Tandem Measurements of Aerosol Properties—A Review of Mobility Techniques with Extensions

Figures & data

TABLE 1 Instrumentation

Instrument	Measured Property	Reference
DMA	Z = neB =	(Knutson and Whitby 1975; Liu and Pui 1974)
APM	m	(Ehara et al. 1996)
ATOFMS	d a ^v; single particle composition	(Gard et al. 1997)
CCN	Activation when exposed to slightly supersaturated water vapor	(Delene and Deshler 2000; Hudson 1989; Roberts and Nenes 2005)
MALS	Light scattering intensity vs. polar and azimuthal angles	(Dick and McMurry 2007; Dick et al. 1998; Wyatt et al. 1988)
Impactor: MOUDI, LPI	d a ^atm	(Hering et al. 1977; Hering and Friedlander 1979; Marple et al. 1991)
OPCs	Integrated light scattering intensity	(Cooke and Kerker 1975; Heyder and Gebhart 1979; Liu and Daum 2000; Szymanski and Liu 1986)
TEM	Morphology, D f ; v	(Park et al. 2004a, 2004b)

TABLE 2 List of acronyms

AMS:	Aerodyne Aerosol Mass Spectrometer
APM:	Aerosol Particle Mass Analyzer
ATOFMS:	Aerosol Time-of-Flight Mass Spectrometer
CCN:	Cloud Condensation Nucleus Concentration
DMA:	Differential Mobility Analyzer
LPI:	Low Pressure Impactor
MALS:	Multiangle Light Scattering
MOUDI:	Microorifice Uniform Deposit Impactor
NAA:	Neutron Activation Analysis
OPCs:	Optical Particle Counters
TDCIMS:	Thermal Desorption Chemical Ionization Mass Spectrometer
TDMA	Tandem Differential Mobility Analyzer
HTDMA:	Hygroscopicity Tandem Differential Mobility Analyzer
RTDMA:	Reaction Tandem Differential Mobility Analyzer
VDMA:	Volatility Tandem Differential Mobility Analyzer
TEM:	Transmission Electron Microscope

FIG. 1 Schematic of aerosol tandem measurements discussed in this article. Particles of a given mobility diameter are selected by a DMA from the sampled aerosol. Further information about aerosol physicochemical properties is obtained one or more additional measurement methods in series. An alternative involves using a TDMA to processes the aerosol prior to measuring additional properties. (Figure provided in color online.)

TABLE 3 Measurements of transport properties

Transport Property	Instruments	Reference
Electrical Mobility: Z = n p eB	DMA	(Knutson and Whitby 1975; Liu and Pui 1974)
Diffusivity: D = kTB	DMA	(Hinds 1999)
Sedimentation Speed: v s = mgB	DMA + APM	(Hinds 1999)
Dynamic Shape Factor: χ =	DMA + TEM	(Kasper 1982; Park et al. 2004c)
Aerodynamic Diameter: (d a ^atm)^2 C c (d a ^atm) =	DMA + APM	(McMurry et al. 2002); Figure 2
Vacuum aerodynamic diameter vs. mobility diameter d a ^v = ; d ve ^2 C(d ve ) =	DMA + AMS DMA + ATOFMS	Figure 2

TABLE 4 Measurements of particle physical/Chemical properties: DMA systems

Properties	Instruments	References
d pae for agglomerates or nanowires	DMA	(Jung et al. 2004; Kim and Zachariah 2005; Park et al. 2004c; Rogak and Flagan 1993)
v or d ve for agglomerates	DMA + TEM	(Lall and Friedlander 2006; Lall et al. 2008; Lall et al. 2006)
Length of Nanowires (Nanotubes)	DMA + TEM	(Kim et al. 2007; Kim and Zachariah 2005, 2006)
Bright/dark particle ratio & mixing state; d m vs. optical size; water uptake	DMA + OPC	(Heintzenberg et al. 2002; Hering and McMurry 1991; Covert et al. 1990)
		(Sorooshian et al. 2008)
		Figure 3
		Figure 4
Mixing state & morphology	DMA + OPC + TEM (OPC & TEM in parallel)	(Heintzenberg et al. 2004; Okada and Heintzenberg 2003)
n	DMA + MALS	(Dick and McMurry 2007)
Shape (spherical vs. nonspherical)	DMA + MALS	(Dick et al. 1998; Sachweh et al. 1995)
ρ effective ; d m vs. m; D f ; morphology	DMA + APM DMA + Impactor DMA + TEM DMA + Mass Spectrometer Ion Mobility Spectrometer (IMS) + Mass Spectrometer	(de la Mora et al. 2003; Fernández de la Mora et al. 1998; Geller et al. 2006; Hering and Stolzenburg 1995; Kelly and McMurry 1992; Maricq and Xu 2004; McMurry et al. 2002; Olfert et al. 2007; Park et al. 2003a; Skillas et al. 1998; Slowik et al. 2004; Stein et al. 1994; Wyttenbach and Bowers 2007); Figure 5
ρ particle	DMA + APM + TEM	(Park et al. 2004c; Park et al. 2004d)
dc m /d log d m ; c m	DMA (SMPS) + APM	(Park et al. 2003b)
Elemental composition of ultrafine particles	DMA + NAA	(Neville et al. 1983)
Nanoparticle composition	DMA + TDCIMS	(Smith et al. 2008; Smith et al. 2005; Smith et al. 2004; Voisin et al. 2003)
Composition of individual mobility-classified particles	DMA + APM + ATOFMS (APM & ATOFMS in parallel)	Figure 6 Figure 7
Size-dependent cloud activation efficiencies	DMA + CCN	(Bilde and Svenningsson 2004; Corrigan and Novakov 1999; Cruz and Pandis 1997; Petters et al. 2007; Bilde and Svenningsson 2004; Corrigan and Novakov 1999; Cruz and Pandis 1997; Petters et al. 2007)

