1. Introduction
The inherent optical properties (IOPs) of particles suspended in natural waters are of interest in several areas of marine science: sediment properties and transport [
1
S. G. Ackleson, “Optical determinations of suspended sediment dynamics in western Long Island Sound and the Connecticut River plume,” J. Geophys. Res.
111(C7), C07009 (2006), doi:. [CrossRef]
]; marine photosynthesis [
2
N. Hoepffner and S. Sathyendranath, “Determination of major groups of phytoplankton pigments from absorption spectra of total particulate matter,” J. Geophys. Res.
98(C12), 22789–22803 (1993). [CrossRef]
]; and remote sensing of ocean color [
3H. R. Gordon, and A. Y. Morel, Remote Assessment of Ocean Color for Interpretation of Satellite Visible Imagery: A Review (Springer-Verlag, 1983).
]). The IOPs include the absorption coefficient (
a), the scattering coefficient (
b), the extinction coefficient
c =
a + b, the volume scattering function
β(Θ) (Θ is the scattering angle), and the backscattering coefficient (
bb
). The extinction coefficient is particularly important in sediment studies, the spectral absorption coefficient in photosynthesis, and the backscattering coefficient in remote sensing (water-leaving radiance ∝
bb
/
a).
For many years, the interpretation of measurements of the IOPs of particles suspended in natural waters (in particular the estimation of their refractive indices) has usually employed the assumption that the particles are spherically symmetric [
4
D. Stramski, E. Boss, D. Bogucki, and K. J. Voss, “The role of seawater constituents in light backscattering in the ocean,” Prog. Oceanogr.
61(1), 27–56 (2004). [CrossRef]
]. The development of electromagnetic scattering codes for computing the scattering from particles with more complex shapes has stimulated interest in the influence of particle shape on the IOPs [
5
H. R. Gordon and T. Du, “Light scattering by nonspherical particles: application to coccoliths detached from Emiliania huxleyi
,” Limnol. Oceanogr.
46(6), 1438–1454 (2001). [CrossRef]
–
7
W. R. Clavano, E. Boss, and L. Karp-Boss, “Inherent Optical Properties of Non-Spherical Marine-Like Particles - From Theory to Observations,” Oceanogr. Mar. Biol.
45, 1–38 (2007). [CrossRef]
]. Gordon and Du [
5
H. R. Gordon and T. Du, “Light scattering by nonspherical particles: application to coccoliths detached from Emiliania huxleyi
,” Limnol. Oceanogr.
46(6), 1438–1454 (2001). [CrossRef]
] and Gordon et al. [
8
H. R. Gordon, T. J. Smyth, W. M. Balch, G. C. Boynton, and G. A. Tarran, “Light scattering by coccoliths detached from Emiliania huxleyi
,” Appl. Opt.
48(31), 6059–6073 (2009). [CrossRef]
[PubMed]
] showed that a complex shape was required to reproduce the spectral variation and absolute magnitude of the backscattering cross section of coccoliths detached from the coccolithophore
E. huxleyi. Gordon [
9
H. R. Gordon, “Backscattering of light from disklike particles: is fine-scale structure or gross morphology more important?” Appl. Opt.
45(27), 7166–7173 (2006). [CrossRef]
[PubMed]
,
10
H. R. Gordon, “Backscattering of light from disk-like particles with aperiodic angular fine structure,” Opt. Express
15(25), 16424–16430 (2007). [CrossRef]
[PubMed]
] showed that small-scale structures (size ≤
λ/4) had little influence on the backscattering of disk-like particles. Clavano et al. [
7
W. R. Clavano, E. Boss, and L. Karp-Boss, “Inherent Optical Properties of Non-Spherical Marine-Like Particles - From Theory to Observations,” Oceanogr. Mar. Biol.
45, 1–38 (2007). [CrossRef]
] carried out a comprehensive study of scattering by spheroid-shaped particles (ellipses of revolution) in random orientation with refractive indices characteristic of particles suspended in water. They showed that the computed IOPs for such particles deviated significantly from those computed for spheres having the same volume and refractive index. The deviations increased as the aspect ratio of the spheroids increased. They also reported data suggesting that the most frequent aspect ratio of living marine particles was ~5.
