Light Absorption by Carbonaceous Particles: An Investigative Review

Figures & data

FIG. 1 Calculating radiative transfer

TABLE 1 Discussions that contribute to understanding of absorption by LAC

General topic	Material	Objective of study	Sample references
Air quality	Atmospheric aerosol	Determine causes of visibility reduction and health impacts	Cartwright et al. 1955 Groblicki et al. 1981 Malm et al. 1994
Astrophysics	Soot, graphite, amorphous carbon	Identify composition of interstellar matter	Draine and Lee 1984 Sakata et al. 1995 Henning et al. 1999
Climate	Atmospheric aerosol	Estimate impact of anthropogenic activity on Earth's radiative balance	Charlson and Pilat 1969 Schneider 1972 Haywood and Shine 1995
Combustion diagnostics	Flame-generated carbon	Determine soot volume fraction with nonintrusive techniques	Santoro et al. 1983 Mountain and Mulholland 1988 Minutolo et al. 1994
Manufacturing	Carbon black	Predict paint color and rubber properties	Biscoe and Warren 1942 Heckman 1964 Medalia and Richards 1971 Mudgett and Richards 1973
Heat transfer	Flame-generated carbon	Calculate heat transfer out of flames	Dalzell and Sarofim 1969 Tien and Lee 1982 Köylü and Faeth 1994
Nuclear winter	Combustion products	Estimate climate of Earth after nuclear war	Turco et al. 1983 Penner and Molenkamp 1989 Nelson 1989
Petrology	Coal	Identify different coal types	Van Krevelen 1958 McCartney et al. 1958 Foster and Howarth 1968
Solid-state physics	Amorphous carbon	Generate thin films with precisely controlled optical properties	McKenzie et al. 1983 Smith 1984 Robertson 1987

FIG. 2 Idealized relationships between absorbing and nonabsorbing material. (a) External mixture: a heterogeneous population of internally homogeneous particles. (b) volume averaged mixture: a homogeneous population of internally homogeneous particles. (c) Heterogeneous particle composition and population. Both (b) and (c) have been called “internal mixtures”.

FIG. 3 Imaginary refractive index predicted by the dispersion model with the parameters of Lee and Tien (1981) and Dalzell and Sarofim (1969). The figure differs from that of Lee and tien because it is evaluated at 300 K instead of flame temperature. See the text (Section 4.2.2, 7.2.2, and 7.6) for caveats on the use of the dispersion model to represent flame generated carbon.

FIG. 4 Volume absorption cross section versus diameter. Refractive index is 1.56–0.47i from Dalzell and Sarofim (1969), wavelength is 550 nm. These results are often divided by the particles' material density and presented as mass absorption cross section. (We favor other refractive indices to represent pure LAC; see Section 7.)

FIG. 5 Contour plots of volume absorption cross section at a wavelength of 550 nm, as a function of (a) diameter and imaginary refractive index, assuming a real refractive index of 1.55; and (b) diameter and real refractive index, assuming an imaginary refractive index of 0.55. These refractive indices are similar to those measured for LAC (see Table 4). The calculations are for a narrow polydispersion of particles (geometric standard deviation of 1.1). Choosing a polydispersion eliminates some of the Mie “wiggles that are observed in true monodispersions but are likely never found in atmospheric aerosol.

FIG. 6 Ratio between predictions of Rayleigh-Debye-Gans aggregate theory and Mie theory for two particles of equivalent mass. Where no contours appear, ratio is constant. Assumptions: real refractive index 1.55, primary spherule diameter 25 nm, wavelength 550 nm.

