MAY 2001

A Continuous-Flow Diffusion Chamber for Airborne Measurements of Ice Nuclei


Department of Atmospheric Science, Colorado State University, Fort Collins, Colorado (Manuscript received 8 November 1999, in final form 1 August 2000) ABSTRACT A continuous-flow thermal gradient diffusion chamber was developed for operating in an aircraft and detecting ice nucleating aerosol particles in real time. The chamber volume is the annular space between two vertically oriented concentric cylinders. The surfaces of the chamber are coated with ice and held at different temperatures, thus creating a vapor supersaturation. Upstream of the chamber, all particles in the sample air larger than 2- m diameter are removed with inertial impactors. The air then flows vertically downward through the chamber, where ice crystals nucleate and grow on active ice nuclei to between 3- and 10- m diameter in 3–10 s of residence time. At the outlet of the chamber, an optical particle counter detects all particles larger than 0.8 m. Those particles larger than 3 m are assumed to be the newly formed ice crystals and comprise the ice nucleus count. This paper describes the principles of operation, hardware and construction, data system, calibration, operational procedures, and performance. Limitations of the technique are presented, and examples of measurements are shown.

1. Introduction Ice nuclei (IN) are aerosol particles that catalyze the formation of ice crystals in clouds (Vali 1985). A wide variety of measurement techniques have been developed over the past 50 years for detecting IN and measuring their characteristics. These techniques include drop freezing, particle capture on supercooled drops, particle capture on filters followed by processing, cloud chambers (static or flow-enhanced diffusion, slow or fast expansion, mixing, sedimenting drops), and others. It is generally agreed that ice will form on nuclei in response to different kinds of thermodynamic forcing, with the primary variables being temperature (T), supersaturation (SS), and the presence of a surface of supercooled liquid water (Vali 1985; Cooper 1974). Four ice nucleation mechanisms are currently recognized: deposition, condensation-freezing, contact-freezing, and immersion-freezing (Vali 1985). In controlled laboratory experiments, it is possible to categorize ice nucleation mechanisms according to whether the water–ice transition occurs primarily through vapor or liquid paths.

*Current affiliation: Research Aviation Facility, National Center for Atmospheric Research, Broomfield, Colorado. Corresponding author address: David C. Rogers, Research Aviation Facility, National Center for Atmospheric Research, 10802 Airport Ct., Broomfield, CO 80021. E-mail: dcrogers@ucar.edu

In a similar fashion, dominant nucleation mechanisms can sometimes be deduced from field data by comparing the predicted sizes and numbers of ice crystals with those observed (e.g., Cooper and Vali 1981; Heymsfield and Miloshevich 1993). In most cases, there is always a degree of uncertainty, and several mechanisms may be active at the same time. Even after 50 years of ice nuclei studies, a calibration standard ice nucleating material does not exist, and there is no general agreement on a standard technique for measuring IN or on how to interpret IN measurements. Because a variety of processes can lead to ice formation, mechanistic measurement approaches are preferred for improving the understanding of these processes. Atmospheric ice processes are very important in determining the properties of clouds and the development of precipitation, hence there is considerable scientific interest in trying to describe ice formation and growth processes (e.g., Szyrmer and Zawadzki 1997). Scientific review articles of cloud microphysics have consistently called for new ideas, greater versatility, and improved performance of ice nuclei measurement techniques (e.g., Hallett 1983; Cooper 1991; Rasmussen 1995; Baker 1997; and others). Topics of interest include the following. R For subsaturated conditions, detecting and quantifying deposition activity [there is some question about whether deposition occurs on natural IN particles. Its appearance is similar to the freezing of solution drops, although it is a conceptually different mechanism (i.e.,

2001 American Meteorological Society


1995b). and a newer laboratory chamber is listed in the right column. such as cycles of condensation and evaporation in clouds. experiments were performed with both natural and laboratory-generated aerosols. The evolution of the instrument is summarized in Table 1. The table shows that only the chamber geometry and diameter have remained the same. and recognizing the need to identify nucleation mechanisms. and in North Dakota (DeMott et al. in the 1993 and 1994 Winter Icing and Storms Projects (Rogers et al. and power. The following sections describe the instru- . hardware and construction. 1996).726 JOURNAL OF ATMOSPHERIC AND OCEANIC TECHNOLOGY VOLUME 18 R R R R R R vapor transfer direct to ice in the absence of the liquid phase)]. and simplified data analysis. but important factors for IN activation were identified. Ice nucleation measurement comparison workshops were held in the United States in 1970 (Grant 1971) and 1975 (Vali 1975). the same technique can be described several different ways. The entire rack-mounted system is approximately 65 110 130 cm tall. ment and its operating principles. competition for vapor in filter processing. physicochemical properties of IN. Thus. In both workshops. Measurements from the various instruments did not produce close quantitative agreement at either workshop. starting with the laboratory prototype described in Rogers (1988). 1 as installed in a standard 19-in. vertical atmospheric profiles of IN concentrations. For CCN. made them much easier to control. Examples of measurements are shown. and requires 15 amps of 120 vac power. Some techniques try to isolate and emphasize one mechanism. and performance. weight. software. calibration. 3. It has some advantages and some disadvantages. It was also used. there is a time delay separating the nucleation event from its detection. It is illustrated in Fig. nucleation mechanism (drop freezing). The chamber described here is a descendent of the laboratory instrument described in Rogers (1988. The chamber was lengthened to increase the time available for nucleation and growth of ice crystals. Description The airborne CFD instrument has been used in several field projects. Important criteria for the airborne version included 1) limiting the size. the increasing activity with particle size. and suggestions for future development are offered. thermodynamic process (expansion). 1994). diffusion chamber. which are discussed here. the ice nucleating response of particles at high supersaturations ( 5%). 2. with other techniques. b) thermal wave from the release of latent heat when a supercooled drop freezes. Operation of the chamber was considerably simplified with the addition of computerized display and data recording in 1996. These comparisons were based on bag samples of air collected by the aircraft and delivered to the laboratory for IN measurements. Of the measurement approaches available today. This paper describes a continuous flow diffusion (CFD) chamber instrument that was developed from an earlier laboratory chamber for airborne use. and 4) simplifying and automating many of the operational and analysis procedures. but there have been no subsequent workshops for ice nuclei. in studies of silver iodide aerosols (DeMott et al. and so forth. or exposure to pollution gases. These upgrades improved the accuracy of sampling conditions. Demonstrating the difficulty of measuring ice nuclei was a significant result in itself. only the controlled-expansion cloud chamber can be used to study all four nucleation mechanisms (DeMott 1995). The chamber volume is an annular gap The variety of different approaches for measuring ice nuclei is diverse. geographic regions and natural processes that produce IN. several intercomparison measurement workshops have taken place since the mid-1970s. filtration). weighs 120 kg. and processes that modify IN activity. 2) ensuring the chamber was air tight. The airborne instrument circumvents the problems associated with collecting air samples in bags and provides the capability for more direct comparisons between aerosol particles and ice formation in clouds. along with other IN instruments. The airborne chamber is in the middle column. 3) recording data at rates 1 Hz or faster. A common feature of ice nuclei instrumentation is that the nucleation event is detected in association with the appearance of the new phase as: a) growth of new ice crystals to detectable size in a supersaturated region. Principles of operation A simplified illustration of the components and conceptual principles of operation in the CFD chamber is shown in Fig. or d) a change in a bulk or ensemble integrated property. a separation is not possible. the freezing of activated cloud condensation nuclei (CCN) at slight water supersaturation (0% to 2%). Motivation for developing the airborne version came from generally favorable quantitative comparisons of IN measurements and aircraft observations of ice in clouds in the same region (Rogers et al. such as the dielectric constant. including sensitivity to vapor supersaturation. rack for the National Center for Atmospheric Research (NCAR) Electra aircraft. c) change in opacity of millimeter size droplets when a supercooled drop freezes (gas bubbles dissolved in liquid are created as ice forms). They can be classified according to instrument type (mixing chamber. limitations of the technique are outlined. The lab instrument was used to measure natural aerosol in Wyoming (Rogers 1993). 1996). 2. The mounting arrangement varies for different aircraft. In all of these cases. 1995a).

