dif- ferent regimes of how particles are “thrown” to the tube wall by eddies: the turbulent diffusion-eddy impaction and the particle inertia-moderated regime (Brockmann, 2011). For the first one, particle deposition increases with particle size as their inertia gets larger. For the second regime, the particles are so large, that their tra- jectory does no longer perfectly follow that of a gas molecule that does not suffer from inertial effects, so particle losses increase slightly with size. There are dif- ferent corrections suggested in the literature. Here, we use a correction based onLiu and Agarwal(1974) who introduced the dimensionless turbulent velocityV+ and the dimensionless particle relaxation timeτ+ in order to describe the transition between the two regimes: ηturb(D) = exp ( − 4 Vt Lw TAS do π ) , (A14) whereVt is the deposition velocity for turbulent inertial deposition, with τ+ = 0.0395Stk Re1/8, (A15) Vt = V+ TAS 5.03Re1/8 . (A16) For the moderate particle inertia regime (τ+ ≥ 12.9), we use a constantV+ = 0.1, and for the turbulent diffusion eddy (τ+ ≤ 12.9) the turbulent velocity is estimated as V+ = 0.0006τ2 +. For the contraction part, there is only one formula available: Inertial loss in a contractionηcont In the contraction part droplets are accelerated due to the decreasing diameter of the transport tubing. Larger parti- cles could eventually not follow the changes in the trajec- tories resulting in wall impaction due to inertia.Muyshondt et al.(1996) experimentally derived a formula for the inertial losses in the contraction part of a transport tubing: ηcont(D) = 1 − 1 1 + 2 [ Stk ( 1 − Ao Ai ) 3.14 exp (−0.0185θcont) ]1.24 , (A17) whereAo is the cross sectional area of the wind tunnel,Ai cross sectional area of the inlet, andθcont is the contraction half angle of the contraction part. The formula is valid for 0.001≤ Stk(1− Ao/Ai) ≤ 100, and 12◦ ≤ θcont≤ 90◦. Un- fortunately, theθcont of the contraction part of the FM-100 is only 6◦. As the losses get smaller with smallerθcont within the validity range, we still use this formula in order to get an upper estimate for the losses, and hence we expect the true losses to be a bit smaller than this estimate. The contraction part is longer than the second part with constant diameter. We therefore assume that we cannot ig- nore the inertial losses due to turbulence (ηturb,cont) as well as the gravitational losses (ηgrav,cont). We therefore determine those efficiencies iteratively using the Eqs. (A13)–(A16). Appendix B List of symobls B1 Latin symbols Ai Cross sectional area of the inlet Ao Cross sectional area of the wind tunnel blow Lower margin for the pulse amplitude of a channel bup Upper margin for the pulse amplitude of a channel CWC Condensed Water Content D Droplet diameter Di Geometric mean diameter of channeli Dlow Diameter for which Mie band =blow Dn,log Median diameter of the log normal droplet size distribution Dup Diameter for which Mie band =bup di Inlet diameter do Diameter of the wind tunnel Atmos. Meas. Tech., 5, 2237–2260, 2012 www.atmos-meas-tech.net/5/2237/2012/ J. K. Spiegel et al.: Evaluating the droplet measurements for FM-100 2257 LWC Liquid Water Content (see Sect.B3 for subscripts used and Sect.B4 for superscripts used) LWCFM Liquid Water Content measured by FM-100 LWCPVM Liquid Water Content measured by PVM-100 Iv Particle losses in the vena contracta Iw Particle losses from direct impaction to the wall imax Number of channels used for droplet sizing with the FM-100 Lk Contributions of the loss mechanismk to the overall losses (k = asp, trm, tsp) Lw Length of the wind tunnel N Droplet number concentration (Sect.B4 for superscripts used) NFM Total droplet number concentration measured by FM-100 Ncr Number concentration of cloud residuals (Ntot-int) Nint Non-activated aerosol number concentration measured with the SMPS at the interstitial inlet Ntot Aerosol number concentration measured with the SMPS at the total aerosol inlet Nt,log Total droplet number concentration of the log normal droplet size distribution n Droplet size distribution (see Sect.B3 for subscripts) n∗(D) Discrete droplet number distribution with bin width1D = 0.02 µm nlog(D) Log normal size distribution ni Droplet number concentration per channel measured by FM-100 PDFi(D) Discrete probability density function of channeli PDFNi(D) Normalized discrete probability density function of channeli Re Reynolds number RH Relative humidity Rv Velocity ratio Stk Stokes number TAS True Air Speed measured by the pitot tube TWC Total Cloud Water U Sampling speed (=velocity at the inlet) U0 Surrounding wind speed VWC Water Content of the Vapor phase Vts Terminal settling velocity Vt Deposition velocity for turbulent inertial deposition V + Dimensionless deposition velocity B2 Greek symbols 1D Bin size used for the stochastic approach 1DR Resolution used for redistributing the channels in the stochastic approach φ Zenith angle of the inlet (instrument positioning) ρH2O Density of water ηasp Aspiration efficiency (ηasp,calmfor the calm regime andηasp,movefor the moving air regime) ηcont Efficiency describing inertial losses in a contraction ηgrav Efficiency describing losses through sedimentation ηgrav,cont Efficiency