In this work, I consider in detail the dependence of IOPs on aspect ratio. Rather than spheroids, I use homogeneous and structured cylinders as the study particle, but make comparisons with similarly-sized spheroids. I consider refractive indices that are within the range expected for marine particles. I also assume throughout that the particles are in random orientation; however, if the particles have a preferred orientation the influence on the IOPs will be large, particularly on backscattering. Generally, particles embedded in an isotropic turbulent flow, will have a random orientation. In contrast, if they are embedded in non-isotropic turbulence [
11
L.-X. Zhang, J.-Z. Lin, and T. L. Chan, “Orientation distribution of cylindrical particles suspended in turbulent pipe flow,” Phys. Fluids
17(9), 093105 (2005). [CrossRef]
] or in a shear flow, there will be a tendency for the particles to align with the flow. This tendency will be particularly important in aligning particles with large aspect ratios, e.g., diatom chains [
12
L. Karp-Boss and P. A. Jumars, “Motion of diatom chains in steady shear flow,” Limnol. Oceanogr.
43(8), 1767–1773 (1998). [CrossRef]
]. In the absence of data concerning particle orientation in the natural waters, we have no basis on which to assume any orientation other than random.
As the principal focus is to study the influence of aspect ratio on the IOPs, the particle diameters are of necessity limited by the storage requirements of the computer code used in the computations. The largest particle that could be examined has a volume-equivalent spherical diameter of ~3.6 μm, and an aspect ratio of 10.
The principal result of the study is that the extinction, scattering, and absorption efficiencies, as well as the scattering phase function, β(Θ)/b, and the backscattering probability, bb
/b, become nearly independent of the aspect ratio (length/diameter) when it becomes greater than ~3−5. This implies that the IOPs of longer cylindrical particles can be inferred from those of particles with aspect ratios in this range.
I begin by reviewing scattering and absorption concepts for finite and infinite cylinders. Next I provide computed absorption and extinction efficiencies and backscattering probability of homogeneous and structured cylinders as a function of their diameter, refractive index, and aspect ratio. These are then compared to those of equal-volume spheres, showing that the spherical assumption is particularly poor at even moderate aspect ratios. Finally, I briefly compare scattering by cylinders and spheroids.
3. Cylinders examined in the present work
The cylinders studied in this work are shown schematically in
Fig. 1
. The upper cylinder is homogeneous with refractive index
mr
−
imi
, relative to water. The lower cylinder (coated) has the same outer diameter (
D) as the homogeneous cylinder, however the core diameter is
D/2 and the core index is
mr
− 4
imi
. The index of the outer layer is
mr
− 0
i, so this simulates a situation in which the mass of absorbing material (or the number of absorbing molecules) is the same in the upper and lower cylinder, and allows simulation of the influence of the distribution of absorbing pigments in cylindrically shaped particles. In marine optics, there are two phenomena that are referred to as the “package effect.” The first is the difference in absorption between equal quantities of absorbing material in solution or in particles suspended in the same volume [
16
L. N. M. Duysens, “The flattening of the absorption spectrum of suspensions, as compared to that of solutions,” Biochim. Biophys. Acta
19(1), 1–12 (1956). [CrossRef]
[PubMed]
–
18
A. Bricaud and A. Morel, “Light attenuation and scattering by phytoplanktonic cells: a theoretical modeling,” Appl. Opt.
25(4), 571–580 (1986). [CrossRef]
[PubMed]
]. The second is the difference in absorption between cells in which the absorbing molecules are uniformly distributed within the cell walls, and cells in which the absorbing molecules are packaged in smaller structures, e.g., chloroplasts [
6
A. Quirantes and S. Bernard, “Light scattering methods for modeling algal particles as a collection of coated and/or nonspherical scatterers,” J. Quant. Spectrosc. Radiat. Transf.
100(1-3), 315–324 (2006). [CrossRef]
,
19
J. R. V. Zaneveld and J. C. Kitchen, “The variation of inherent optical properties of phytoplankton near an absorption peak as determined by various models of cell structure,” J. Geophys. Res.
100(C7), 13,309–13,320 (1995). [CrossRef]
]. It is the second that we examine by considering the two cases in
Fig. 1.
Fig. 1 Specifications of the cylinders examined in this study.
The computations were carried out for
D = 0.5, 1.0, 1.5, 2.0 μm,
L = 0.5, 1.0, 3.0, 5.0, 7.0, 10.0, 15.0, and 20 μm,
λ = 400, 500, 600, and 700 nm (in vacuum), and
mr
−
imi
= 1.02, 1.05, 1.05 – 0.002
i, 1.05 – 0.008
i, 1.05 – 0.010
i, 1.05 – 0.040
i, 1.10, 1.15, and 1.20, relative to water. The discrete-dipole approximation code [
20
B. T. Draine, “The discrete-dipole approximation and its application to interstellar graphite grains,” Astrophys. J.
333, 848–872 (1988). [CrossRef]
,
21
B. T. Draine and P. Flatau, “Discrete dipole approximation for scattering calculations,” J. Opt. Soc. Am. A
11(4), 1491–1499 (1994). [CrossRef]
] DDSCAT 7.0 was used for most of the computations presented here. The orientational averaging was carried out in the manner prescribed in the DDSCAT code. This averaging is not optimum for scattering by a very long cylinder because for a given orientation the scattered light is in the form of a thin cone containing the incident beam and the axis of which cone is coincident with the axis of the cylinder [
13C. F. Bohren, and D. R. Huffman, Absorption and Scattering of Light by Small Particles (Wiley-Interscience, 1983).