Computer-generated plots cles .1 Two refrigerated bath circulators Same 1996–98 Airborne Same 150 100 or 150 Same Same Two refrigerated bath circulators Either Climet Same Same Optional Same 6–60 s particle spectra Same Same Same 8 thermocouples Same Integrated MCA Same Same 1998—Lab version 100 50 Same Same One refrigeration compressor and expansion valves Particle detector Climet A6065a Climet 7350A Applying ice on walls Spray water on walls with Flood chamber volume with wachamber open ter Warm wall Inside cylinder Outside cylinder Insulated wall surface (drop evap. 10 s particle spectra (1998) Sample conditions: flow profile.2 s particle count. Airborne chamber in middle column.Foam insulation on lower 1/3 of Lower 1/3 section plastic PVC oration region) inside cylinder pipe Data logging Strip chart. computer files and Computer written notes Time resolution 10 s to 5 min 0. TABLE 1. 727 FIG. Rack mount arrangement for CFD chamber system as configured for NCAR Electra aircraft. Postexperiment analysis Real-time calculation and dissample location. critical flow Airflow Rotameters Rotameters and mass flow sensors Air pressure Aneroid gage Strain gage sensor Temperature 4 thermocouples 6 thermocouples Temperature reference Thermocouples 2 precision thermistors Particle size Separate MCA Single threshold (’96). Description Chamber geometry Chamber length (cm) Growth region (cm) Cylinder diameters (cm) Annular gap (cm) Thermal control 1982–88 Vertical axis concentric cylinders 45 30 8. ‘‘Same’’ indicates earlier feature was used again. and parti.MAY 2001 ROGERS ET AL. Scales are in. play super-saturation. pressure. 10 1. temperature. Lab version in right column. integrated MCA (’98) Exhaust air Discard Recycle to sheath Real-time data display Temperature. Properties and evolution of three ice nuclei CFD chambers. MCA multi-channel analyzer. 1.

2. reducing it to 4.5 m). Ice crystals were grown as spheres. droplets lowered it to 19%. the calculated supersaturation decreased according to the vapor excess. the sample temperature corresponds to the average temperature of the two wall temperatures. Actually. Temperature and supersaturation conditions at location of sample air as calculated from warm and cold wall temperatures with flow of 10 L min 1 (Rogers 1988). Since there are particles 3 m in the air. In the first few centimeters. the sample is exposed to 25 C and water saturation. 20 C. Equations for calculating the time-dependent temperature. the sample air is not located in the middle. The cylinders are held at different temperatures. 3. It is possible to set the wall temperatures to obtain very high water supersaturations (SS w ) nominally up to 60% and higher. The calculations assumed 1000 cm 3 of CCN particles (activating half at 0. When only droplets were present (no ice crystals). Nucleated concentrations of ice ranged from 0. We estimated the effect on SS w due to vapor competition by droplets and crystals. they could be erroneously counted as crystals. instead. Sample temperature and supersaturation are independently controllable. The pulses are digitized and accumulated in a multichannel analyzer (MCA) and recorded by computer. thereby limiting the attainable supersaturation. although CCN and IN will activate and grow.079 cm 3 at 40% SS w . This evaporation region helps to exaggerate the size difference between ice crystals ( 3– 10 m) from the much smaller residues of cloud droplets ( 0. and by 40% SS w .1% and the remainder at 0. as described in section 3b. the amplitudes of the OPC voltage pulses correspond to particle size. and a supersaturation forms between them. (1992). the droplets had only a slight effect on the vapor field. Simplified illustration of CFD chamber components and operating principles. but slightly on the cold side of the midpoint. The aerosol sample comprises about 10% of the total flow. Generally speaking. The wall temperatures and rate of airflow determine the temperature and supersaturation that the sample experiences. droplets lowered it to 9. and isohumes (% water supersaturation) curve from lower left to upper right. forcing water droplets to evaporate (Rogers 1988). and ice particle concentrations from Meyers et al. The ultimate limit depends on CCN concentration. In order to avoid that error. and whether any ice nuclei are present. using equations for a parallel plate CFD chamber from Rogers (1988) and from Plooster (1985). particles larger than 2 m are removed at the inlet of the instrument by an impactor system.04 and 1. whereas the supersaturation corresponds to their difference. and velocity profiles were derived in Rogers (1988).97%. FIG. at 20%. Figure 3 shows the relationship between temperatures of the warm and cold walls and the sample conditions at a position four tenths of the distance from the cold wall to the warm wall (a typical location) after steady-state linear profiles of temperature and vapor concentration are achieved.8%. and this change in boundary conditions creates a region that is below water saturation. The detection of ice crystals (or ice nuclei) is based on a particle size exceeding 3 m.728 JOURNAL OF ATMOSPHERIC AND OCEANIC TECHNOLOGY VOLUME 18 FIG. This chart provides guidance for setting the sample conditions. Droplets and crystals nucleate in the supersaturated region and grow as they pass through the first two-thirds of the chamber.5%). at 10% SS w . One may ask why measurements of IN should be made at such high supersaturations when the common understanding among cloud physicists is that the max- .1-cm annular space between two lamina of particle-free sheath air. between two ice-coated cylinders. Isotherms ( C) slope from upper left to lower right. temperature. For example. Ice crystal growth was estimated using a diffusional growth equation with the same condensation and thermal accomodation coefficients as assumed for water (0. There was no discernable effect of ice crystal growth to reduce SS w beyond the effect from droplets. due to the convective component of the flow. supersaturation. the sample is smoothly injected into the 1. The last third has no ice on the warm cylinder. as follows: at 5% SS w . the particles are counted with an optical particle counter (OPC). it is dry and a poor heat conductor. respectively).038 cm 3 at 5% SS w to 4. with the walls at 31 and 16 C. the presence of droplets reduced the supersaturation to 36%. At the chamber’s outlet.