TABLE 2 Direct methods of measuring absorption by particles

Method	References
Particles collected on filter
Most operate on similar principle
Integrating plate	Lin et al. 1973; Horvath 1997
Integrating sandwich	Clarke et al. 1987
Laser transmission	Rosen and Novakov 1983; Gundel et al. 1984
Aethalometer	Hansen et al. 1984; Weingartner et al. 2003
Particle soot absorption photometer (PSAP)	Weiss and Waggoner 1984; Bond et al. 1999
Multi-angle absorption photometry (MAAP)	Petzold et al. 2005
Integrating sphere	Fischer 1970; Heintzenberg and Meszaros 1985; Hitzenberger 1996
Particles suspended in air
Photoacoustic	Terhune and Anderson 1977; Japar and Killinger 1979; Foot 1979; Roessler and Faxvog 1979; Arnott et al. 1997
Difference (extinction minus scattering)	Lewis and Dzubay 1986; Horvath 1993b
Flux divergence	Pilewskie et al. 2003

TABLE 3 Correction factors for absorbing particles collected on filter

Filter type	Absorption correction	Scattering correction	Particle orientation	Notes/Citation
Zefluor	2.43 ± 0.13	—	Toward detector	No loading correction apparent.
				Szkarlat and Japar 1981
Zefluor	1.3 ± 0.14	—	Toward lamp	Szkarlat and Japar 1981
Pallflex E70-2075W (PSAP)	2.2 ± 0.2 ^a	0.04 ± 0.04	Toward detector	Value given is for lightly loaded filter; loading correction is supplied by manufacturer.
				Bond et al. 1999
Nuclepore (Integrating Plate)	1.23 ± 0.13	0.09 ± 0.02	Toward detector	No filter orientation effect observed. ^b No loading correction determined.
				Bond et al. 1999
Quartz 2500 Q20F (Aethalometer AE-30)	2.14 ± 0.6	0.007 ± 0.004	Toward lamp	Averaged data for 450 and 660 nm; higher correction for coated aerosol.
				Weingartner et al. 2003
Quartz and Millipore (Laser transmission)	3.5	—	Toward detector	Combined Sadler et al. 1981 comparison of laser transmission and IP with Bond et al. 1999 calibration of IP

TABLE 4 Published values of LAC refractive index

Reference	Cited by	Real (n)	Imag. (k)	Material
Measurements
Coal
McCartney et al. 1965	TW	1.7–2.0	0.25–0.5	Coal of various ranks
Gilbert 1962		1.8–2.05	0–0.8	Coal from specific mines
Carbon particles
1 Batten 1985	H	1.20–1.35	0.1–0.22	Kerosene soot
2 Chang and Charalampopoulos 1990		1.77	0.63	Premixed propane-oxygen, φ = 1.8
3 Chippett and Gray 1978		1.9	0.35	Smoke generator
4 Dalzell and Sarofim 1969	H	1.56	0.47	Average of coal and propane soots
5 Erickson et al. 1964		1.4	1.0	Benzene-air flame
6 Habib and Vervisch 1988		1.3	0.3	Premixed flames, various fuels
7 Janzen 1979	FMK	2.0	1.0	Carbon black
8 Lee and Tien 1981	CHH	1.95	0.48	Polystyrene and plexiglas flames
9 Mullins and Williams 1987		1.88–1.93	0.39–0.45	Toluene, propane, n-heptane
10 Marley et al. 2001		1.87	0.56	Soot from candle flame
11 Marley et al. 2001		1.68	0.56	Diesel soot
12 Pluchino et al. 1980	H, CHH	1.7–1.8	0.6–0.8	Carbon black, single particle
13 Powell and Zinn 1983	CHH	1.108	0.075	Flaming polymeric materials
14 Senftleben and Benedict 1918	TW	1.9	0.65	Arc-lamp soot
15 Stagg and Charalampopoulos 1993		1.52	0.36	Propane flame
16 Wu et al. 1997		1.58	0.51	Turbulent diffusion flames
Graphite
Egan 1982	CHH	1.67–2.05	0.01–0.7	1st Intercomparison work
Taft and Phillip 1965		2.58	1.44	Graphite (normal incidence)
Tsu et al. 1978	CHH	2.05–2.75	0.66–1.46	3 grades of graphite
17 Greenaway et al. 1969	MR	2.72/1.46	1.34/0.0	Graphite (normal/parallel incidence)
Stagg and Charalampopoulos 1993		2.65	1.39	Pyrolytic graphite
Derived Values
Original source	Cited by	Real (n)	Imag. (k)	Notes
Dalzell and Sarofim 1969	MR	1.84	0.46	Adjusted for void fraction
Janzen 1979	H, FMK	1.25	0.25	Hypothesized for 75% air, 25% soot
Janzen 1979	H, FMK	1.5	0.5	Hypothesized for 50% air, 50% soot
Ergun and McCartney 1960 ^a	MR	2.02	0.56	Interpolated to H/C ratio of carbon black
Secondary References
Citing reference	Cited by	Real (n)	Imag. (k)	Original source
Ackermann and Toon 1981	H	1.94	0.66	Senftleben and Benedict 1918
Bergstrom 1972	FMK, CHH	1.95	0.66	Senftleben and Benedict 1918
Bergstrom 1973	H	2.0	0.66	Senftleben and Benedict 1918
Twitty and Weinman 1971	FMK	1.80	0.8	See this tabulation
Hess and Herd 1993	FMK	2.0	1.0	Janzen 1979
Hänel 1987	H	1.9	1.0	Value not found in Hänel paper
Janzen 1979	CHH	1.4–2.35	0.46–1.42	Values not found in this paper
Jaenicke 1988	H, CHH	1.75	0.44	Twitty and Weinman
Kattawar and Heard 1976	H	1.95	0.66	Senftleben and Benedict 1918
Ouimette and Flagan 1982	H	1.56	0.47	Dalzell and Sarofim 1969
Roessler and Faxvog 1980	H	1.96	0.66	Senftleben and Benedict 1918
Roessler and Faxvog 1980	CHH	1.75	0.5	Value not found in cited paper
Roessler and Faxvog 1980	H	2.0	0.66	Value not found in cited paper
Shettle and Fenn 1979	H	1.76	0.45	Average of Twitty and Weinman 1971
“various textbooks”	H	2.0	1.0	Probably from Janzen 1979