]. The cone broadens as the cylinder’s length decreases. A more robust formal of the averaging for long cylinders has been described by Haracz, et al. [
22
R. D. Haracz, L. D. Cohen, and A. Cohen, “Scattering of linearly polarized light from randomly oriented cylinders and spheroids,” J. Appl. Phys.
58(9), 3322–3327 (1985). [CrossRef]
]; however, as we show later, we believe that averaging process in DDSCAT is sufficiently accurate for the cylinders studied here.
The computations were carried out on an 80 CPU cluster with a total memory of 160 GB. The dipole density was such that their lattice spacing was ~λ /18 at 400 nm and ~λ/31 at 700 nm. This insured that the backscattering cross section could be computed with an error < about 5%. Even with the multi-processor cluster, the computations were very time consuming for the larger particles: ~10 days were required to compute the scattering (at 4 wavelengths) by a cylinder with D = 1.5 μm, L = 15 μm and m = 1.20.
4. Extinction and absorption efficiencies
The extinction and absorption efficiencies were computed using from the orientationally-averaged extinction and absorption cross sections
and
through
and
where
is the orientationally-averaged projected area (shadow) of the particle. Using the computed efficiencies for finite-length cylinders, I asked several questions: (1) how do the efficiencies depend on the aspect ratio (
AR ≡
L/
D) and diameter of the cylinders?; (2) how do the efficiencies compare with those for an infinite cylinder with the same diameter?; and (3) how do the efficiencies depend on the distribution of absorbing material within the cylinders (
Fig. 1)?
Figure 2
provides the computed values of
Qc
and
Qa
for the all aspect ratios that were examined with absorbing cylinders (
mi
> 0) and
mr
= 1.05. The notation in the legend is explained in the figure caption. The upper two panels are for all aspect ratios (1/3 – 30) and the lower panels for
AR ≥ 3. The lines correspond to exact computations for infinite cylinders with the same diameter using the IPHASE code [
15
G. R. Fournier and B. T. Evans, “Approximations to extinction from randomly oriented circular and elliptical cylinders,” Appl. Opt.
35(21), 4271–4282 (1996). [CrossRef]
[PubMed]
]. For the case with weaker absorption, the results clearly show that the efficiencies closely follow those for infinite cylinders as long as
AR ≥ 3, for both the coated and the homogeneous cylinders. For the case with stronger absorption, the “package effect,” the decrease in absorption when the absorbing molecules are not uniformly distributed with in the particle, results in lower absorption efficiency.
Fig. 2 Extinction and absorption efficiencies computed for randomly orientated, homogeneous or coated cylindrically shaped particles, given that their diameter and aspect ratio are known so that their orientationally-averaged projected area is πD(L + D/2)/4. Here, ρ = 2α (mr
−1) and ρ′ = 4α mi
, where mr
− imi
, is the refractive index of the particle relative to water, and α = πD/λ, with D the cylinder’s (outer) diameter and λ the wavelength of light in the water. Solid lines are the exact computations for randomly oriented, infinite cylinders. The notation “m=1.05-040i_1.05-000i” indicates that the refractive index of the core is 1.05 – 0.040i, and the refractive index of the coating is 1.05 – 0.000i, etc. In the case of coated cylinders, ρ and ρ′ are computed using the mi
of the associated homogeneous particle. Top: all aspect ratios (1/3 – 30). Bottom: all aspect ratios ≥ 3.
This packaging effect is displayed more clearly in
Fig. 3
, for which I provide the ratio of the absorption efficiencies
Qa
for a coated cylinder with indices
minside
= 1.05−0.040
i and
moutside
1.05−0.000
i (
Qa
(Packaged)) to that of a homogeneous cylinder
minside
=
moutside
= 1.05−0.010
i (
Qa
(Homo)). Note that both cylinders contain the same number of absorbing molecules. The figure shows that the effect of the absorbing pigment packaging is greatest in the blue region of the spectrum and for larger-diameter cylinders. The maximum decrease in
Qa
due to the packaging is about 25%. Although the symbols do not differentiate between cylinder lengths, for a given diameter the packaging effect is smallest in the shortest cylinder and depends very little on the length once
AR exceeds unity. In the case with less overall absorption, i.e.,
minside
= 1.05−0.008
i and
moutside
= 1.05−0.000
i compared to that of a homogeneous cylinder
minside
=
moutside
= 1.05−0.002
i, similar results are obtained; however, the maximum decrease in
Qa
due to the packaging is only about 10% (
Fig. 2.).