4. to operate at outside pressure in a pressurized cabin. Airflow A sketch of the airflow distribution in the CFD system is shown in Fig. Mass flow meters monitor the air flows. of which the sample is 10%. the walls are dry for the first 10 cm.. racks in an aircraft cabin as small as that of a Beech King Air ( 127 cm height). flows. and 2) to preserve the temporal resolution for real-time sampling.g. while the temperature is adjusting. transient high supersaturations should be avoided. High supersaturations may also be appropriate for laboratory experiments on particles with hydrophobic surfaces. the air can be quite humid. allowing mechanistic studies of particular nucleation mechanisms. The scientific goals included sampling in the temperature range 10 to 40 C and humidity from ice saturation to 20% water supersaturation. even when CCN concentrations are high. Several ways are employed in the CFD to avoid such transients. Rogers et al. Another reason is that high SS w set points ensure that water saturation is exceeded. Shaw 1998). Perma-Pure tube) can be used to reduce the vapor concentration. a diffusion dryer (e. For example. This air contains less moisture. since it is ice-saturated at the cold wall temperature. Smooth laminar flow is needed 1) so that the temperature and humidity fields are well defined. and to use a sufficiently small amount of conventional electrical power (115 vac 60-Hz single phase) for laboratory or aircraft operation. Rogers 1988). Hobbs and Rangno 1990. sheath 9L imum rarely exceeds 1% or 2% in natural clouds. First. with sampling rate at least 1 L min 1 . The total flow through the CFD chamber is 10 L min 1 . Inlet and exhaust min 1 .MAY 2001 ROGERS ET AL. If the sample is saturated and colder than the sheath air. With high SS w . 1973. and temperatures. 729 FIG. Baker 1991. In measurements of any cloud-active aerosol particles.g. so that the ball-type flow meters are not nec- . The other 90% is filtered and returned to the chamber as sheath flow. Mahata et al. Electrical sensors measure the pressures. Specifications Performance goals for the airborne chamber were established from scientific and practical criteria. it has been speculated that part of the discrepancy between ice concentrations observed in clouds and measurements of IN could be attributed to an occasional occurrence of very high supersaturations in small pockets in cumulus clouds (e. 90% of the chamber’s exhaust air is filtered and used as sheath air. The response of natural aerosol particles to high SS w can be explored with the CFD. 4. 1 L min 1 . and droplets will supercool and grow quickly enough to avoid the freezing point depression of concentrated solutions. 1994. all CCN are activated. In this case.. Airflow in CFD chamber instrument. There are several reasons. a. When sampling at low altitudes in the summer. b. The second way of avoiding transients is to keep the walls dry initially. then calculations indicate transient supersaturations can occur in excess of the steady SS values achieved downstream (Fitzgerald 1970. The present design meets these goals. in the CFD. The practical goals were to have the instrument fit in standard 19-in.

7 m. The bypass protects the mass flow meter from damage by any residues of water. essary. Further evidence that the sample remains in a laminar layer and does not spread in this kind of chamber was provided by timing experiments in Rogers (1994). so crystals could evaporate and/or melt in transit. The large variability above 1. so we expected the merging of sample and sheath air to be smooth with little mixing. in field studies. This bypass is used for a short time after the icing procedure. 200 MCA channels cover the size range 0. (Dots) Measured efficiency for double impactor and 0. Measurements of the collection efficiency at room pressure ( 850 mb) are shown in Fig. The OPC (Climet 7350A sensor) attaches to the base of the CFD chamber. The inner cylinder consists of the copper pipe with a . the Reynolds number in the chamber is 40. for identifying boundaries between regions with different atmospheric aerosol structure. c. although there is little time available ( 12 ms). Otherwise. This region is insulated but not cooled. The impacting surface is coated with a thin layer of vacuum grease to increase the likelihood that impacting particles will stick. At the system inlet. but they provide convenient visual cues and confirmation of the electronically measured values. Inlet impactor removes particles 2 m upstream of CFD chamber. FIG. a bypass in the airflow can be selected (Fig. 6. Hardware components and construction The walls of the CFD chamber are constructed of 3 and 4 in. Figure 5 shows the construction of these impactors. and they confirmed that the flows merged smoothly. 4). but 95% of these are captured in the second stage. for calculating the fraction of total particles that are IN. when the chamber is flooded with water. The air pump is a diaphragm type and produces oscillations 30 Hz in the airflow. type DVW.8 L min 1 and particle density 1. there are two identical inertial impactors in series to remove particles larger than 2 m. For particles 2 m. Cut-away view shows construction based on compression tubing tee. 6 along with theoretical calculations based on Ranz and Wong (1952). approximately 5% get past the first stage.8 L min 1 . Rigid stainless steel tubing is used where possible. 11 cm long from the chamber to the crystal impaction surface.5 g cm 3 . Beyond the crystal collector. flexible electrically conductive tubing is used on the inlet side of the CFD and silicone tubing on the outlet side. 5. Not shown in the airflow diagram is a parallel branch with a condensation nucleus (CN) counter. All of the air flows through the OPC and then through the crystal impactor (described later). and. Efficiency of inlet impactor to remove particles. Flow visualization tests were performed to examine the sample injection region. Check valves and ballast tanks ( 1 L) on the inlet and outlet of the pump are used to damp these oscillations. and impactor are coaxial tubes. OPC. was measured by an OPC sampling ambient air with and without the impactor. The CFD outlet. well within the laminar flow regime. Figure 7 shows the arrangement of components and geometry.6 to 4. The distance from the jet nozzle to the impaction surface is adjusted to equal the nozzle diameter in order to optimize its performance (Marple and Liu 1974). as a function of particle size. The 90% cutoff occurs at 1. diameter copper tubing. The CN measurements are complementary to the IN data and are valuable for estimating particle losses in the inlet piping. to put ice on the walls.5 m is due to the large sampling uncertainty (very few particles got past the impactor). there was no indication of turbulence or shear induced mixing.730 JOURNAL OF ATMOSPHERIC AND OCEANIC TECHNOLOGY VOLUME 18 FIG. These oscillations show up in the mass flow sensors and can produce erroneous estimates of the average flow through aliasing.8 m. With total air flow of 10 L min 1 . Two such impactors are used. The collection efficiency. All airflow passes through the crystal collector just below the OPC. (Thin line) Theoretical collection efficiency based on Ranz and Wong (1952) equations for a single round jet impactor with 0.