FIG. 7 Refractive indices from Table 4. Numbers on each data point refer to reference numbers in the table. Curve marked “void fraction” assumes that LAC has a single refractive index and that variation can be expressed by the Bruggeman effective-medium theory. Curve marked “graphitization" shows variation in refractive index of carbon containing different sp2-bond content. See text in Section 7.2.3 for further explanation.

TABLE 5 Refractive indices that lie along the upper void-fraction line in Figure 7, for 550 μm

n	k
1.75	0.63
1.80	0.67
1.85	0.71
1.90	0.75
1.95	0.79

FIG. 8 Comparison of mass absorption cross sections tabulated (a) in previsous reviews, showing large variability, and (b) in this review for near-source measurements, with much smaller variability. Legend in Figure 8a: (1) Traceable to value reported. (2) Not traceable to value reported.

TABLE 6 Published values of LAC refractive index: original inferences, derived values and secondary references

		Value	Wave-length		Adjusted		Normalization/
Citation		(m^2/g)	(nm)	Adjust-ments	to 550 nm	Measurement	Comments on fuel
Measurements
Diesel engines—direct
Truex and Anderson, 1979	H,L	17	514	1	15.9	Photoacoustic	None
Japar and Szkarlat, 1981		8.9	514.5	1	8.3	Photoacoustic	Mass after extraction
Schnaiter et al. 2003		6.6 ± 0.4	550	—	6.6	Difference (ext-scat)	None
Scherrer et al. 1980		9.0	550	2	7.4	IP/Nuclepore	Non-volatile mass
Szkarlat and Japar, 1981	H	8.28 ± 0.23	514	1	7.7	Photoacoustic	Soxhlet extraction
Diesel engines—traffic tunnels
Japar et al. 1981		8.0 ± 0.4	500	1	7.3	Calibrated IP	Extractable in organic solvent
Szkarlat and Japar, 1983	H	10.9	500	1,3	8.3	Calibrated IP	Mass after extraction
Other combustion aerosol
Bruce et al. 1991		4.55	488	1	4.0	Photoacoustic	None
Colbeck et al. 1989		8.1	632	1	9.3	Ext minus scat	95% “elemental carbon”
Colbeck et al. 1997		7.5	632	1	8.6	Ext minus scat	None; C/H ratio 5 molar
Gundel et al. 1984	L	25.4	633	1, 4	8.4	Laser transmission	Solvent extraction
Japar & Killinger, 1979		1.5	600	1	1.6	Photoacoustic	Mass after extraction
Mullins & Williams, 1984		4.1 ± 0.1	450	1, 5, 6	5.8	Not identified	None; C/H ratio 6–9 molar
Marley et al. 2001		10.5	550	7	See note	Integrating sphere	None
Mulholland & Choi, 1998		6.4 ± 0.5	633	1	7.4	Difference (ext-scat)	None
Patterson et al. 1991		5.3 ± 0.7	633	1	6.1	Difference (ext-scat)	None
Roessler & Faxvog, 1979	L	8.3 ± 0.9	514.5	1	7.8	Photoacoustic	None
Röhl et al. 1982		11.9	600	1, 8	7.9	Photoac. on filter	None
Sheridan et al. 2005		7.5 ± 1.2	550	1	7.5	Difference (ext-scat)	Thermal; should be mostly EC
Carbon black
Ballach et al. 2001		6.5	550	—	6.5	Integrating sphere	None