Fig. 3 This figure provides the ratio of absorption efficiencies (coated to homogeneous) of strongly absorbing cylinders as a function of wavelength. The diameter of the cylinder (in μm) is specified in the legend. For each diameter, the symbols refer to cylinder lengths ranging from 0.5 to 15 μm. The figure shows that the effect of the absorbing pigment packaging is greatest in the blue region of the spectrum and for larger-diameter cylinders. Although the symbols do not differentiate between cylinder lengths, for a given diameter the packaging effect is smallest in the shortest cylinder and depends very little on the length once the aspect ratio (length/diameter) exceeds unity.
The extinction efficiencies of finite cylinders with larger values of
ρ are compared with those of infinite cylinders in
Fig. 4
. In this case the refractive index is 1.20 and since there is no absorption
Qb
=
Qc
. The figure clearly shows that for
AR ≥ 3, the extinction efficiency is again close to that of an infinite cylinder, with all cases except two differing by less than ± 10% (RMS difference ~5%).
Fig. 4 Qc
as a function of
ρ, computed for non-absorbing cylinders (
m = 1.20 – 0.000
i) with diameters (
D) ranging from 0.5 μm to 2.0 μm. Left: 0.25 ≤
AR ≤ 30 (points colored in red are
AR = 2). Right: 3 ≤
AR ≤ 30. The solid curve is the extinction efficiency (for a unit length) of randomly-oriented infinite cylinders. As in
Fig. 2,
ρ = 2
α (
m −1) with
α = π
D/
λ.
Thus, it is clear that for homogeneous cylindrically-shaped particles with aspect ratios > about 3, the extinction efficiency becomes close to that of an infinite cylinder, i.e.,
Qc
(
D,
m,
AR) ≈
Qc
(
D,
m,∞). This implies that
, or for two aspect ratios
AR and
AR′ (both > about 3),
Similar expressions hold for the orientationally averaged absorption and scattering efficiencies. Although
has not been computed for coated cylinders, presumably
Eq. (15) should hold for such particles as well.
5. Phase function and backscattering probability of cylinders
We have seen that the extinction and absorption efficiencies of micrometer-sized cylindrical particles depend little on the aspect ratios as long as
AR ≥ 3. Is this the case for the phase function and backscattering probability? I mentioned earlier that the default orientational-averaging scheme used in DDSCAT 7.0 was employed in the present computations. Is this default sufficient to provide orientational averaging for long cylinders? To examine this question, I computed the orientationally-averaged phase function (and
) for cylinders with small and large
AR. To achieve the very large variation in
AR, I used
D = 0.25 μm. The results of this computation are shown in
Fig. 5
. One sees that with the exception of small scattering angles (Θ ≤ 8°), as
AR increases the computed phase function simply becomes “noisier.” This is what would be expected, as the scattering pattern (for a given orientation) degenerates into an infinitely thin cone as
L → ∞. Careful examination shows that there is a high correlation between the “noise” at
AR = 100 and 200, etc., as would be expected as the scattering cone thins. Since the thickness of the scattering cone depends mostly on
λ / L (the thickness decreases as
L increases), I conclude that for the values of
L examined in this work (≤ 25 μm) the averaging procedure in DDSCAT is sufficiently accurate to yield reliable phase functions and backscattering probabilities.
Fig. 5 Orientationally averaged scattering phase functions for long cylinders as a function of aspect ratio (
AR). The values of the computed backscattering probabilities are 0.0212, 0.0212, 0.0209, 0.0218, and 0.0220, for
AR = 5, 10, 100, 200, and 270, respectively. The values of the extinction efficiency (
Qc
) are 0.999, 1.007, 1.032, 1.033, 1.033, and 1.034 for
AR = 5, 10, 100, 200, 270, and ∞, respectively. The value of
ρ for these efficiencies is 1.0472, so these computations fall very close to the continuous curve in
Fig. 4. (Note,
L = 1.25, 2.50, 25.0, 50.0, and 67.5 μm for
AR = 5, 10, 100, 200, and 270, respectively.)