Thermocouples are supported by the coil and push against the inner surface of the pipe. The data systems for the airborne and lab CFD chambers are nearly identical. making it slow to respond when the temperature changed. 7). 731 ice application procedure. 8. soft copper tubing. The CFD chamber is constructed of two concentric cylinders. delrin.74 cm. The gap then narrows to 1. At this point. The calibrations include voltage. Overall height 100 cm. of these 32 channels. The o-rings remain flexible at temperatures below 50 C. chamber pressure.MAY 2001 ROGERS ET AL. as a check on consistency and to look for stability and drift of the A/D converter. From the top down. temperature. of which 4 are on the inside of the inner cylinder and 4 are on the outside of the outer copper cylinder (Fig. The amount of oil was reduced by 50% by filling the inside of the inner cylinder with high-density hollow polyethylene balls (20-mm diameter). During construction. airflow. It was wrapped tightly around the 4-in. coiled to be a snug fit inside the 3-in. Temperatures are measured with 2 thermistors and 12 type-T thermocouples (copper-constantan). Basic calibrations are performed on the electronics before and after field campaigns. The collection of signals is illustrated in Fig. copper pipe. the gap between the inner and outer walls is 1. and aerosol particle size.12 cm for the remainder of the chamber. The refrigerant evaporator coil for the outer cylinder is also 3/8-in. A precision voltage source (AD580J device. All surfaces of the copper pipe chamber walls were treated with an ebonizing solution to make them wettable and to avoid oxidation of the copper.500v) is built into the signals interface box. The refrigerant evaporator for the inner cylinder is 3/8-in. shown separated here. 2. d. copper pipe. the thermocouple junctions were dipped in thermal epoxy adhesive to provide electrical insulation and to prevent oxidation. This epoxy was also used to attach thermocouples to the outside of the outer cylinder. however. Locations of thermocouples (Tc) and thermistors (Ts) indicated. PVC. The layer is very wettable (small contact angle). they are: PVC pipe. The sample and sheath flows are combined at the top section of the chamber in the delrin–PVC section. 16 are for low-level (microvolt) thermocouple inputs. The ebonizing solution is caustic and reacts with the copper to form a thin surface layer of black cupric sulfide crystals. Analog electrical signals for temperature. and refrigerant pressure are measured with an 8-channel 12-bit analog-to-digital card. Using only oil. The inside of the inner cylinder is filled with heat transfer oil to improve the thermal connection between the refrigerant coil and the cylinder wall. would give the cylinder a large heat capacity. it allows water to flow smoothly and cover the entire surface rather than beading up. Small copper tubing is for refrigerant. air pressure. the thermistors and thermocouples were FIG. airflow. The sample air passes through a thin slit (0. A digital input/output card communicates with the refrigeration control electronics. pipe in a spiral with 5-cm spacing between adjacent turns and attached to the pipe with a wide solder joint to enhance the heat transfer. 7. Before the chamber was assembled.25 mm) in an annular blade in the middle of this gap. so the power for the data system is filtered through an uninterruptible power supply. Its voltage is measured every time the data system starts. Interruptions and spikes in electrical power are common on aircraft. All temperatures are ultimately referenced to a platinum resistance thermometer (PRT). Joints where the outer cylinder components can be separated are sealed with ethylene-propylene o-rings and vacuum grease. soft copper tubing. and the other 16 are for higher level (millivolt) signals. It provides a stable source for the thermistors and a calibration reference check for all voltage conversions. It has a thermal R-value of 15 per layer (thermal conductivity 10 3 erg s 1 cm 1 K 1 or 40% of the value for dry air). Five sections comprise the outer cylinder. During the . It is light in weight and unaffected by moisture. and a delrin cone. structural brass collar soldered at the top and a delrin cone at the bottom. Inputs for two of the channels are multiplexed to 32 channels with a vendor-provided expansion board. a laminate of aluminum foil and polyethylene bubble pack. The outside of the chamber is wrapped in three layers of Reflectix insulation. Signals and data system The data system is based on an IBM-type PC computer (486DX-66) with plug-in cards and an electronic interface for signal conditioning. Sheath air flows along the inside and outside of the blade and enfolds the sample air at its tip.

The MCA sorts pulses into 256 channels and accumulates a pulse height spectrum every 10 s. The thermistor beads were also coated with thermal epoxy. Thermocouple temperatures are calculated from a third-order polynomial equation that was derived from the manufacturer’s (Omega ) tabulated values of voltage and temperature from 40 to 60 C. CJC cold junction compensation for thermocouples. After the chamber was assembled. They are used in a resistance bridge with metal film resistors and the precision voltage source. this error can be several degrees. One was mounted near a thermocouple in the middle of the outer cylinder. Calibration checks have shown that the overall accuracy of the temperature measurements remains within 0. it was no longer possible to collocate and calibrate all the temperature sensors simultaneously. On the multiplexer card (Fig.5 C from 20 to 50 C. each of these connections is another thermocouple and adds a potential error. This point is illustrated later in section 5 of this paper. The MCA is a PC plug-in card (Oxford PCA3) of the type designed for nuclear decay measurements. the connections are made on an isothermal cold junction reference (6-mm-thick aluminum plate covered with 1 cm of thermal insulation). OPC optical particle counter. When temperatures are being changed.4 C from 20 to 40 C. Total and sheath airflows are measured with mass airflow sensors (Honeywell Microbridge type AWM5104vn). 8) is independent of the MCA. Accuracy was within 0. When steady conditions have been established. and the other is in a thermowell immersed in the center of the inner cylinder. Therefore. which serves as our standard. the error is relatively small ( 1 C). It generates a digital logic pulse that is counted by the data system when a pulse exceeds the preset .732 JOURNAL OF ATMOSPHERIC AND OCEANIC TECHNOLOGY VOLUME 18 FIG. MCA multichannel analyzer. A/D analog-to-digital converter. a thermocouple junction is formed. Coefficients derived from our calibrations are used in the real-time CFD data system. 8). 8. Air pressure of the chamber and aircraft cabin are measured with factory-calibrated Motorola MPX4115 piezo-resistive sensors. The plate temperature is measured with an imbedded LM-35 sensor that is calibrated against a PRT standard.5 C from 20 to 50 C. since they determine the sampling temperature and supersaturation. There is an intrinsic uncertainty or error in these values because our measurements are made not on the surface of the ice but on the copper walls. The OPC produces one analog pulse for each particle. Block diagram of signal processing in CFD data system. The cubic fit is within 0. These were factory-calibrated with dry nitrogen. Additional calibrations are done at our laboratory using a Wallace and Tiernan aneroid gage.03 C of tabulated values. The temperatures of particular importance are those of the ice surfaces. Where two different metals connect. and the correction is applied in software. immersed in a temperature-controlled bath circulator and were calibrated against a PRT. thermocouple signal wires (copper and constantan) are attached to screw terminal connectors and to tinned copper signal lead wires. with pulse amplitude increasing approximately with the surface area of the particle. To correct for this. two precision thermistors (YSI 44003A) were installed in the CFD chamber to serve as independent measurements and built-in calibrations of the thermocouples. We performed additional calibrations with air using a Gilibrator (volume measurement) and local pressure and temperature to convert volume flow to mass flow. The threshold circuit (Fig. Their published accuracy is 0. The pulses go to both the MCA and a threshold circuit. hence.