Donoian & Medalia, 1967 ^a		9.62	550	5	6.9	Difference (ext-scat)	None
Clarke and Noone, 1985	H	6.6–8	550	8	7.3	IP calibration curve	None
Spark discharge
Ballach et al. 2001		2.9 ± 0.1	550	a	2.9	Integrating sphere	None
Schnaiter et al. 2003		2.9 ± 0.5	550	—	2.9	Ext minus scat	None
Ambient—fine
Adams et al. 1990		10	514	1	9.3	Photoacoustic	Thermal-optical after extraction
Edwards et al. 1983	L	7–12	550			IP/Nuclepore	Thermal EC
Groblicki et al. 1981 ^b	L, H	11.8	550			IP/Nuclepore	Slope vs EC, SSA∼ 0.67
Japar et al. 1986	L	11–12	650			IP/Nuclepore	Thermal-optical
Liousse et al. 1993		5	Broadband			Aged	Thermal (presumably
”		20	Broadband			Fresh	Cachier method)
Ambient—coarse
Groblicki et al. 1981 ^c	H	3.8	550
Calculations						Comments
Chylek et al. 1981	H	5	514			No voids
Chylek et al. 1981	L	12.5	514			Value of 12.5 does not appear in this paper
Jennings and Pinnick, 1980	L	3.5–8.6				Mie, 2.0–1.0 i, particles 0.35–1.06μ m
Nelson, 1989	L	8–10	550			Fractal, m = 1.75–0.5 i and 2.0–1.0 i
Roessler, 1984	H	5.0	570			Small-sphere limit, m = 2-1i, density 2 g/cm3
Rosen and Hansen, 1984	L	8.3–18.1	500			Spherical, externally mixed, or internally mixed with organic and/or sulfate in observed ratios
Secondary references						Original source
Clarke, 1989	H	9.68				Donoian and Medalia, 1967
Heintzenberg, 1982	L	9.68				Donoian and Medalia, 1967
Clarke et al. 1987	L	9.68				Donoian and Medalia, 1967
Japar et al. 1984		9.8^c				Szkarlat and Japar, 1981; Szkarlat and Japar, 1983
Patterson et al. 1986	L	6.75				Szkarlat and Japar, 1981
Waggoner et al. 1981	L	5–11				Denver Brown Cloud (perhaps Groblicki et al. 1981)
References not available to us
Marshall et al. 1986	H	6.7				Reference not given by Horvath
Hitzenberg, 1990	L	2–12				Conference proceedings
Kreiner, 1985	H	6.6				Ph.D. thesis
Adjustments: (1) Adjusted to 550 nm, assuming that absorption is inversely proportional to wavelength. (2) Corrected for enhancement by Nuclepore filter according to Table 3. (3) Used 9.1 m^2/g (authors' regression of absorption on elemental carbon content) instead of authors' value, which was designed to estimate optical properties of diesel particulate emissions alone and contained higher uncertainty. (4) Corrected for enhancement by quartz filter according to Table 3. (5) Corrected for suspension in liquid medium, which increases absorption cross section relative to suspension in air. (6) Adjusted to log-base-e from log-base-10. (7) Integrating sphere used without calibration; correction factor unknown. (8) Authors used model to correct for filter effects, and we use the corrected value.
Notes:

TABLE 7 Measured values of single-scattering alberdo from fresh combustion aerosol

Reference	Wavelength (nm)	w0	Source
Roessler and Faxvog, 1980	514.5	0.15 ± 0.05	Acetylene smoke
Scherrer, 1981	535–550	0.17 ± 0.05	Diesel engine at several speeds
Colbeck et al. 1989	632	0.28–0.25	LPG combustion
Koylu, 1994	514.5	0.18–0.29	Turbulent diffusion flames: acetylene, propylene, ethylene, propane
Mulholland, 1998	633	0.19–0.25	Laminar & turbulent acetylene & ethylene flames
Schnaiter et al. 2003	550	0.20 ± 0.01	diesel engine

FIG. 9 Mass absorption cross sections m²/g for fresh LAC: measured values from Figure 8(b) (shaded region, with central estimate marked by a thick line), and calculated values using the best guess of refractive index for fully-graphitized carbon; see Figure 7. Central curve shows “void-fraction” line in Figure 7 (approximately 1.8–0.74i); higher and lower curves are similar “void-fraction” lines assuming that pure LAC has refractive indices of 2 − 1i and 1.96 − 0.66i. The latter two values are not expected to represent atmospheric LAC, as discussed in text. Assumed density is 1.8 g /cm³.

TABLE 8 Atmospheric field programs that have measured quantities relevant to LAC or absorption