D = 0.25 μm,
m = 1.20,
λ = 400 nm.
Figure 6
provides another example of the weak dependence of the scattering phase function (and degree of linear polarization) on aspect ratio. Virtually the only differences in the phase function between
AR = 20 and
AR = 3 are the enhanced scattering near zero degrees and the deeper minima near 30°, 50°, 80°, and 130° for
AR = 20. This weak dependence on aspect ratios as long as
AR ≥ 5 is also displayed by the backscattering probability as shown in
Fig. 7
for a wide range of refractive indices and particle diameters.
Fig. 6 Orientationally-averaged scattering phase functions (left) and degree of linear polarization (right) at 600 nm (vacuum) for homogeneous cylinders with a diameter of 1 μm and length of 3 μm (D1xL3) and 20 μm (D1xL20). The refractive index is 1.05 – 0.002i. The oscillatory nature of the phase function is determined mostly by D/λ, but with some dependence on m.
Fig. 7 Examples of the variation of the backscattering probability with aspect ratio for cylinder diameters between 0.5 and 1.5 μm and refractive indices ranging from 1.02 to 1.20. The black curves are for a vacuum wavelength of 400 nm and the red curves for 700 nm.
These computations show that when
AR > about 3–5,
and in a manner similar to
Eq. (13),
with both
AR′ >
AR ≈3-5 (
Figs. 7 and
13
). I used
Eq. (14) to compute the orientationally averaged backscattering cross section for cylinders with
D = 1 μm and
AR′ ≥ 5 from
AR = 3 and for
AR′ ≥ 7 from
AR = 5 with
m = 1.05 – 0.010
i. The rms error was 2.5% for
AR = 3 and 1.2% for
AR = 5. Similar computations with
m = 1.20 – 0.000
i resulted in rms errors of 8.1% and 2.6% for
AR = 3, and 5, respectively.
Fig. 13 Backscattering probability as a function of aspect ratio and the imaginary part of the refractive index for non-absorbing to strongly absorbing, homogeneous and structured cylinders. D is in micrometers.
6. Cylinders compared to equal-volume spheres
A well-known approach to estimating the complex refractive index of marine particles, e.g., phytoplankton, is to measure their extinction and absorption coefficients and the particle volume (e.g., with a Coulter Counter). The particles are then assumed to be homogeneous spheres and the extinction and absorption efficiencies are computed. Real and imaginary parts of the refractive index are then found which, for a spherical particle, would yield the same extinction and absorption efficiencies (see, for example, Ref.
18
A. Bricaud and A. Morel, “Light attenuation and scattering by phytoplanktonic cells: a theoretical modeling,” Appl. Opt.
25(4), 571–580 (1986). [CrossRef]
[PubMed]
). I have tested this approach using the extinction and absorption cross sections described above for cylinders. Rather than using the exact computation of
Qc
and
Qa
for spheres, it is much simpler to use the analytical formulas of the van de Hulst anomalous diffraction approximation for the scattering and absorption efficiencies of a homogeneous sphere. These are [
14H. C. Van de Hulst, Light Scattering by Small Particles , (Wiley, 1957).
]
and
where
ρ = 2
α (
mr
−1),
ρ′ = 4
α mi
, tan
β =
mi
/(
mr
−1), and
α = π
d/
λ, with
d the sphere’s diameter and
λ the wavelength of light
in the water. In this analysis, we take
d to be the diameter of a sphere with the same volume as the cylinder, i.e., the
equal-volume sphere.
Fig. 8
provides the extinction and absorption efficiencies computed assuming the spherical shape, e.g.,
, along with
Qc
and
Qa
computed with the Van de Hulst anomalous diffraction theory (VdH), and with exact the Mie theory (MIE). There are three important observations to be made from
Fig. 8: (1) the volume-equivalent sphere assumption is not very good in the case of
Qc
(left figure) even if full Mie theory is used; (2) the volume-equivalent sphere assumption is better in the case of
Qa
(right figure), especially if full Mie theory is used; and (3) the package effect, while relatively unimportant for
Qc
, is important in
Qa
(right figure) for the case with stronger absorption, but not for the case with weaker absorption.
Fig. 8 The extinction (left) and absorption (right) efficiencies computed by dividing the associated cross sections by the projected area of a volume-equivalent sphere as a function of ρ and ρ ′. Here, ρ = 2α (mr
−1) and ρ′ = 4α mi
, where mr
− imi
, is the refractive index of the particle relative to water, and α = πd/λ, where d is now the diameter of the volume-equivalent sphere. For a given experimentally-determined Qa
, the dashed vertical arrow provides the correct ρ ′ (and, hence mi
), while the solid vertical arrow provides the retrieved value of mi
.