describing gravitational losses in a contraction ηsmp Sampling efficiency ηtot Inlet efficiency ηtrm Transmission efficiency ηtsp Transport efficiency ηturb Efficiency describing losses through turbulent inertial deposition ηturb,cont Efficiency describing inertial losses due to turbulences in a contraction λ Laser wavelength θ Angle of inlet inclination (instrument positioning) θcont Contraction half angle θs Sampling angle σlog Logarithmic width of the log normal droplet size distribution τ+ Dimensionless particle relaxation time B3 Subscripts used forD, n and LWC dft Used for values deduced from the geometric mean diameter of the default channels geo Used for values deduced from the geometric mean diameter of the Mie channels max Used for values deduced from the maximum diameter of the Mie channels min Used for values deduced from the minimum diameter of the Mie channels PDF,a µm Used for values deduced from the stochastic approach with bin size1D = a µm B4 Superscripts used forN and LWC eff corrected for particle losses www.atmos-meas-tech.net/5/2237/2012/ Atmos. Meas. Tech., 5, 2237–2260, 2012 2258 J. K. Spiegel et al.: Evaluating the droplet measurements for FM-100 Acknowledgements.We thank the International Foundation High Altitude Research Stations Jungfraujoch and Gornergrat (HFSJG) for the opportunity to perform experiments on the Jungfraujoch. This work was supported by MeteoSwiss within the Global Atmosphere Watch programme of the World Meteorological Organization. We would like to thank Swiss Meteorological In- stitute (MeteoSwiss) for providing meteorological measurements, Berko Sierau and Ulrike Lohmann (IAC-ETHZ) for loaning us their FM-100, Darrel Baumgardner for fruitful discussions on Mie scattering, Bernd Pinzer for interesting discussions on probability density functions and Nina Buchmann for comments on this manuscript. Edited by: S. Malinowski References Albrecht, B. A.: Aerosols, Cloud Microphysics, and Fractional Cloudiness, Science, 245, 1227–1230, 1989. Allan, J. D., Baumgardner, D., Raga, G. B., Mayol-Bracero, O. L., Morales-Garćıa, F., Garćıa-Garćıa, F., Montero-Mart́ınez, G., Borrmann, S., Schneider, J., Mertes, S., Walter, S., Gysel, M., Dusek, U., Frank, G. P., and Krämer, M.: Clouds and aerosols in Puerto Rico – a new evaluation, Atmos. Chem. Phys., 8, 1293– 1309,doi:10.5194/acp-8-1293-2008, 2008. Arends, B. G., Kos, G. P. A., Maser, R., Schell, D., Wobrock, W., Winkler, P., Ogren, J. A., Noone, K. J., Hallberg, A., Svennings- son, I. B., Wiedensohler, A., Hansson, H. C., Berner, A., Solly, I., and Kruisz, C.: Microphysics of clouds at Kleiner Feldberg, J. Atmos. Chem., 19, 59–85,doi:10.1007/BF00696583, 1994. Baltensperger, U., Schwikowski, M., Jost, D., Nyeki, S., Gäggeler, H., and Poulidas, O.: Scavenging of atmospheric constituents in mixed phase clouds at the high-alpine site Jungfraujoch Part I: Basic concept and aerosol scavenging by clouds, Atmos. Environ., 32, 3975–3983,doi:10.1016/S1352-2310(98)00051-X, 1998. Baumgardner, D.: An analysis and comparison of five water droplet measuring instruments, J. Appl. Meteorol., 22, 891–910, 1983. Baumgardner, D., Dye, J. E., Gandrud, B. W., and Knollenberg, R. G.: The forward scattering spectrometer probe (FSSP-300) during the airborne arctic stratospheric expedition, J. Geophys. Res., 97, 8035–8046, 1992. Baumgardner, D., Gayet, J. F., Gerber, H., Korolev, A., and Twohy, C.: CLOUDS — Measurement Techniques In Situ, in: Encyclo- pedia of Atmospheric Sciences, Academic Press, 489–498, 2003. Baumgardner, D., Kok, G., and Chen, P.: Multimodal Size Distribu- tions in Fog: Cloud Microphysics or Measurement Artifact?, in: 5th International Conference on Fog, Fog Collection and Dew, held 25–30 July 2010, M̈unster, Germany, vol. 1, p. 73, 2010. Baumgardner, D., Brenguier, J., Bucholtz, A., Coe, H., DeMott, P., Garrett, T., Gayet, J., Hermann, M., Heymsfield, A., Korolev, A., Krämer, M., Petzold, A., Strapp, W., Pilewskie, P., Taylor, J., Twohy, C., Wendisch, M., Bachalo, W., and Chuang, P.: Airborne instruments to measure atmospheric aerosol particles, clouds and radiation: A cook’s tour of mature and emerging technology, Atmos. Res., 102, 10–29,doi:10.1016/j.atmosres.2011.06.021, 2011. Beiderwieden, E.: Fogwater fluxes above a subtropical mon- tane cloud forest, Phd thesis, Westfälische Wilhelms-Universität Münster, 2007. Beiderwieden, E., Wolff, V., Hsia, Y., and Klemm, O.: It goes both ways: measurements of simultaneous evapotranspiration and fog droplet deposition at a montane cloud forest, Hydrol. Process., 4189, 4181–4189, 2008. Bennartz, R., Fan, J., Rausch, J., Leung, L. R., and Heidinger, A. K.: Pollution from China increases cloud droplet number, suppresses rain over the East China Sea, Geophys. Res. Lett., 38, L09704, doi:10.1029/2011GL047235, 2011. Bohren, C. F. and Huffman, D. R.: Absorption and Scattering of Light by Small Particles: the Interference Structure, vol. 29, John Wiley & Sons, 1983. Brockmann, J. E.: Aerosol Transport in Sampling Lines and Inlets, in: Aerosol Measurement: Principles, Techniques, and Applica- tions, chap. 6, 3rd Edn., edited by: Kulkarni, P., Baron, P., and Willeke, K., John Wiley & Sons, 69–105, 2011. Bruijnzeel, L. A. S., Eugster, W., and Burka