			Measurement
Date	Program	Location	Method	Reference	Notes
Early Radiation Measurements—not specific to LAC
1946, 1960's	British Met Office	London, UK	[1]	Waldram, 1945; Roach, 1961; Robinson, 1970	Divergence technique—found large heating rates ∼ 20°/day presumably due to LAC
1970	CAENEX	Russian Desert	[1] spectral	Kondratyev et al. 1973; 1979	First spectral flux divergence to estimate aerosol absorption; showed hematite absorption
1972	GAARS	Southwest US	[1]	Grams et al. 1972	Flux divergence technique to estimate absorption; (SSA = 0.9) over the S.W. US desert
1976	Sutro Tower	San Francisco, CA	[1]	Russell et al. 1979; 1984	Flux divergence from tower measurements; (SSA = 0.9) near SF
1983	AGASP-1	Arctic	[7], [1]	Hansen and Rosen, 1984; Bodhaine et al. 1984; Ackerman and Valero, 1984	measured absorption by LAC in Arctic Haze
Early LAC Measurements—no absorption
1970	ACHEX	Los Angeles, CA	[3]	Hidy et al. 1980	First use of thermal method
1978	Denver Brown Cloud	Denver, CO	[3, 6]	Groblicki et al. 1981, Wolff et al. 1981	Established LAC as cause of the Denver Brown Cloud
1990–2002: Climate-Related Aerosol Field Programs
1991	Kuwait Oil Fires	Kuwait	[1]	Pilewskie and Valero, 1992; Weiss and Hobbs, 1992	Measured large optical depths with high heating rates
1995	ACE-I	Tasmania	[6]	Quinn et al. 1998 ACE I special issue	Very little absorption
1996	NFRAQS	Colorado	−[9]	Moosmuller et al. 1998	Photoacoustic technique
1996	TARFOX	North Atlantic	[1]	Novakov et al. 1997; Hignett et al. 1999, Russell et al. 1999; Bergstrom et al. 2002	Measured absorption from NE US (SSA ∼ 0.85)
1996	ARACHNE-96	Eastern Mediterranean	[6]	Formenti et al. 2001	Measured absorption above Negev Desert (SSA ∼ 0.89–0.94)
1997	ACE II	Azores	[6]	Russell and Heintzenberg, 2000 Tellus special issue	Measured absorption from Southwest Europe
1998	LACE-98	Germany	[1]	Ansmann et al. 2002 Special reprint issue JGR	Reported mean refractive index
1998	MINT	Germany	[several]	Wex et al. 2002
1998	STAAARTE-MED	Mediterranean	[6]	Formenti et al. 2002	SSA est 0.89
1999	INDOEX	Indian Ocean	[6, 2]	Mayol-Bracero et al. 2002b Quinn et al. 2002	SSA est 0.9; MAC 8.1
2001	MINOS	Crete	[6]	Sciare et al. 2003	SSA est 0.87, MAC ∼ 7
2001	ACE Asia	East Asia	[several]	Huebert et al. 2003, Bergstrom et al. 2004 JGR special issue	SSA range 0.88 for bc, 0.95 for dust Wide range of MAC's reported
2000–2003	APEX	Japan, Korea, China	[6]	Nakajima et al. 2003	SSA varies from 0.8 to 0.98
2002	CLAMS	North Atlantic	[6]	Magi et al. in press	Preliminary results SSA = 0.9
2002	NEAQS	North Atlantic	[6]	Quinn and Bates, 2003	SSA est 0.95
2003	ARM Aerosol IOP	Oklahoma	[several]	Ferrare et al. in preparation
1990–2002: Biomass burning
1992	SAFARI 92	South Africa		Andreae et al. 1996
1993	SCAR-A	US	[2]	Soulen et al. 2000
1994	SCAR-C	US?	[2]	Martins et al. 1996
1995	SCAR-B	Brazil	[several]	Kaufman et al. 1998, Reid et al. 1998, Martins et al. 1998	Compared several methods
1997	ZIBBEE–97	Africa	[2]	Eck et al. 2001
1998	LBA	Brazil	[7]	Artaxo et al. 2002	Found SSA = 0.83–0.92
1999	BIBLE-B	East Asia		Liley et al. 2002
2000	SAFARI 2000	South Africa	[1, 6]	Swap et al. 2003; Pilewskie et al. 2003, Bergstrom et al. 2003; Eck et al. 2004	Several methods used for absorption, no mass measurements
Continuous measurements
	UK Smoke Network	184 sites in UK	Filter reflectance	Edwards et al. 1983
	CMDL	5 baseline; 4 regional	[6]	Sheridan and Ogren, 1999	Remote locations
	IMPROVE	Continental US	[6]	Malm et al. 1994	Provides maps of BC
	GAW	22 sites worldwide		Lavanchy et al. 1999 GAW home page http://rea.ei.jrc.it/netshare/wilson/WDCA/	Jungfraujoch
	AERONET	∼ 200worldwide	[2]	Holben et al. 1998, Dubovik et al. 2002	Routinely publishes SSA results
	TOMS (satellite)	Global coverage	[2]	Torres et al. 1998	Used extensively to show existence of absorbing particles
	MODIS (satellite)	Global coverage	[2]	Kaufman et al. 2002, Hsu et al. 2004	Publishes optical depth and size information Multi-component methods
	AVHRR (satellite)	Global coverage	[2]	Husar et al. 1997, Christopher et al. 1996	Broad band measurement
	SeaWiFS	Global coverage	[2]	Higurashi and Nakajima, 2002, Kahn et al. 2001	Multi-component methods
	MISR	Global coverage	[2]		Multi-Angle retrieval
Measurement methods: [1] Flux divergence from radiometer measurements at two levels in the atmosphere; [2] Inversion of sky or satellite radiance; [3] Thermal technique; [4] Integrating sphere; [5] Integrating plate; [6] PSAP; [7] Aethalometer; [8] Laser integrating plate, [9] photoacoustic

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