How much error does the deviation of the derived
Qc
and
Qa
from Eqs. (18) and (19) make in estimating the refractive index? Given the volume of the particle, and assuming a spherical shape,
d and
α are determined. Calculations of the beam attenuation coefficient and absorption coefficients for coated cylinders were inserted into
Eqs. (15) and
(16) to find
mr
and
mi
.
Figure 9
provides the resulting computations for a coated cylinder with indices
minside
= 1.05−0.040
i and
moutside
= 1.05−0.000
i, and all combinations of diameter and length. Recall that the package effect is larger for this case. Ideally one should derive an index of 1.05−0.010
i, based on the concentration of absorbing material. Clearly,
mi
is retrieved to within ± 20% with an average (over all sizes) close to 0.010, and the retrieved
mr
appears to be too low in almost all cases, but averages ~1.044. One notes that if the exact Mie theory were used in the retrieval of
mi
(
Fig. 8) the retrieved values would be about 10% larger than shown in
Fig. 9 due to the inaccuracy of the Van de Hulst approximation to
Qa
[
Eq. (15)]. However, the exact Mie results cannot actually be used because
mr
is required, and as we see in the figure, it is strongly dependent on
AR. Thus, it is clear that measuring particle volume and the extinction and absorption cross sections, assuming the particles are spherical, then applying
Eqs. (15) and
(16) does yield meaningful results for
mi
even for particles with large aspect ratios; however, the retrieved values of
mr
depend strongly on the aspect ratio. It is interesting to note that if one employed the homogeneous infinite-cylinder assumption in the analysis of the cross sections (
Fig. 2) for this example, the error in the retrieved
mi
would actually be larger than for the equivalent-volume sphere approach: accurate retrieval would require consideration of the package effect, probably by using a coated infinite-cylinder retrieval model.
Fig. 9 An example of retrievals of the real and imaginary parts of the refractive index for coated cylinders for all the combinations of diameter and length, using the van de Hulst approximation. Ideally one should derive a real part of 1.05 and an imaginary part of 0.010. The scatter shows that mi
is retrieved to within ± 20% (somewhat better in the red) with an average (over all sizes) close to 0.010, and that the retrieved mr
appears to be too low in almost all cases, but averages ~1.044.
For larger values of the refractive index of the cylinder, this method fails completely when the cylinder becomes too large. A dramatic example of this failure is provided in
Fig. 10
, which shows
Qc
for cylinders determined from the cross-sectional area of the equal-volume sphere (in a manner identical to that in
Fig. 8), and
ρ evaluated using the diameter of the equal-volume sphere. The thick solid line in the figure is the Van de Hulst approximation to
Qc
. Note that for
ρ > about 3, for most cases shown, there is no refractive index value for equal-volume spheres that can produce the associated extinction efficiency. Thus, this method often fails to provide
any value for
m.
Fig. 10 The extinction efficiency computed by dividing the associated extinction cross section by the projected area of a volume-equivalent sphere as a function of ρ. Here, ρ = 2α (mr
−1) and α = πd/λ, where d is the diameter of the volume-equivalent sphere. Points for some given diameters and lengths are connected by smooth curves (for which λ varies from 400 to 700 nm). The red curves are for diameters of 1.0 and 1.5 μm with AR = 10. The thick curve is the Van de Hulst approximation to Qc
for spheres.
Given the values of
mr
and
mi
derived from measurements of the absorption and extinction efficiencies, the particle volume, and the assumption of sphericity (using the methodology described above, when it works, i.e., for low-index cylinders), how well does the predicted backscattering cross section reproduce the actual backscattering cross section of cylindrical particles? To shed light on this question, I used the retrieved refractive indices shown in
Fig. 9 and Mie theory to compute
for comparison with its cylindrical counterpart
for each wavelength and particle size. The ratio
shows some spectral variation, but to gain a better perspective on the influence of particle shape, I averaged
R over the visible spectrum for each size.
Figure 11
(black points/lines) shows the resulting
R for particles with diameters ~1-3 times the wavelength as a function of the aspect ratio. The red points/lines on the figure provide
R values when the true value of the cylinder’s refractive index is used to compute the backscattering the sphere, rather than that determined from particle extinction, absorption, and volume. We note that for cylinders in this size range,
R is greater than 1 and increases approximately linearly with aspect ratio. The large values of
R when the index is retrieved from extinction, etc., is due to the increased error in the derived values of
mr
as the aspect ratio increases (the retrieved
mr
becomes smaller as the aspect ratio increases, and
is a strong function of
mr
). Thus, the extinction, absorption, volume, and sphericity-assumption methodology cannot yield reliable values of the backscattering cross section of cylindrically shaped particles with even moderate (>5) aspect ratios; however, if the correct refractive index is known and used in the computation, the backscattering of the equal-volume sphere is much closer to that of the cylinder.