top) was made to set the sampling at 20 C and water supersaturation of 5%. Refrigerant pressures are measured at the low-pressure ends of the evaporator coils. The outer wall began warming. Temperature control The temperature of the chamber is controlled by cooling or heating the walls with a compressed gas refrigeration system that is similar to a conventional household refrigerator appliance. high-pressure gas from the compressor to the evaporator coils.MAY 2001 ROGERS ET AL. 733 FIG. Line (E) at top is expansion pressure regulator valve used to separate refrigerant flows to inner and outer cylinders. Thermal wave at 2150 UTC is from flooding chamber with water to put ice on walls. the walls were both 25 C. Cooling occurs as liquid refrigerant (DuPont Suva HP-81) evaporates in coils of copper tubing on the CFD chamber walls. Saturation vapor pressures determine the boiling points of the refrigerant. Ice nuclei sampling 2110–2145 and 2205–2245 UTC. and temperature response on inner (i) and outer (o) walls as measured by thermistors and thermocouples. An example of the temperature control by the refrigeration system is shown in Fig. 9. that is. Rapid warming of the walls can be achieved by routing hot. smaller valve openings. Illustration of (from top) refrigeration valve control. an expansion valve adjustment (line E. refrigerant pressures. the sampling conditions were obtained. . In general.m particle and 10 L min 1 flow. and within about 10 min. At 2107 UTC. Initially. The temperature of the walls is determined by three refrigerant expansion valves that are controlled by the user through the data system computer. e. and these are calculated and displayed by the data system. threshold value corresponding to a 3. lower tempera- tures are achieved with lower pressures. 9.

Our calibrations showed the response is flat from 1. Error bars are standard deviation. the airflow is divided among as many as five converging nozzles.m diameter. it covers 0. particles spend greater time in the beam. inside it. 6). but we operate it over a range from 5 to 20 L min 1 . the design goal was 50% cutoff at 3. the reciprocal of the airflow rate. Curves show simple fit.1 L min 1 . this OPC was not suitable for calibrating the collection efficiency of the inlet impactor (Fig. Figure 10 also shows that the OPC has a strong sen- FIG. the dominant peak is in channel 68 7 (standard deviation). atomized from aqueous dispersions. where the peak channel corresponds inversely with flow rate. The other peaks were recorded using the same particle source but with different flow rates through the OPC.4 to 2 m.734 JOURNAL OF ATMOSPHERIC AND OCEANIC TECHNOLOGY VOLUME 18 FIG. The explanation for this is that the light detector in the OPC is a PIN photodiode.m oleic acid droplets at 3 different flow rates. 10.m particle produces the same amplitude pulse as a 2. the airflow through the center nozzle can be adjusted by plugging some of the other nozzles with ball bearings. The ice crystals that are collected contain the ice nucleating particles.m particle.0. The OPC is over sampled in the sense that the MCA provides 256 channels (or more). Polystyrene latex spheres 0.1 m oleic acid particles. Note effect of volume flow rate. Voltage pulse height distributions from the Climet were measured with the MCA and were used to set the threshold counting circuit voltage to correspond to 3. This sensitivity is clearly illustrated in Fig. The crystal impactor in Figs.m particles at 10 L min 1 . and the detector produces larger voltage pulses.47 to 2. The response of this OPC for monodisperse particles is fairly narrow. 2 and 4 is an inertial type device for collecting ice crystals that nucleated and grew in the chamber. A series of calibrations was performed to establish the OPC’s response to both particle size and flow rate. it is sensitive to the residence time that particles spend in the region illuminated by the laser beam. The manufacturer’s specification is 1. we used a different OPC (Climet A6065A) that does not have this flat response characteristic. most often at 10 L min 1 . At a flow rate of 6. Therefore. Channel 5 10/Flow · Dia 2 for 6. and 20 L min 1 . that is. were also used for calibration. The CFD chamber threshold counting voltage is set for 3. Particles larger than the primary peak are also evident. For example. and particle density.m particles. the OPC range is 2 to 22 m. 11. 10 shows MCA spectra for monodisperse 6. This warming is useful for effecting rapid temperature changes and for melting the ice off the chamber walls.1.4582). For that purpose. although the OPC is not capable of resolving more than 21 channels.6. To achieve this over a range of flow rates. 12. f.588). As a charge integrating device. The results are shown in Fig. 1. Three pulse height calibration spectra for 6. that were produced by a vibrating orifice aerosol generator (Berglund and Liu 1973). With one stage of manufacturer-supplied amplification. The cut-off size and efficiency of collection depend on flow rate. As the ice evapo- . these form when multiplets of the primary particles agglomerate.0 m (n 1. air density and viscosity. Calibration of Climet OPC using spheres of oleic acid or polystyrene latex at three different flow rates. 10.5 to 2 m.4746) and oleic acid (n 1. sitivity to flow rate. Particle detection The Climet OPC was calibrated with monodisperse spheres of glycerin (n 1. Fig.0 CFM (28. At 20 L min 1 . It consists of a centimeter-size replaceable cartridge.1. At smaller flow rates. 11.3 L min 1 ) for this OPC. a 1.to 22. with resolution 10% of the mean size.m diameter. The center nozzle is directed at a post that holds a transmission electron microscope (TEM) grid. that is.