TABLE 5 Measurements of particle physical/Chemical Properties: TDMA systems

Properties	Instruments	References
Water uptake; mixing state	HTDMA	(Liu et al. 1978; McMurry and Stolzenburg 1989; Swietlicki et al. 2008)
Vapor pressure/volatility; mixing state	VTDMA	(Orsini et al. 1999; Philippin et al. 2004; Rader et al. 1987; Riipinen et al. 2007; Sakurai et al. 2003b; Tao and McMurry 1989; Villani et al. 2007)
Reactivity	RTDMA	(Gupta et al. 1995; Holm and Roberts 2007; Liao et al. 2006; Liao and Roberts 2006; McMurry et al. 1983; Zhang et al. 2008a)
Sintering or fusion of agglomerates	TDMA	(Cho et al. 2007; Nakaso et al. 2002)
Morphology & elemental composition-dependent water uptake	HTDMA + TEM	(McMurry et al. 1996)
Volatile mass fraction vs. T	VTDMA + APM	(Sakurai et al. 2003a)
Effective density vs. RH	HTDMA + APM	(Zhang et al. 2008b); Figure 8
Density vs. extent of volatilization; Density of evaporated mass	VTDMA + APM	Discussion
Dependence of composition on volatilization	VTDMA + ATOFMS	Figures 9 and 10
Cloud Activation of Coated Particles	RTDMA + CCN	(Abbatt et al. 2005; Cruz and Pandis 1998)

FIG. 2 DMA-ATOFMS measurements of vacuum aerodynamic diameter d _a ^v vs. mobility diameter d _m for polystyrene latex (PSL) spheres and for flame soot agglomerates. The value of the slope of the linear relationship between d _a ^v and d _m for the spherical PSL particles (1.06) is close to the PSL density (1.054 g cm^{− 3}), as expected from theory (DeCarlo et al. 2005). Also shown are data for flame soot obtained using a DMA and an Aerodyne AMS (Slowik et al. 2004) (the “type I” particles in that study). The ATOFMS data shown here apply to lean combustion conditions. Also shown are calculated aerodynamic diameters at atmospheric pressure for the soot measured in this study.

FIG. 3 DMA-OPC measurements of count frequency vs. light scattering intensity for 450 nm mobility diameter particles. Data are shown for measurements in urban St. Louis (July 8 and 9, 2001) and for laboratory measurements of diesel exhaust aerosol. Note that the optical signature of the diesel exhaust particles is similar to that for the “dark” particles (i.e., those that scattered relatively little light and therefore produced a small voltage pulse) that were observed in St. Louis. On these two days, most of the particles in St. Louis were “bright,” and likely consisted of sulfate/organic mixtures.

FIG. 4 DMA-OPC measurements of measured light scattering intensity vs. mobility diameter for polystyrene spheres (PSL), dioctyl sebacate (DOS) oil droplets, and diesel exhaust soot. OPC measurements were done using a PMS Lasair 1002. The diesel soot was measured in the exhaust of a John Deere 4045 engine operating with 400 ppm sulfur fuel at 50% load (Wang 2002).

FIG. 5 DMA-APM measurements of effective density for particles with nominal mobility size of 100 and 300 nm. The data from the 2002 study in Atlanta are compared with previous measurements in Atlanta and Los Angeles using the same measurement method. Laboratory measurements for diesel exhaust particles are also shown. We have categorized the effective densities as “low” (< 1 g/cm³), “intermediate” (1.0–2.0 g/cm³), and “high” (> 2.0 g/cm³).

FIG. 6 DMA-ATOFMS measurements of 500 nm mobility diameter particles from the exhaust of a Catepillar C-12 heavy duty diesel engine. Note that when classified according to vacuum aerodynamic diameter, d _a ^v , these particles separate cleanly into two groups with distinctly different compositions. Those with smaller d _a ^v consist primarily of carbon soot. Those with larger d _a ^v consist primarily of sulfates and metals. (Figure provided in color online.)

FIG. 7 DMA-APM-ATOFMS measurements of artifacts that occur when particles consisting of sulfuric acid/ammonium sulfate internal mixtures flow through the APM. Plotted is the sum of mass 59 plus 99 peaks vs. the sulfuric acid mole fraction in laboratory calibration particles of 300 nm mobility size. Separate measurements on atomized ferrofluid used in the APM rotating seals show that those peaks are associated with this ferrofluid. The artifact arises when a basic gas, volatilized from the ferrofluid, is absorbed by the acidic particles.

FIG. 8 HTDMA-APM measurements of effective densities of atmospheric particles measured in urban Atlanta (2002) along with thermodynamic predictions for pure ammonium sulfate and sulfuric acid particles as a function of relative humidity.

FIG. 9 VTDMA-ATOFMS measurements of comparison of averaged (a) positive and (b) negative ion mass spectra for “more volatile” and “less volatile” 300 nm mobility diameter particles in urban Atlanta on August 20, 2002.

FIG. 10 VTDMA-ATOFMS measurements of average mass spectra for the four types of “less volatile” 300 nm mobility diameter particles in urban Atlanta on August 20, 2002: (a) “Soot or EC” (14%), (b) “PAH” (22%), (c) “K, sulfate, CN compounds, and organics” (57%), and (d) “oxidized metals” (7%).

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