Fig. 11 Backscattering by a cylinder divided by backscattering by an equal-volume sphere. Black curves: refractive index in the computation of σbb
for spheres is that derived using the refractive index determined from the extinction and absorption cross sections using the equivalent-volume sphere assumption. Red curves: refractive index in the computation of σbb
for spheres is the same value used for the cylinders, i.e., the correct value. Diameter (D) is in micrometers, and the true value of the refractive index is 1.05–0.010i.
The backscattering ratio
R for the higher index (1.20 – 0.000
i) is shown in
Fig. 12
. Note that in this case
. Thus, in the size range examined here, backscattering by cylinders appears to be larger than equal-volume spheres at low refractive indices and smaller at high refractive indices.
Fig. 12 Backscattering by a cylinder divided by backscattering by an equal-volume sphere. As the refractive index in this case cannot be derived from the extinction efficiency, in the computation of σbb
for spheres m is the same value used for the cylinders. Diameter (D) is in micrometers, the wavelength is 400 nm, and the true value of the refractive index is 1.20–0.000i.
Absorption appears to have only a small effect on the backscattering by cylinders; however, the packaging of the absorbing substance within the cylinder can have a significant effect, especially when the absorption is large.
Figure 13 provides the backscattering probability for cylinders (homogeneous and packaged) for all cases studied with
mr
= 1.05. Note that when the absorption is weak (
mi
= 0.002 with a homogeneous distribution of absorbing molecules, ■, or
mi
= 0.008 with the absorbing molecules confined to the inner cylinder of
Fig. 1, ▲) there is little difference in the backscattering probability and that of a non-absorbing cylinder (♦). In contrast, for the more strongly absorbing, homogeneous (◊) or packaged (□), cylinders, absorption clearly influences the backscattering probability with larger values for the packaged case.
7. Comparison with spheroids
A limited number of computations have been carried out for prolate spheroids to see if the conclusions regarding the influence of aspect ratio on light scattering by cylinders applies to spheroids. Fournier and Evans [
23
G. R. Fournier and B. T. Evans, “Approximation to extinction efficiency for randomly oriented spheroids,” Appl. Opt.
30(15), 2042–2048 (1991). [CrossRef]
[PubMed]
] have provided a highly accurate anomalous diffraction approximation to
Qc
for spheroids. If one uses their relationships for a spheroid with minor axes
D and major axis
L (
AR = L/
D), it is seen that
Qc
becomes almost independent of
AR for
AR > about 3. I have carried out computations (using DDSCAT) for spheroids with
D = 0.5, 1.0, and 1.5 μm, and
AR = 3, 5, and 10, for
m = 1.05 – 0.010
i and
m = 1.20 – 0.000
i. The resulting values of
Qc
(and
Qa
) are virtually independent of
AR and agree well with the Fournier and Evans [
23
G. R. Fournier and B. T. Evans, “Approximation to extinction efficiency for randomly oriented spheroids,” Appl. Opt.
30(15), 2042–2048 (1991). [CrossRef]
[PubMed]
] result for large
AR (e.g.,
AR = 100).
The independence of the backscattering probability on
AR for
AR
3-5 for cylinders is also seen for spheroids of similar size. The results presented in
Table 1
suggest that the backscattering probability for spheroids becomes essentially constant for
AR > about 5. Thus, our conclusions regarding the dependenceof light scattering properties on
AR for cylinders appear to apply equally well to spheroids.
Table 1 The RMS the Backscattering Probability for Spheroids with Aspect Ratio AR = 10 to that for Spheroids with the Same Minor Axes but Aspect Ratio AR. D = 0.5, 1.0, and 1.5 μm, and λ = 400, 500, 600, and 700 nm
| m
| AR = 3 | AR = 5 |
|---|
| 1.05 – 0.010i
| 10.9 | 3.4 |
| 1.20 – 0.000i
| 18.6 | 2.5 |
It should be noted that when
D and
L are <<
λ, and the polarizabilities are determined in the electrostatic approximation (Rayleigh approximation [
13C. F. Bohren, and D. R. Huffman, Absorption and Scattering of Light by Small Particles (Wiley-Interscience, 1983).
,
14H. C. Van de Hulst, Light Scattering by Small Particles , (Wiley, 1957).