the pump is switched off. the IN are left on the TEM grid as residuals. Rogers . The strategy for TEM sampling is to keep the chamber temperature and supersaturation steady. 1973. Then it enters an endless polling loop with a sequential interrogation of the analog and digital cards. After this test. Temperature and supersaturation control The temperature and vapor fields of the sample are dominated by the walls. Sample and sheath air are valved off. Then the pump is switched off. The monitor displays the measured and derived values as well as information about data logging and instrument status or errors. with some components in assembler code and linkable drivers provided by the hardware manufacturers. One method we tried was to flush the cold chamber with a continuous stream of air saturated with water at 20 C. and the chamber pressure is monitored for 1 min. and aerosol sampling begins. the pump is switched on.3 min) to limit the amount of data loss in case of power failure. and the water drains through the pump and back into the tank in 25 s. Sinnarwalla and Alofs 1973. A satisfactory result was obtained by pumping a premeasured volume ( 3 L) of deionized water into the chamber through the outlet hole in the bottom. Coating the chamber wall surfaces with ice Ice is applied to the walls by first removing the OPC and cooling the chamber to 20 C. frost can extend several hundred micrometers into the chamber. At start up.1 mm thick on the inner and outer walls. and the chamber is pumped down to 180 mb. In either case. which typically requires sample times of 30 min or more. and to estimate the number of particles collected from the OPC count. 735 rates. The data are recorded as a series of small binary files ( 30 kbytes). and the airflow is adjusted to 10 L min 1 . Calculations based on the wall temperatures and airflow rates are made in real time to predict the location. We believe that these particles are ice fragments that break off the walls and fall into the air stream. particles 3 m are detected by the OPC even when sampling filtered. The MCA spectra are recorded in separate files. The goal is to collect at least several hundred particles on each grid. but the results were unsatisfactory. During development of the airborne chamber. A new file is created every 200 records ( 3. After several hours. This volume of water reaches the top of the copper section of the outer cylinder within 12 s. and correction factors are applied. Calculations indicate that the incoming air reaches steady-state profiles in 2 s (Mahata et al. the OPC is reattached to the chamber. The thickness was estimated by thawing the ice and measuring the melt water. The software was written primarily in Borland Turbo Pascal . morphology. temperature. Tests of the ability of the CFD technique to separate IN from non-IN are described in Kreidenweis et al. Without reicing. Next. As the chamber and its descendents were developed. 3). At present. (1998). and a pressure leak test is performed to check that the chamber is air tight. The explanation of this phenomenon is not obvious. Software Data logging and display are accomplished with a single MS-DOS program. and composition can be studied with single particle analysis techniques. water vapor is continuously subliming from the warm wall and depositing on the cold wall. leaving a smooth layer of ice 0. the chamber is returned to ambient pressure. At this point. b. g. derived parameters are calculated. Pressure increases of 0 to 1 mb min 1 are considered acceptable. Operating procedures This section describes the chamber preparation and the procedures for sampling. Their size.MAY 2001 ROGERS ET AL. so as not to mix nucleation mechanisms. an unacceptably high background rate. 4. analog measurements are made of 23 parameters. This process eventually leads to the formation of frost crystals growing on the cold wall and ice-free or rough ice patches on the warm wall. In the earlier prototype (Rogers 1988). one cycle in the loop takes 1 s. the inner cylinder was removed so that water could be sprayed and smoothed onto the walls. and each measurement is an average of 10 A/D conversions. This rapid flooding of the chamber with water produces a strong thermal wave. but there are two possible sources of particles: frost fragments breaking off the cold wall and residues of ice fingers (spicules) from the warm wall (Oraltay and Hallett 1989). the particle count rate will continue to rise and can reach a few per second. the program establishes communications with the electronics and loads the calibration values. these procedures evolved and were modified as needed for field or lab operations. Results using this technique in a field study are reported in Chen et al. this procedure was not suitable for airborne applications. as can be seen in Fig. To retrieve the recorded data. We have found that after 2–3 h. a. the problem is solved by flooding the chamber with water to refresh the ice surface. Because of the gradients in temperature and vapor pressure. wall temperatures are set to obtain the desired conditions (Fig. 9 at 2150 UTC. the binary records are unpacked and concatenated. Temperature excursions on the outer wall are larger because the outer cylinder has less mass than the inner cylinder with its heat transfer oil. It produced thick layers of frost near the entrance region with little ice elsewhere. (1998). particle-free air. and supersaturation of the air sample lamina using equations from Rogers (1988). several different methods were explored to put ice on the walls. After applying the ice.

30% of the total CN aerosol is lost. and the uniformity of wall temperatures. and the supersaturation was 5.3 m). Since this determines the amount of growth time available.7 C ( 0. we examined MCA spectra during the 20 May . which is injected at the top of the chamber. Typically. we use wall temperatures averaged from thermocouples. however. 9. the stability after reaching set points. Typical times needed to flush the piping are 5– 10 s.0 C ( 0. haze droplets. That is. the outer cylinder thermistor measured 9. Because the sample air is injected into a centrally located lamina. low number concentrations of ice nuclei add an additional limitation on temporal resolution.736 JOURNAL OF ATMOSPHERIC AND OCEANIC TECHNOLOGY VOLUME 18 1988). not including those near the top. Notice that the topmost thermocouples (#0 and #4) are the warmest places on the walls. the thermistor was 24. The airborne CFD uses only a refrigeration compressor. The response of wall temperatures to changes in the refrigerant expansion valves was shown in Fig. 5. Size alone differentiates them from cloud droplets. little information is available on their size. In the CFD system. 12. and an empirical correction is applied to the CN data. etc. the locations where ice crystals nucleate may vary. the NCAR Electra during Lake-ICE/Snowband (Kristovich et al. These gradients are more obvious when the same data are plotted with the thermocouples referenced to the thermistors. To illustrate the range of particle sizes measured by the OPC.97% 0. since there are no such things as standard ice nuclei.6 C ( 0. c. the CFD method can resolve 1-s changes in aerosol properties (Rogers 1994). The temperature stability of this system can be estimated from 2130 to 2145 UTC (3 min after the last valve adjustment) in Fig. Since IN are relatively scarce. Measurements from one of the Arctic flights are used to illustrate several aspects of the CFD’s performance and the types of data it produces.9 to 0. Travel times from the system inlet through the piping and the CFD chamber depend on how the CFD is installed in different aircraft and on the lengths and ventilation rates of tubing. Laboratory versions of the CFD chamber use two temperature-controlled bath circulators in which the refrigeration compressors run constantly and the electrical heaters control the temperature of the fluid. For example. Typically. however. as in Fig. valves. thermocouples #0 through #3 differed from the thermistor by 0. A more accurate assessment of the losses would involve estimates of particle sizes. a zero response is usually obtained after filtered air has flushed through the chamber. and the NCAR C-130 in the combined NSFSHEBA/NASA FIRE Arctic Cloud Experiment (Curry et al. and then the wall temperatures were adjusted for sampling at 10 C and 1% SS w . Performance and examples of measurements The new airborne chamber has been used on several aircraft. These times are estimated by using an OPC at the outlet and admitting ambient air or particle-free air at various places in the piping network.5). The chamber was reiced at 2150 UTC.7 to 0. Notice that the thermocouple temperatures (bottom panel) mimic the thermistor temperatures and show that gradients in the wall temperatures occur during temperature changes.2 C. 1998). In addition to the deliberate removal of particles 2 m by the inlet impactor. To the extent that thermocouple temperatures accurately represent the ice surfaces. There is. tees. 12. however.05 C). 2000). temperature. However. For setting the sampling conditions. and electrical charge. Filtered air There is no way to perform ice nuclei calibrations. and the effect of the filter is not dramatic. We estimate the magnitude of these losses with a CN counter by sampling cabin air with and without the tubing. This method of measuring ice nuclei relies on identifying ice crystals (containing ice nuclei) solely on the basis of their optically measured size. the calculated temperature was 19. the crystal count on sample air is usually a small number (few counts per minute). 2000). pressure. 4) to remove essentially all particles from the sample (99. There are uncertainties that can reduce the size of crystals and weaken the power of this method.2). the National Aeronautics and Space Administration’s (NASA’s) Ames DC-8 during the SUCCESS project (Rogers et al. Our practice is to use this filter for brief periods ( 1 min) several times per hour to estimate the background (or blank) count. air can be valved through a HEPA filter (Fig. including transport through the chamber to the OPC. or dry aerosol. humidity. its effect is immediately seen on the concentration of small particles in the MCA spectra. During this 15-min period. crystal sizes will vary accordingly. At the location of the air sample lamina. For the ice nucleating particles.0% ( 0. there are diffusion and deposition losses in the piping. On the inner cylinder. as the growth rates are approximately proportional to supersaturation. a standard to produce particle-free air—a HEPA filter. the supersaturations and sampling temperatures will also vary longitudinally in the chamber. Longitudinal gradients are evident as deviations from horizontal lines. the number of particles 2 m falls to 0. including the University of Wyoming’s King Air 200T for engineering tests. probably due to heating from the airflow. the four outer thermocouples differed from the thermistor by 0. They occur when temperature adjust- ments are being made and are of short duration ( 1 min).2). and we were interested in seeing how its performance compared with bath circulators in terms of the cooling time. Calculations of growth rates suggest there is ample justification for this approach.1 C and were stable ( 0.3). and no corrections are applied.