]), the total scattering for spheroids is proportional to the square of the volume times a factor that is dependent on
AR. This latter factor becomes nearly independent of
AR for
AR >
~ 3 for the refractive indices of interest here. In this case,
and
Equation (17) replaces
Eq. (13) in this regime, and since
independent of
AR, a similar expression replaces
Eq. (14). Again, similar expressions also apply to cylinders.
8. Concluding remarks
As stated in the abstract, I have shown the extinction, absorption, and scattering efficiencies, and the backscattering probability of randomly oriented, homogeneous and structured, cylinders become nearly independent of the aspect ratio when
AR > ~3-5, for refractive indices characteristic of marine particles (organic and inorganic). This applies to cylinders with diameters in the range 0.25 to 1.5 μm when illuminated with visible light (wavelength, 400-700 nm). Some long-chain phytoplankton, e.g.,
Prochlorotrix hollandica, fall in this size range [
24M. Jonasz, and G. R. Fournier, Light Scattering by Particles in Water, Theoretical and Experimental Foundations (Academic Press, 2007).
]. It should also apply to much larger cylindrically-shaped particles, i.e., in sizes for which geometrical optics is applicable. Computational schemes for intermediate sized cylinders with high aspect ratios are not available; however, as the validity of the observation does not appear to depend on the actual diameter of the cylinders (
Figs. 7 and
13) in the size ranges examined, one would expect that it would apply to intermediate sized particles as well. A limited number of computations for prolate spheroids suggest that the observations apply equally well to particles with this shape. This should simplify the inclusion of
AR-distributions in the characterization of scattering by marine particles.
In order to interpret measured particle extinction and absorption cross sections to obtain the refractive index for single-species of phytoplankton, it is of course best to use a close approximation to the particle’s shape in the necessary model calculations, i.e., there is no canonical shape that can be used for all particles. For cylindrical particles with aspect ratios greater than 3, it appears that infinitely-long cylinders (homogeneous or coated) with the same diameter (shorter dimension) are adequate for estimation of the refractive index. For other particles, other shapes will be appropriate; however, I expect that for particles that can be represented by “simple” shapes, e.g., spheroids, linear chains of spheres or spheroids (homogeneous or coated), etc., the cross sections will be proportional to the length, and the efficiencies will depend mostly on diameter for aspect ratios 3 or greater, as they do for cylinders. For the commonly used equivalent-volume-sphere approximation to obtain refractive index [
18
A. Bricaud and A. Morel, “Light attenuation and scattering by phytoplanktonic cells: a theoretical modeling,” Appl. Opt.
25(4), 571–580 (1986). [CrossRef]
[PubMed]
], we found that for cylinders the absorption index (
mi
) can be determined with reasonable accuracy, i.e., ~ ± 20%, when
mr
is low as it usually is for phytoplankton [
24M. Jonasz, and G. R. Fournier, Light Scattering by Particles in Water, Theoretical and Experimental Foundations (Academic Press, 2007).
]. Remarkably, this approximation is actually better in retrieving
mi
than using a homogeneous cylinder to model (incorrectly) a coated cylinder (
Fig. 2). This suggests that in the absence of shape information, the equivalent-volume-sphere approximation is capable of yielding realistic estimates of
mi
for low-
mr
particles that deviate significantly from spheres. When
mr
is high, the method fails completely (
Fig. 10), and a more appropriate shape is required to interpret the observed cross sections.
In the case of backscattering, for the low index particles we examined, using the index retrieved through the equal-volume-sphere assumption, and computing
σbb
for the equal-volume sphere, can lead to an underestimation (
) of cylinder backscattering by a significant factor (
Fig. 11), largely because of the inaccuracy in estimation of
mr
; however, if the correct value of the refractive index is known, the error is significantly decreased. For the high-index case (for which the equal-volume-sphere analysis fails), given the correct value of the refractive index, the equal-volume sphere backscatters more than the cylinder, i.e.,
Thus, prediction of
by this method for low index particles could account for some of the “missing” backscattering suggested for marine particles [
4
D. Stramski, E. Boss, D. Bogucki, and K. J. Voss, “The role of seawater constituents in light backscattering in the ocean,” Prog. Oceanogr.
61(1), 27–56 (2004). [CrossRef]
]; however, when the correct index is used in the computations, the underestimation is greatly reduced or eliminated completely.
Although the computations presented here represent a grossly inadequate span of cylinder sizes due to inadequate computer resources, they do suggest the manner in which particles with high aspect ratios can be included in scattering computations carried out at lower aspect ratios, particularly when the diameter of the particle is of the order of λ.