the background is estimated by sampling through the HEPA filter for a few minutes every hour (cf. The IN concentrations ranged from 0 to 88 L 1 .MAY 2001 ROGERS ET AL. and relative humidity 23%. The maximum would be smaller if the average were taken over longer intervals. each MCA spectrum (10 s) had between 0 and 7 ice crystals. For the CFD method. All methods of measuring IN require an evaluation of and accounting for the background or blank count. If a different size was used as a threshold. The NCAR C-130 was level at 4-km above mean sea level (MSL). There were 158 particles 3 m. the largest count in a second was 5. respectively. 4. 14 shows the integrated size spectrum. We interpret the slope change at 2–3 m as dividing ice crystals from other particles. the background is estimated by processing a filter that has sampled no air or that has sampled only particlefree air. 1998 field experiment over the Arctic Ocean that was described earlier. This is the number of crystals that are detected when no IN particles are present. Aerosol concentrations were fairly uniform during this time. ambient temperature 14 C. The IN were sampled at 23 to 20 C and 15% to 9% SS w . Fig. and 5 m are 158. For example. as mentioned earlier. There are typically a great number of samples with zero counts. 11 with counts of 2. as indicated by CN. the numbers exceeding 3. 13. This largesize range of crystals is a feature typical of MCA spectra for the CFD. Of the 1169 displayed. the IN concentration is plotted in Fig. and conversely. The last third of the chamber has no ice on the warm . and 82. and the average concentration was 16 per liter. For example. the integrated count would change. From 2111 to 2133 UTC. 106. 12. 14 shows particles from 1 to 13 m. The IN data (second panel from bottom) are shown as both the 1-s crystal count and the 10-s average number concentration (plotted upside down for comparing with the counts). there are 1050 s with 0 counts. flying a series of open rectangle patterns with 8-km legs ( 1 min). PCASP. 13 as 10-s average values. After accounting for the background. 102 with counts of 1. and Fig. The air was cloud free. 9. Sampling conditions in the CFD chamber during this time were shown in Fig. and FSSP-300 measurements. The size distribution in Fig. the concentration of IN is calculated by subtracting the background count from the total.. The counting statistics can be approximated with a Poisson or exponential distribution. Difference between thermocouple and thermistor temperatures for outer cylinder (top) and inner cylinder (bottom) for same time period as Fig. Figure 13 also illustrates features that are typical of real-time IN measurements made in the field. etc. Data from 120 spectra were summed in order to increase the number of crystals and produce an average spectrum. with membrane filters. Uppermost thermocouples are 4 and 0. 737 FIG. 4).

even for SS w up to 5%. 13. 256 channels were collapsed to 30 bins 0. Same data shown with filled circles (left scale) and open circles on folded (right scale) for clarity 3 m. some droplets do not evaporate to subdetectable residues. Calculations were made for the geometry and residence time in the new chamber and incorporating ice crystal growth. That is. 14 suggests there is probably a size overlap between ice crystals and other particles. Size distribution of particles 20 May 1998 2122–2133 UTC.738 JOURNAL OF ATMOSPHERIC AND OCEANIC TECHNOLOGY VOLUME 18 FIG. this size information can be . In controlled laboratory experiments. and all crystals do not nucleate at the same time and grow to the same size. Calculations by Rogers (1988) indicated it is unlikely that cloud droplets can exceed 3 m at the chamber outlet. but those calculations assumed boundary conditions for the ideal evaporation case (warm wall dry with no heat flux). These calculations also indicated ice crystal diameters at the chamber outlet should show clear size separation from liquid droplets. as described in section 3. They indicate it is unlikely that droplets can exceed 3 m at the chamber outlet for SS w up to 9%. as explained earlier in section 3. In spite of the size calculations. 14. Note 10-s average IN concentration (second panel from bottom) is plotted upside down and referenced to ordinate on right side. FIG. and they assumed crystals nucleated immediately when the vapor became supersaturated. the absence of a discernable particle gap in Fig. Time history of CFD chamber measurements during field project. accumulated from 120-MCA spectra.4 m wide. wall to force droplets to evaporate. For example. Crystal count threshold at 3 m. ice crystals should range in size from 8 to 12 m at 5% SS w and 20 C.

Size distributions of 0. the increasing activity for this dataset is due to supersaturation. The rapid increase that occurs above water saturation suggests that the strong contribution is due to the onset of another mode.2 m (dry size) ammonium sulfate particles growing in CFD chamber at 20 C and extremely high water supersaturations. 15. as labeled. The exact value of particle size that determines the threshold counting of ice crystals can occupy a range of values and cannot be precisely defined. is small. It is critical in the sense of avoiding two kinds of errors: counting droplets that have grown to large sizes and failing to detect ice crystals that have not grown large enough. The aerosol particles are sampled in normal atmospheric concentrations. and 3446. The results from this experiment indicate that droplet size can exceed the ‘‘crystal threshold’’ of 3 m when SS w 20%.m diameter was extracted with an electrical differential mobility analyzer. such as condensationfreezing. 0 counts are plotted at 0. To the ex- . these are active CCN but poor IN at temperatures above 45 C (Chen et al. 739 FIG. the number of particles exceeding the 3. For the supersaturations shown. The size range 1 to 18 m is covered with 256 channels. and particle size spectra were measured every 10 s. The CFD chamber sampling temperature was 20 C. the droplet sizes increased dramatically and consistently. 2 10 6 . the fraction was 0 to 10 5 . and a monodisperse fraction of 0. if they could reach 3 m.m threshold was 0. until other methods are developed for differentiating droplets from ice crystals. laboratory tests were performed with ammonium sulfate particles.MAY 2001 ROGERS ET AL. For convenience. Figure 16 shows this dependence for the 10-s average IN concentrations. The fraction of total aerosol particles active as ice nuclei is the ratio of IN and CN concentrations. IN activity is also a strong function of temperature. 2000). Qualifying this technique—Advantages and disadvantages The advantages of the CFD method are listed here. Ten-second average IN concentrations showing rapid increase above water saturation. Sample temperature 23 to 20 C. for these data. Below water saturation. 6. At supersaturations below 25%. In general. on average.1 on logarithmic sale. and as supersaturation increased. For our experiment. 16. a few particles 3 m were seen. the supersaturation was increased from 3% to more than 40% with respect to water. but since the temperature was approximately constant at 20 C. 104. 2000). the CCN particles were atomized from aqueous solution and then dried. in particular. 540. In order to estimate how large droplets might grow in the chamber and. FIG. Examples from this series of data are shown in Fig. useful for studying nucleation mechanisms and growth (Chen et al. Therefore. but a value of 20% is a reasonable estimate. the SS w where droplets exceed 3 m are unknown. it appears that peak SS w 20% is an upper limit for this technique.2. 15. the contribution by deposition (sorption) nucleation. Another example of CFD data was drawn from the same time period of the 20 May 1998 case to show the dependence of IN activity on supersaturation. The temperature and supersaturation are controllable and are relatively well defined. With natural CCN particles instead of these laboratory aerosols. 15 for SS w of 16% to 40%. Over a period of 25 min. not supported on a substrate but freely floating in air.

When the IN concentration and the background are both small. Jaenicke’s (1993) ‘‘remote continental’’ air has 0. although there will be large variability in the vertical and between different air mass types.0007 L 1 . and measurements are available in real time. In order to provide adequate time for particle nucleation and growth. 16) was 10 5 . depending on the temperature and supersaturation. SS) should be constant so that later analyses may be able to relate IN activity to physical and chemical properties of the aerosol. poor sensitivity for some nucleation mechanisms. 6). It would put ice crystals (containing nuclei) into a separate airstream at the outlet of the CFD. Temporal resolution 1 s is possible. This stream could feed into a variety of . this technique provides no information about the IN activity of larger particles.g. The sample can be exposed to extremely high supersaturations that are well defined up to 20%. A related question is the number of non-IN particles that are mistakenly counted because they exceed 3 m. this technique is unsuitable for measuring contact freezing nucleation and immersion-freezing. Sassen 1974). we plan to revise this practice and use preset points and automated feedback control.. In particular. spectra require much more time than is available. This might be possible with a cross-polarization–type detector (e. as a rough estimate. 6).21% of these can get past the impactors (Fig. The known disadvantages are described here..740 JOURNAL OF ATMOSPHERIC AND OCEANIC TECHNOLOGY VOLUME 18 tent that temperature and supersaturation determine the nucleation mode. leaving 0. such as a counter-flow virtual impactor. SS) conditions are fixed. Although it is possible to derive temperature and supersaturation response ‘‘spectra’’ for IN. the maximum fraction in our results for Arctic air (Fig. lacking capability for unattended operation. 54% (Fig. and of these. mechanistic studies of ice formation can be done with this technique. This is an overestimate because particles will be removed by piping upstream and downstream of the impactors. the (T. other studies have shown that IN activity generally increases with particle surface area (e. thermal gradient continuous-flow diffusion chamber was developed for airborne measurements of ice nucleating particles and has been used on several field projects. the (T.g. It is difficult to detect homogeneous freezing nucleation with this technique because of slow crystal growth rates at the colder temperatures. At present. and no sampling of particles 2 m. DeMott 1990). Turner and Radke 1973. While this seems insignificant. Another possible solution to this problem is to increase the concentration of aerosol particles by virtual impactor methods (e. Only a small fraction of these are active as ice nuclei. etc. SS) spectra throughout soundings. For example. At present. They include statistical sampling limitations. To overcome this limitation. and the vertical structure of IN concentration is measured for one set of conditions. It is twice as long as the airborne chamber to provide more growth time.13 L 1 to be detected by the OPC. above water saturation. 7. Thus. This was described for the measurements in Fig. Residence time in the airborne CFD chamber is 5 s. The chamber samples at one set of temperature and supersaturation (T. Increasing the airflow rate would improve the sampling statistics and the potential for time-resolved sampling. hence the unmeasured IN may have been 0. depending on IN concentration. short-term estimates of either will contain large uncertainties. Because nearly all particles 2 m are deliberately removed by impactors at the instrument’s inlet. do not get past the inlet impactors.. Choosing the conditions requires careful thought in order to obtain the most useful information. the sampling statistics are poor. this instrument is not suitable for unattended operation because the ice must be resurfaced approximately every 2 h. there are 61 L 1 larger than 3 m. and 0. For example.13 cm 3 particles exceeding 2 m. Although it would be interesting to have (T. Thus. a laboratory version CFD chamber has been built (Table 1). when the aircraft is making large changes in altitude. or 70 L 1 . All IN measurement techniques have a background that needs to be estimated and subtracted. 14. vertical soundings of IN can be obtained. greater flow rate would necessitate a larger chamber and/or more precise measurements of particle size. the wall temperatures are set by the operator. SS) conditions at a time. For example. Consideration should be given to the ice forming processes that one wants investigate or to the type of data being sought. ice crystals would form by deposition nucleation below water saturation. A flow-through detector that could differentiate water from ice at small sizes ( few micrometers) would be a great advantage. Similarly. This number can also be estimated from typical size distributions.g. Another device that would extend the potential applications of IN measurements is an inline large particle separator. as selected by the operator. Berezinskiy and Stepanov 1986. Sioutas et al. Any nucleation modes requiring several seconds or more will not be detected. Some improvements for future studies with this type of instrument are suggested here. the removal of particles 2 m may be a significant limitation for de- tecting ice nuclei that are active at the warmest temperatures. and its optical particle counter is used at higher gains to measure smaller particles. when TEM impactor samples are being collected. nucleation could occur through both deposition and condensation-freezing. For example. Because of typically low IN concentrations and the small sample rate ( 1 L min 1 ). with the intention of reducing the already large number of variables that are important for ice formation. Conclusions An ice. several tens of minutes are needed to obtain such spectra. The number of particles 2 m that are not sampled can be estimated from typical atmospheric aerosol size distributions. Therefore. 1994). for Jaenicke’s (1993) remote continental air.

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